Login In
2026 Volume 37 Issue 8
2026, 37(8): 111084
doi: 10.1016/j.cclet.2025.111084
Abstract:
Lithium-sulfurized polyacrylonitrile (Li-SPAN) batteries have attracted attention as a unique subset of lithium-sulfur batteries owing to their effectiveness in mitigating the shuttle effect caused by the dissolution of polysulfides. However, traditional SPAN electrodes typically exhibit an active material loading capacity of < 40 wt% and demonstrate suboptimal reaction kinetics, which limits their actual performance. In this study, a composite film (CoS2/FeS2@SeSPAN/CNTs) was developed, which is poised to serve as the cathode in commercial Li-SPAN batteries. The film was fabricated by forming a PAN framework through casting, subsequently growing Fe-ZIF-67 on it via hydrothermal processing, and converting it into CoS2/FeS2 heterostructure and SeSPAN through heat treatment. The porous structure of this material provided numerous sites for active material storage. This effect led to an active material loading capacity of 61 wt%. Experimental results and density functional theory simulations indicated that, owing to the shielding effect of the cathode solid electrolyte interface, the additionally stored active material exhibited an extended all-solid-state reaction mechanism. Furthermore, the internal electric field generated by the CoS2/FeS2 heterostructure effectively enhanced the adsorption and catalytic conversion of solid polysulfides, thereby improving lithium-ion migration efficiency. As a result, the active material stored in dual-mode exhibited high utilization rates. At a current density of 1 C, the capacity retention of the CoS2/FeS2@SeSPAN/CNTs cathode was 97.9% after 800 cycles. This result demonstrated that the design and development of the CoS2/FeS2@SeSPAN/CNTs composite film significantly enhanced the electrochemical performance of Li-SPAN batteries while paving the way for the commercial exploration of other heterostructural materials in energy storage systems.
Lithium-sulfurized polyacrylonitrile (Li-SPAN) batteries have attracted attention as a unique subset of lithium-sulfur batteries owing to their effectiveness in mitigating the shuttle effect caused by the dissolution of polysulfides. However, traditional SPAN electrodes typically exhibit an active material loading capacity of < 40 wt% and demonstrate suboptimal reaction kinetics, which limits their actual performance. In this study, a composite film (CoS2/FeS2@SeSPAN/CNTs) was developed, which is poised to serve as the cathode in commercial Li-SPAN batteries. The film was fabricated by forming a PAN framework through casting, subsequently growing Fe-ZIF-67 on it via hydrothermal processing, and converting it into CoS2/FeS2 heterostructure and SeSPAN through heat treatment. The porous structure of this material provided numerous sites for active material storage. This effect led to an active material loading capacity of 61 wt%. Experimental results and density functional theory simulations indicated that, owing to the shielding effect of the cathode solid electrolyte interface, the additionally stored active material exhibited an extended all-solid-state reaction mechanism. Furthermore, the internal electric field generated by the CoS2/FeS2 heterostructure effectively enhanced the adsorption and catalytic conversion of solid polysulfides, thereby improving lithium-ion migration efficiency. As a result, the active material stored in dual-mode exhibited high utilization rates. At a current density of 1 C, the capacity retention of the CoS2/FeS2@SeSPAN/CNTs cathode was 97.9% after 800 cycles. This result demonstrated that the design and development of the CoS2/FeS2@SeSPAN/CNTs composite film significantly enhanced the electrochemical performance of Li-SPAN batteries while paving the way for the commercial exploration of other heterostructural materials in energy storage systems.
2026, 37(8): 111173
doi: 10.1016/j.cclet.2025.111173
Abstract:
O3-layered oxides are considered promising for various applications due to their high capacity. However, these O3-type materials are prone to undergo an irreversible O3-P3 phase transition, which adversely impacts their structural stability. Elemental doping has been identified as an effective strategy to mitigate this issue. However, substituting Cu at the redox center reduces the capacity of the pristine material. The unique introduction of the Sb element reduces the lattice oxygen ratio, leading to a significant increase in initial capacity. Thus, the Cu/Sb co-doped material NaNi0.37Mn0.49Cu0.13Sb0.01O2 (NNMCS) with unique O3-dominated phase transition process, was successfully prepared using the high temperature solid-phase method. Cu/Sb doping increases Mn4+ concentration through the charge compensation mechanism at transition metal sites, mitigating the negative structural effects of the dual simplicial state eg orbitals in the high-spin Mn3+ state. Doping with Cu/Sb increases the electron cloud density at the transition metal sites, enhancing the electron shielding effect and ultimately causing the distance between the transition metal sites to expand. The increased distance between the transition metal sites indirectly promotes flexibility during transition metal migration, resulting in electrode materials with a smaller rate of lattice parameter change during cycling and ultimately enhancing phase transition reversibility. As a result, NNMCS demonstrates a high initial specific capacity of 188 mAh/g and 78% capacity retention after 200 cycles at 1 C within a 2.0–4.3 V window. This work provides valuable insights into the coupling mechanism between capacity and structural stability in layered oxides for sodium-ion batteries.
O3-layered oxides are considered promising for various applications due to their high capacity. However, these O3-type materials are prone to undergo an irreversible O3-P3 phase transition, which adversely impacts their structural stability. Elemental doping has been identified as an effective strategy to mitigate this issue. However, substituting Cu at the redox center reduces the capacity of the pristine material. The unique introduction of the Sb element reduces the lattice oxygen ratio, leading to a significant increase in initial capacity. Thus, the Cu/Sb co-doped material NaNi0.37Mn0.49Cu0.13Sb0.01O2 (NNMCS) with unique O3-dominated phase transition process, was successfully prepared using the high temperature solid-phase method. Cu/Sb doping increases Mn4+ concentration through the charge compensation mechanism at transition metal sites, mitigating the negative structural effects of the dual simplicial state eg orbitals in the high-spin Mn3+ state. Doping with Cu/Sb increases the electron cloud density at the transition metal sites, enhancing the electron shielding effect and ultimately causing the distance between the transition metal sites to expand. The increased distance between the transition metal sites indirectly promotes flexibility during transition metal migration, resulting in electrode materials with a smaller rate of lattice parameter change during cycling and ultimately enhancing phase transition reversibility. As a result, NNMCS demonstrates a high initial specific capacity of 188 mAh/g and 78% capacity retention after 200 cycles at 1 C within a 2.0–4.3 V window. This work provides valuable insights into the coupling mechanism between capacity and structural stability in layered oxides for sodium-ion batteries.
2026, 37(8): 111179
doi: 10.1016/j.cclet.2025.111179
Abstract:
The under-barrier Raman relaxation process has long presented a formidable challenge in advancing the performance of single-molecule magnets (SMMs). Exploring the nuanced differences in Raman relaxation processes between two structurally analogous systems remains relatively uncharted territory. Herein, two Dy(Ⅲ)-based single-ion magnets (SIMs) with pentagonal bipyramidal geometry were reported, and their Raman relaxation behaviors were regulated by precisely adjusting the protonation level of the bis-hydrazone moiety. Intriguingly, under the optimal magnetic field, the degree of protonation shows no impact on the Raman exponent n but causes a distinct variation in the Raman relaxation coefficient C. The effects of deprotonation on the molecular geometry and charge distribution were elucidated through ab initio and electrostatic potential (ESP) calculations. Deprotonation results in an asymmetric charge distribution within the equatorial plane, causing the coefficient C to increase substantially by 3.5 times, aligning closely with the theoretical calculation value of approximately 2.8 times. This study provides concise and effective molecular archetypes for investigating the Raman relaxation process.
The under-barrier Raman relaxation process has long presented a formidable challenge in advancing the performance of single-molecule magnets (SMMs). Exploring the nuanced differences in Raman relaxation processes between two structurally analogous systems remains relatively uncharted territory. Herein, two Dy(Ⅲ)-based single-ion magnets (SIMs) with pentagonal bipyramidal geometry were reported, and their Raman relaxation behaviors were regulated by precisely adjusting the protonation level of the bis-hydrazone moiety. Intriguingly, under the optimal magnetic field, the degree of protonation shows no impact on the Raman exponent n but causes a distinct variation in the Raman relaxation coefficient C. The effects of deprotonation on the molecular geometry and charge distribution were elucidated through ab initio and electrostatic potential (ESP) calculations. Deprotonation results in an asymmetric charge distribution within the equatorial plane, causing the coefficient C to increase substantially by 3.5 times, aligning closely with the theoretical calculation value of approximately 2.8 times. This study provides concise and effective molecular archetypes for investigating the Raman relaxation process.
2026, 37(8): 111180
doi: 10.1016/j.cclet.2025.111180
Abstract:
Decorating semiconductor metal oxides (SMOs) with noble metals particles has been proved to be effective method to enhance their gas-sensing performance. However, the issue of noble metal particles aggregation might affect the sensitivity and stability of the material. Herein, a strategy is proposed for the construction of noble metals particles decorated SMOs featuring optimized gas sensing performance through the derivation of metal-organic frameworks (MOFs). By utilizing Sn/Zn-ZIF-8 framework as precursor to encapsulate Pt nanoparticles (NPs) followed by calcination, a core-shell structure of SnO2-ZnO encapsulated with Pt NPs (Pt@SnO2-ZnO) was successfully constructed. The Sn/Zn-ZIF-8 framework structure prevents the aggregation of Pt NPs, which facilitates the adsorption and dissociation of oxygen and methanol molecules. Thereby the Pt@SnO2-ZnO based gas sensor exhibited significantly enhanced response (73.6) towards 10 ppm methanol at 320 ℃ and exceptionally low theoretical detection limit (0.18 ppb), providing an effective approach for the modification of SMOs-based gas-sensing materials.
Decorating semiconductor metal oxides (SMOs) with noble metals particles has been proved to be effective method to enhance their gas-sensing performance. However, the issue of noble metal particles aggregation might affect the sensitivity and stability of the material. Herein, a strategy is proposed for the construction of noble metals particles decorated SMOs featuring optimized gas sensing performance through the derivation of metal-organic frameworks (MOFs). By utilizing Sn/Zn-ZIF-8 framework as precursor to encapsulate Pt nanoparticles (NPs) followed by calcination, a core-shell structure of SnO2-ZnO encapsulated with Pt NPs (Pt@SnO2-ZnO) was successfully constructed. The Sn/Zn-ZIF-8 framework structure prevents the aggregation of Pt NPs, which facilitates the adsorption and dissociation of oxygen and methanol molecules. Thereby the Pt@SnO2-ZnO based gas sensor exhibited significantly enhanced response (73.6) towards 10 ppm methanol at 320 ℃ and exceptionally low theoretical detection limit (0.18 ppb), providing an effective approach for the modification of SMOs-based gas-sensing materials.
2026, 37(8): 111181
doi: 10.1016/j.cclet.2025.111181
Abstract:
The development of electrode materials with a rapid diffusion kinetics and low polarization is crucial for improving energy storage in magnesium ion batteries (MIBs). Herein, the magnesium tungstate with thermal stability and good chemical stability is proposed as the electrode material in MIBs for the first time. According to the simulated results of density functional theory (DFT) calculations, the high exposed (001) plane of MgWO4 can be achieved as the preferred orientation for Mg2+ fast insertion/extraction. The MgWO4 microflowers with exposed (001) plane architecting by uniform nanosheets were successfully synthesized through a high-efficient microwave radiation strategy. The synthesis mechanism of MgWO4 microflowers was explored as "self-assembly-dissolution-recrystallization-Ostwald ripening" through the evolutions of the morphology and microstructure under continuous reaction timespan. As a MIB electrode material, the MgWO4 microflowers exhibit a good reversible specific capacity (54.6 mAh/g) and cycling stability (70.9% capacity retention after 100 cycles). In conclusion, the MgWO4 material with exposed (001) facet and layered pore structure effectively overcomes the slow diffusion kinetics in MIBs, presenting a new avenue for the design and synthesis of novel reversible electrode materials of MIBs.
The development of electrode materials with a rapid diffusion kinetics and low polarization is crucial for improving energy storage in magnesium ion batteries (MIBs). Herein, the magnesium tungstate with thermal stability and good chemical stability is proposed as the electrode material in MIBs for the first time. According to the simulated results of density functional theory (DFT) calculations, the high exposed (001) plane of MgWO4 can be achieved as the preferred orientation for Mg2+ fast insertion/extraction. The MgWO4 microflowers with exposed (001) plane architecting by uniform nanosheets were successfully synthesized through a high-efficient microwave radiation strategy. The synthesis mechanism of MgWO4 microflowers was explored as "self-assembly-dissolution-recrystallization-Ostwald ripening" through the evolutions of the morphology and microstructure under continuous reaction timespan. As a MIB electrode material, the MgWO4 microflowers exhibit a good reversible specific capacity (54.6 mAh/g) and cycling stability (70.9% capacity retention after 100 cycles). In conclusion, the MgWO4 material with exposed (001) facet and layered pore structure effectively overcomes the slow diffusion kinetics in MIBs, presenting a new avenue for the design and synthesis of novel reversible electrode materials of MIBs.
2026, 37(8): 111189
doi: 10.1016/j.cclet.2025.111189
Abstract:
Zeolite-like metal–organic frameworks (ZMOFs) are a unique branch of MOFs, compared to MOFs, the design and synthesis of ZMOFs is challenging due to the peculiar T-O-T angle. Herein, the first ZMOF with unique two-fold interpenetrated SOD topology, [(CH3)2NH2][Zn(2,5-ABTC)0.5(TAZ)]·DMF ·H2O (JLU-MOF119, 2,5-H4ABTC = 2,2′,5,5′-azobenzene tetracarboxylic, TAZ = 1H-tetraazol, DMF = N,N-dimethylformamide), was successfully constructed by utilizing a novel 4 + 4 + 2 strategy. In such a structure, the 4-connected 2,5-H4ABTC ligand serves as the 4-membered ring (4MR) of the structural building units, and the TAZ linker coordinates with the Zn2+ center to form a 6-membered ring (6MR), which assembles with the tetrahedral building units (TBU) to construct the SOD topology. Notably, the stretched and distorted 4MR, which gives rise to two distinct 6MR and a twisted framework, finally leads to the formation of a unique 2-fold interpenetrated SOD framework. The pore structure of JLU-MOF119 is featured by the ultra-microporous pore and the polar surface of the SOD cages caused by uncoordinated N and O sites coming from 2,5-H4ABTC and TAZ ligands, resulting in one-step C2H4 purification from C2H2/CO2/C2H4 mixtures. The dynamic breakthrough and recycling experiments confirm that the C2H4 purity is high up to 99.2%. The successful construction of JLU-MOF119 in this work breaks the theory of forbidden interpenetration in ZMOFs, which will provide more possibilities for structural design and the construction of more complicated structures.
Zeolite-like metal–organic frameworks (ZMOFs) are a unique branch of MOFs, compared to MOFs, the design and synthesis of ZMOFs is challenging due to the peculiar T-O-T angle. Herein, the first ZMOF with unique two-fold interpenetrated SOD topology, [(CH3)2NH2][Zn(2,5-ABTC)0.5(TAZ)]·DMF ·H2O (JLU-MOF119, 2,5-H4ABTC = 2,2′,5,5′-azobenzene tetracarboxylic, TAZ = 1H-tetraazol, DMF = N,N-dimethylformamide), was successfully constructed by utilizing a novel 4 + 4 + 2 strategy. In such a structure, the 4-connected 2,5-H4ABTC ligand serves as the 4-membered ring (4MR) of the structural building units, and the TAZ linker coordinates with the Zn2+ center to form a 6-membered ring (6MR), which assembles with the tetrahedral building units (TBU) to construct the SOD topology. Notably, the stretched and distorted 4MR, which gives rise to two distinct 6MR and a twisted framework, finally leads to the formation of a unique 2-fold interpenetrated SOD framework. The pore structure of JLU-MOF119 is featured by the ultra-microporous pore and the polar surface of the SOD cages caused by uncoordinated N and O sites coming from 2,5-H4ABTC and TAZ ligands, resulting in one-step C2H4 purification from C2H2/CO2/C2H4 mixtures. The dynamic breakthrough and recycling experiments confirm that the C2H4 purity is high up to 99.2%. The successful construction of JLU-MOF119 in this work breaks the theory of forbidden interpenetration in ZMOFs, which will provide more possibilities for structural design and the construction of more complicated structures.
2026, 37(8): 111191
doi: 10.1016/j.cclet.2025.111191
Abstract:
The CO2 electroreduction is a valuable technology towards carbon neutrality but facing great challenge in fabricating efficient and stable electrode. Here we propose the construction of self-supported nanoarray electrode of ultrathin carbon-coated Bi nanospheres through a self-assembly and Joule heating method for high-efficiency electrocatalytic CO2 reduction. The electrode combines the advantages of facilitating electron transfer, accelerating the subsequent electro-proton coupling step in CO2 reduction process and protecting Bi nanoparticles from aggregation or electrochemical corrosion. The highest Faraday efficiency for formic acid in a solid-state electrolyte cell reaches 95.46% with a partial current density of 119.10 mA/cm2 and remains above 90% for 110 h. This route for assembling self-supported nanoarray electrode is rapid, facile, and can be employed in the large-scale fabrication of industrial electrodes in the future.
The CO2 electroreduction is a valuable technology towards carbon neutrality but facing great challenge in fabricating efficient and stable electrode. Here we propose the construction of self-supported nanoarray electrode of ultrathin carbon-coated Bi nanospheres through a self-assembly and Joule heating method for high-efficiency electrocatalytic CO2 reduction. The electrode combines the advantages of facilitating electron transfer, accelerating the subsequent electro-proton coupling step in CO2 reduction process and protecting Bi nanoparticles from aggregation or electrochemical corrosion. The highest Faraday efficiency for formic acid in a solid-state electrolyte cell reaches 95.46% with a partial current density of 119.10 mA/cm2 and remains above 90% for 110 h. This route for assembling self-supported nanoarray electrode is rapid, facile, and can be employed in the large-scale fabrication of industrial electrodes in the future.
2026, 37(8): 111192
doi: 10.1016/j.cclet.2025.111192
Abstract:
Electrochemical ozone production (EOP) has emerged as an eco-friendly, cost-effective alternative to the current industrial corona discharge approach; however, the low Faradaic efficiency (FE) of electrochemical ozone production (EOP) and anode instability at high current density of the conventional plate electrode hinders its actual application. Herein, we introduce a strategy to enhance the EOP performance of β-PbO2 by constructing a three-dimensional (3D) porous architecture. This approach elevates the EOP FE of the 3D-porous β-PbO2@Ti mesh anode (14.73%) to over twice that of the conventional β-PbO2@Ti mesh (6.11%) at a current density of 100 mA/cm2. Furthermore, it demonstrates a robust service life and consistent O3 production capability, sustaining stable output over extended periods (70 h, 20 h) at higher current densities (100, 250 mA/cm2). This strategy of external structural anode modification exerts a beneficial effect on the internal oxygen environment within β-PbO2, increasing the availability of adsorption sites for oxygen intermediates and thus providing favorable conditions for efficient O3 generation. This work shows the potential of 3D porous anode for practical industrial deployment of EOP.
Electrochemical ozone production (EOP) has emerged as an eco-friendly, cost-effective alternative to the current industrial corona discharge approach; however, the low Faradaic efficiency (FE) of electrochemical ozone production (EOP) and anode instability at high current density of the conventional plate electrode hinders its actual application. Herein, we introduce a strategy to enhance the EOP performance of β-PbO2 by constructing a three-dimensional (3D) porous architecture. This approach elevates the EOP FE of the 3D-porous β-PbO2@Ti mesh anode (14.73%) to over twice that of the conventional β-PbO2@Ti mesh (6.11%) at a current density of 100 mA/cm2. Furthermore, it demonstrates a robust service life and consistent O3 production capability, sustaining stable output over extended periods (70 h, 20 h) at higher current densities (100, 250 mA/cm2). This strategy of external structural anode modification exerts a beneficial effect on the internal oxygen environment within β-PbO2, increasing the availability of adsorption sites for oxygen intermediates and thus providing favorable conditions for efficient O3 generation. This work shows the potential of 3D porous anode for practical industrial deployment of EOP.
2026, 37(8): 111212
doi: 10.1016/j.cclet.2025.111212
Abstract:
Transition metal oxides are regarded as promising alternatives to graphite anode material due to their high theoretical capacities. However, their low conductivity, large volume change and fragile structure during battery operation hamper large-scale applications. Herein, we synthesize F-doping and oxygen defect CoO composite (F/O-CoO) through a facile hydrothermal and following annealing process. Benefiting from the synergy of F-doping and oxygen defect, the F/O-CoO anode material delivers a high reversible capacity of 1112 mAh/g at 0.5 C and capacity retention of 609 mAh/g (79.1%) at 2 C after 400 cycles, as well as a rate capacity of 449 mAh/g at 5 C. This superior capacity enhancement is attributed to the enrichment of oxygen defect and necessary substitution of lattice oxygen atom by F, which play an important role in improving electrical conductivity and thus reducing polarization. DFT calculation provides a further explanation that F doping can reduce the Li+ adsorption energy and the bandgap energy of F/O-CoO material, as well as increase Li+ storage sites and Li+/e- conductivity.
Transition metal oxides are regarded as promising alternatives to graphite anode material due to their high theoretical capacities. However, their low conductivity, large volume change and fragile structure during battery operation hamper large-scale applications. Herein, we synthesize F-doping and oxygen defect CoO composite (F/O-CoO) through a facile hydrothermal and following annealing process. Benefiting from the synergy of F-doping and oxygen defect, the F/O-CoO anode material delivers a high reversible capacity of 1112 mAh/g at 0.5 C and capacity retention of 609 mAh/g (79.1%) at 2 C after 400 cycles, as well as a rate capacity of 449 mAh/g at 5 C. This superior capacity enhancement is attributed to the enrichment of oxygen defect and necessary substitution of lattice oxygen atom by F, which play an important role in improving electrical conductivity and thus reducing polarization. DFT calculation provides a further explanation that F doping can reduce the Li+ adsorption energy and the bandgap energy of F/O-CoO material, as well as increase Li+ storage sites and Li+/e- conductivity.
2026, 37(8): 111227
doi: 10.1016/j.cclet.2025.111227
Abstract:
Although the distinctive physicochemical properties of Pt-based intermetallic nanomaterials are well-recognized, the critical influence of Pt skin-induced lattice strain effects on their enzyme-mimicking catalytic performance remains unexplored. This knowledge gap primarily stems from the technical challenges in achieving atomic-level precision and structural uniformity when engineering active sites within Pt-based intermetallic systems. Herein, we demonstrate exceptional peroxidase-like catalytic activity (25.545 U/mg) and remarkable specificity through strain-engineered L10 PtCo@Pt core-shell architectures. Experimental and theoretical analyses reveal that significantly reduces H2O2 adsorption energy (-1.49 eV) and the energy barrier of rate-determining step (0.128 eV). This strain-driven electronic modulation enables a 17.4-fold enhancement in peroxidase-like activity compared to conventional Pt nanoparticles, establishing a quantitative correlation between interfacial lattice compression (3.5% strain) and catalytic efficiency. Three key advances emerge from this work: (1) Identification of lattice strain as a dominant descriptor for nanozyme specificity in H2O2 activation, (2) development of a universal synthesis framework (<1 min) for ordered intermetallic core-shell systems, and (3) demonstration of strain engineering as a generalizable strategy exceeding noble metal-dependent activity enhancement. The developed methodology not only resolves long-standing challenges in scalable nanozyme production but also opens new avenues for designing biocatalysts through atomic-level strain manipulation.
Although the distinctive physicochemical properties of Pt-based intermetallic nanomaterials are well-recognized, the critical influence of Pt skin-induced lattice strain effects on their enzyme-mimicking catalytic performance remains unexplored. This knowledge gap primarily stems from the technical challenges in achieving atomic-level precision and structural uniformity when engineering active sites within Pt-based intermetallic systems. Herein, we demonstrate exceptional peroxidase-like catalytic activity (25.545 U/mg) and remarkable specificity through strain-engineered L10 PtCo@Pt core-shell architectures. Experimental and theoretical analyses reveal that significantly reduces H2O2 adsorption energy (-1.49 eV) and the energy barrier of rate-determining step (0.128 eV). This strain-driven electronic modulation enables a 17.4-fold enhancement in peroxidase-like activity compared to conventional Pt nanoparticles, establishing a quantitative correlation between interfacial lattice compression (3.5% strain) and catalytic efficiency. Three key advances emerge from this work: (1) Identification of lattice strain as a dominant descriptor for nanozyme specificity in H2O2 activation, (2) development of a universal synthesis framework (<1 min) for ordered intermetallic core-shell systems, and (3) demonstration of strain engineering as a generalizable strategy exceeding noble metal-dependent activity enhancement. The developed methodology not only resolves long-standing challenges in scalable nanozyme production but also opens new avenues for designing biocatalysts through atomic-level strain manipulation.
2026, 37(8): 111228
doi: 10.1016/j.cclet.2025.111228
Abstract:
The nickel-rich layered cathode materials (LiNixCoyMn1-x-yO2) in lithium-ion batteries suffer from labile surface reactivity, leading to the formation of residual lithium impurities and the induction of interfacial side reactions, ultimately degrading battery performance. Here, a controlled reaction between residual lithium and the glassy material H3BO3 on the surface of commercial LiNi0.82Co0.12Mn0.06O2 cathode materials converts into a protective fast ionic conductor layer. It was observed that sintering temperatures distinctly influenced the composition and structure of interface coating, subsequently affecting electrochemical properties of cathode. Notably, upon treatment at a relatively low temperature of 300 ℃, the surface of sample was enveloped in an amorphous LiBO2 layer, which effectively alleviates interfacial side reactions, stabilizes the crystal structure and enhances lithium-ion transport kinetics. Furthermore, during cycling, the amorphous LiBO2 coating facilitates the formation of a stable cathode electrolyte interphase layer enriched with LiF. Consequently, the material exhibits exceptional electrochemical performance, balancing high capacity and excellent cycling stability. This interfacial engineering strategy, compatible with industrial-scale processing, provides a viable pathway to enhance the durability of nickel-rich cathodes for high-energy-density batteries.
The nickel-rich layered cathode materials (LiNixCoyMn1-x-yO2) in lithium-ion batteries suffer from labile surface reactivity, leading to the formation of residual lithium impurities and the induction of interfacial side reactions, ultimately degrading battery performance. Here, a controlled reaction between residual lithium and the glassy material H3BO3 on the surface of commercial LiNi0.82Co0.12Mn0.06O2 cathode materials converts into a protective fast ionic conductor layer. It was observed that sintering temperatures distinctly influenced the composition and structure of interface coating, subsequently affecting electrochemical properties of cathode. Notably, upon treatment at a relatively low temperature of 300 ℃, the surface of sample was enveloped in an amorphous LiBO2 layer, which effectively alleviates interfacial side reactions, stabilizes the crystal structure and enhances lithium-ion transport kinetics. Furthermore, during cycling, the amorphous LiBO2 coating facilitates the formation of a stable cathode electrolyte interphase layer enriched with LiF. Consequently, the material exhibits exceptional electrochemical performance, balancing high capacity and excellent cycling stability. This interfacial engineering strategy, compatible with industrial-scale processing, provides a viable pathway to enhance the durability of nickel-rich cathodes for high-energy-density batteries.
2026, 37(8): 111230
doi: 10.1016/j.cclet.2025.111230
Abstract:
We report herein the synthesis, structure and catalysis of a cobalt-kernelled icosahedral gold nanocluster CoAu12, providing an opportunity for the in-depth understanding of rarely reported Co-doped gold nanoclusters. CoAu12 possesses a symmetric and contracted metal kernel compared to the 4d and 5d metal-kernelled MAu12 nanoclusters (M = Pd, Pt, Rh, Ir, Au), thus exhibiting highly structural stability. Meanwhile, CoAu12 demonstrates efficient energy and electron transfer activity toward oxygen, thus endowing this nanocluster with exceptional catalytic activity in converting oxygen to singlet oxygen as well as superoxide. Structural features such as the unpaired electron of CoAu12 have been verified as contributing to its catalytic activity. Efficient organic transformations involving singlet oxygen and superoxide were developed based on the structurally stable and catalytically active CoAu12 nanocluster.
We report herein the synthesis, structure and catalysis of a cobalt-kernelled icosahedral gold nanocluster CoAu12, providing an opportunity for the in-depth understanding of rarely reported Co-doped gold nanoclusters. CoAu12 possesses a symmetric and contracted metal kernel compared to the 4d and 5d metal-kernelled MAu12 nanoclusters (M = Pd, Pt, Rh, Ir, Au), thus exhibiting highly structural stability. Meanwhile, CoAu12 demonstrates efficient energy and electron transfer activity toward oxygen, thus endowing this nanocluster with exceptional catalytic activity in converting oxygen to singlet oxygen as well as superoxide. Structural features such as the unpaired electron of CoAu12 have been verified as contributing to its catalytic activity. Efficient organic transformations involving singlet oxygen and superoxide were developed based on the structurally stable and catalytically active CoAu12 nanocluster.
2026, 37(8): 111263
doi: 10.1016/j.cclet.2025.111263
Abstract:
The low-temperature performance of lithium iron phosphate (LiFePO4) batteries remains a significant challenge. Electrolyte engineering has emerged as an effective strategy to address this issue efficiently. Herein, ethyl pentafluoropropionate (pFEP) is introduced into the carbonate-based electrolyte as a functional additive that enables LiLFP cells to cycle at −20 ℃ or even −40 ℃. Molecular dynamics (MD) simulations and spectroscopic characterization demonstrate that adding only 3% pFEP could effectively modify the electrolyte solvation structure, significantly increasing the content of contact ion pairs (CIPs) and aggregates (AGGs). This structural modification promotes the formation of a uniform LiF-rich interphase, which is crucial for improved battery performance. As a result, LiLFP cell with active cathode loading of 8.5 mg/cm2 delivers 117.2 mAh/g and cycling stability over 130 cycles at −20 ℃. This work provides a cost-effective strategy for enhancing the low-temperature performance of LFP batteries.
The low-temperature performance of lithium iron phosphate (LiFePO4) batteries remains a significant challenge. Electrolyte engineering has emerged as an effective strategy to address this issue efficiently. Herein, ethyl pentafluoropropionate (pFEP) is introduced into the carbonate-based electrolyte as a functional additive that enables LiLFP cells to cycle at −20 ℃ or even −40 ℃. Molecular dynamics (MD) simulations and spectroscopic characterization demonstrate that adding only 3% pFEP could effectively modify the electrolyte solvation structure, significantly increasing the content of contact ion pairs (CIPs) and aggregates (AGGs). This structural modification promotes the formation of a uniform LiF-rich interphase, which is crucial for improved battery performance. As a result, LiLFP cell with active cathode loading of 8.5 mg/cm2 delivers 117.2 mAh/g and cycling stability over 130 cycles at −20 ℃. This work provides a cost-effective strategy for enhancing the low-temperature performance of LFP batteries.
2026, 37(8): 111264
doi: 10.1016/j.cclet.2025.111264
Abstract:
Self-trapped exciton (STE) emissions based on Sb3+ ion materials have recently received widespread attention, due to the excellent photoluminescence (PL) properties and stereochemical activity of Sb3+ ions. Pressure can precisely regulate the electronic structure and configuration of chromophores, becoming an effective approach to enhance the STE emissions. Recently, STE emission enhancements in Sb3+-based materials under pressure mainly focus on metal halides, however, studies on inorganic oxides are very limited. Herein, the high-pressure STE behavior of SbTaO4 was investigated up to 13.2 GPa. The STE emission exhibits a bi-peak feature, and the strongest emission occurs at 3.8 GPa, in which two peaks are enhanced by ~20 and ~3 times and the STE emission displays a bright green color. The mechanism is explained using a variety of methods, including steady-state PL spectroscopy, kinetic spectroscopy, Raman spectroscopy, cryogenic PL spectroscopy and theoretical calculations. It shows that the strong electron-phonon coupling of SbTaO4 is weakened, which suppresses non-radiative transitions. Also, the distortion of the [SbO4] unit inhibits the transition between two STE states. The synergistic effect of these factors leads to a strong enhancement of the STE emission in SbTaO4 under pressure. The STE emission enhancement of SbTaO4 highlights the potential of inorganic oxides for future high-pressure STE exploration and provides the promising material in photonic devices under extreme conditions.
Self-trapped exciton (STE) emissions based on Sb3+ ion materials have recently received widespread attention, due to the excellent photoluminescence (PL) properties and stereochemical activity of Sb3+ ions. Pressure can precisely regulate the electronic structure and configuration of chromophores, becoming an effective approach to enhance the STE emissions. Recently, STE emission enhancements in Sb3+-based materials under pressure mainly focus on metal halides, however, studies on inorganic oxides are very limited. Herein, the high-pressure STE behavior of SbTaO4 was investigated up to 13.2 GPa. The STE emission exhibits a bi-peak feature, and the strongest emission occurs at 3.8 GPa, in which two peaks are enhanced by ~20 and ~3 times and the STE emission displays a bright green color. The mechanism is explained using a variety of methods, including steady-state PL spectroscopy, kinetic spectroscopy, Raman spectroscopy, cryogenic PL spectroscopy and theoretical calculations. It shows that the strong electron-phonon coupling of SbTaO4 is weakened, which suppresses non-radiative transitions. Also, the distortion of the [SbO4] unit inhibits the transition between two STE states. The synergistic effect of these factors leads to a strong enhancement of the STE emission in SbTaO4 under pressure. The STE emission enhancement of SbTaO4 highlights the potential of inorganic oxides for future high-pressure STE exploration and provides the promising material in photonic devices under extreme conditions.
2026, 37(8): 111266
doi: 10.1016/j.cclet.2025.111266
Abstract:
In this study, we employed sodium hydroxide and 2,6-pyridinedimethanol as modulators to tailor the structure of metal-organic crystals via “coordination modulation strategy”. Based on this strategy, two copper-based crystalline materials were synthesized via hydrothermal synthesis and structurally characterized. Single-crystal X-ray diffraction analysis elucidates that [Cu2(μ2–OH)(μ3–OH)(H2dcppa)(H2O)]·H2O (dcppa = 3-(3′,5′-dicarboxyphenoxy)phthalic acid, CP-1) exist a kind of [Cu4(μ2–OH)2(μ3–OH)2(H2O)2]4+ cluster. Each [Cu4(μ2–OH)2(μ3–OH)2(H2O)2]4+ is interconnected in-plane with H2dcppa ligands, forming a four-directional extended coordination network that ultimately generates a periodically arranged layered architecture. In [Cu4(Hdcppa)2(H2dcppa)(H2O)3] (MOF-1), there are two types of binuclear copper building blocks, [Cu2(H2O)]4+ and [Cu2(H2O)2]4+, respectively. The adjacent [Cu2(H2O)]4+ units are interconnected via Hdcppa ligands, forming a 1D metal-organic chain. These 1D chains are connected by [Cu2(H2O)2]4+ to establish a 2D layer, which is further extended by H2dcppa ligands to a 3D framework. The successful implementation of this synthetic route further validates the feasibility and effectiveness of combining hydrothermal methods with coordination modulation strategies for the targeted construction of functionalized metal-organic crystals. The proton conductivities (σ) of CP-1 and MOF-1 were measured under conditions of 85 ℃ and 98% relative humidity (RH), resulting in values of 2.14 × 10−3 and 2.55 × 10–2 S/cm, respectively. This study presents a novel approach to fabricating MOFs as proton conductors through coordination modulation strategy.
In this study, we employed sodium hydroxide and 2,6-pyridinedimethanol as modulators to tailor the structure of metal-organic crystals via “coordination modulation strategy”. Based on this strategy, two copper-based crystalline materials were synthesized via hydrothermal synthesis and structurally characterized. Single-crystal X-ray diffraction analysis elucidates that [Cu2(μ2–OH)(μ3–OH)(H2dcppa)(H2O)]·H2O (dcppa = 3-(3′,5′-dicarboxyphenoxy)phthalic acid, CP-1) exist a kind of [Cu4(μ2–OH)2(μ3–OH)2(H2O)2]4+ cluster. Each [Cu4(μ2–OH)2(μ3–OH)2(H2O)2]4+ is interconnected in-plane with H2dcppa ligands, forming a four-directional extended coordination network that ultimately generates a periodically arranged layered architecture. In [Cu4(Hdcppa)2(H2dcppa)(H2O)3] (MOF-1), there are two types of binuclear copper building blocks, [Cu2(H2O)]4+ and [Cu2(H2O)2]4+, respectively. The adjacent [Cu2(H2O)]4+ units are interconnected via Hdcppa ligands, forming a 1D metal-organic chain. These 1D chains are connected by [Cu2(H2O)2]4+ to establish a 2D layer, which is further extended by H2dcppa ligands to a 3D framework. The successful implementation of this synthetic route further validates the feasibility and effectiveness of combining hydrothermal methods with coordination modulation strategies for the targeted construction of functionalized metal-organic crystals. The proton conductivities (σ) of CP-1 and MOF-1 were measured under conditions of 85 ℃ and 98% relative humidity (RH), resulting in values of 2.14 × 10−3 and 2.55 × 10–2 S/cm, respectively. This study presents a novel approach to fabricating MOFs as proton conductors through coordination modulation strategy.
2026, 37(8): 111268
doi: 10.1016/j.cclet.2025.111268
Abstract:
The bulk anomalous photovoltaic effect (BAPV) in non-centrosymmetric materials can produce photovoltage exceeding the bandgap, distinguishing them from traditional semiconductors and offering substantial potential in photovoltaics. Chiral hybrid perovskites, characterized by asymmetric structure and structural tunability, present promise to generate BAPV with desired optoelectronic properties. Herein, we introduced chiral (S)- and (R)-α-methylbenzylamine (S/R-α-MBA) cations to construct a pair of lead-free chiral-polar perovskites, denoted as (S-α-MBA)4Bi2I10 and (R-α-MBA)4Bi2I10 (1S and 1R). Remarkably, 1S and 1R exhibited the distinctive BAPV effect with an impressive photovoltage of 15 V, highlighting the potential for prominent photovoltaic performance. Furthermore, self-powered broadband photoresponse is realized via photo-induced pyroelectricity based on inherent spontaneous polarization in 1S and 1R. The fabricated photodetectors demonstrated enhanced photocurrent response compared to those relying on the photovoltaic effect alone. This innovation eliminates the confinement of photodetection by material semiconductor properties, thereby effectively broadening their application scope.
The bulk anomalous photovoltaic effect (BAPV) in non-centrosymmetric materials can produce photovoltage exceeding the bandgap, distinguishing them from traditional semiconductors and offering substantial potential in photovoltaics. Chiral hybrid perovskites, characterized by asymmetric structure and structural tunability, present promise to generate BAPV with desired optoelectronic properties. Herein, we introduced chiral (S)- and (R)-α-methylbenzylamine (S/R-α-MBA) cations to construct a pair of lead-free chiral-polar perovskites, denoted as (S-α-MBA)4Bi2I10 and (R-α-MBA)4Bi2I10 (1S and 1R). Remarkably, 1S and 1R exhibited the distinctive BAPV effect with an impressive photovoltage of 15 V, highlighting the potential for prominent photovoltaic performance. Furthermore, self-powered broadband photoresponse is realized via photo-induced pyroelectricity based on inherent spontaneous polarization in 1S and 1R. The fabricated photodetectors demonstrated enhanced photocurrent response compared to those relying on the photovoltaic effect alone. This innovation eliminates the confinement of photodetection by material semiconductor properties, thereby effectively broadening their application scope.
2026, 37(8): 111280
doi: 10.1016/j.cclet.2025.111280
Abstract:
The Sierpiński triangle (ST) is a widely-known deterministic fractal structure that has attracted considerable attention recently. The fabrication of nitrogen-doped defect-free STs is appealing yet challenging. This is due to factors such as the increase in active sites, the random generation of nucleation centers, and the experimental growth conditions. In this contribution, we utilize a combination of density functional theory (DFT), Monte Carlo simulation (MC) and scanning tunneling microscopy (STM) to investigate the formation of nitrogen-doped STs. These STs are formed with nitrogen-rich, conformationally flexible 2,2′:6′,2′′-terpyridine-6,6′′-dicarbonitrile (TDBT) molecules and Fe atoms on Au(111). The replacement of benzenes with three pyridine side groups facilitates the formation of the nitrogen-doped STs with a relatively high order because of the energetic preference of molecular configurations. The introduction of the rigid 4,4″-dicyano-1,1′:3′,1″-terphenyl (C3PC) molecules markedly induces the structural transformation of the STs from ordered to high-entropy. Moreover, the nitrogen-doped STs with an order of up to 4 can be directly visualized by low-temperature STM.
The Sierpiński triangle (ST) is a widely-known deterministic fractal structure that has attracted considerable attention recently. The fabrication of nitrogen-doped defect-free STs is appealing yet challenging. This is due to factors such as the increase in active sites, the random generation of nucleation centers, and the experimental growth conditions. In this contribution, we utilize a combination of density functional theory (DFT), Monte Carlo simulation (MC) and scanning tunneling microscopy (STM) to investigate the formation of nitrogen-doped STs. These STs are formed with nitrogen-rich, conformationally flexible 2,2′:6′,2′′-terpyridine-6,6′′-dicarbonitrile (TDBT) molecules and Fe atoms on Au(111). The replacement of benzenes with three pyridine side groups facilitates the formation of the nitrogen-doped STs with a relatively high order because of the energetic preference of molecular configurations. The introduction of the rigid 4,4″-dicyano-1,1′:3′,1″-terphenyl (C3PC) molecules markedly induces the structural transformation of the STs from ordered to high-entropy. Moreover, the nitrogen-doped STs with an order of up to 4 can be directly visualized by low-temperature STM.
2026, 37(8): 111310
doi: 10.1016/j.cclet.2025.111310
Abstract:
Lithium metal anodes are a compelling option for high-energy-density rechargeable batteries. However, they face challenges such as uncontrolled dendrite growth and unstable interphase, particularly at elevated areal capacities. In this study, we introduce a multi-functional skeleton design that promotes uniform nucleation and growth of Li metal, enhancing interfacial stability. Our innovation features a skeleton-alloy-fluorinated hybrid framework, incorporating abundantly N-doped lithiophilic sites and MgF2 particles within a carbon fiber matrix. The lithophilic carbon fiber provides numerous Li nucleation sites, mitigating Li deposition inhomogeneity and suppressing dendrite formation. The LiMg alloy phase formed by MgF2 further promotes homogeneous Li growth. Additionally, the resulting LiF can passivate and protect Li metal at the electrode-electrolyte interface, enhancing the cycling stability of Li anode. Employing this co-engineering strategy, the as-designed composite Li anode lasts over 1000 h in symmetric cells. Li-S full cells deliver 3.9 mAh/cm2 after 200 cycles at a high sulfur loading of 11.0 mg/cm2. This multi-functional approach provides insights for advancing lithium metal battery applications.
Lithium metal anodes are a compelling option for high-energy-density rechargeable batteries. However, they face challenges such as uncontrolled dendrite growth and unstable interphase, particularly at elevated areal capacities. In this study, we introduce a multi-functional skeleton design that promotes uniform nucleation and growth of Li metal, enhancing interfacial stability. Our innovation features a skeleton-alloy-fluorinated hybrid framework, incorporating abundantly N-doped lithiophilic sites and MgF2 particles within a carbon fiber matrix. The lithophilic carbon fiber provides numerous Li nucleation sites, mitigating Li deposition inhomogeneity and suppressing dendrite formation. The LiMg alloy phase formed by MgF2 further promotes homogeneous Li growth. Additionally, the resulting LiF can passivate and protect Li metal at the electrode-electrolyte interface, enhancing the cycling stability of Li anode. Employing this co-engineering strategy, the as-designed composite Li anode lasts over 1000 h in symmetric cells. Li-S full cells deliver 3.9 mAh/cm2 after 200 cycles at a high sulfur loading of 11.0 mg/cm2. This multi-functional approach provides insights for advancing lithium metal battery applications.
2026, 37(8): 111311
doi: 10.1016/j.cclet.2025.111311
Abstract:
We report a facile low-temperature synthesis of Fe-doped NiSe2 nanoparticles as an efficient pre-catalyst, which undergoes complete electrochemical reconstruction into amorphous γ-FexNi1-xOOH nanosheets (< 2 nm thickness) during activation process of cyclic voltammetry. The reconstituted catalyst achieves record-low overpotentials of 163 mV at 20 mA/cm2 and 230 mV at 300 mA/cm2, with a Tafel slope of 33.8 mV/dec and a turnover frequency (TOF) of 0.1 s-1 at overpotential of 210 mV. Remarkably, it shows outstanding operational stability with negligible activity decay after 300 h chronopotentiometry at 100 mA/cm2. Through multimodal ex situ/in situ characterizations, we conclusively identify the in situ-formed amorphous γ-FexNi1-xOOH nanosheets as the active phase, where Fe doping optimizes the electronic structure of Ni sites while the ultrathin morphology maximizes exposed active centers. This work establishes a universal precatalyst engineering strategy through controlled structural evolution of metastable precursors, applicable to diverse energy conversion systems.
We report a facile low-temperature synthesis of Fe-doped NiSe2 nanoparticles as an efficient pre-catalyst, which undergoes complete electrochemical reconstruction into amorphous γ-FexNi1-xOOH nanosheets (< 2 nm thickness) during activation process of cyclic voltammetry. The reconstituted catalyst achieves record-low overpotentials of 163 mV at 20 mA/cm2 and 230 mV at 300 mA/cm2, with a Tafel slope of 33.8 mV/dec and a turnover frequency (TOF) of 0.1 s-1 at overpotential of 210 mV. Remarkably, it shows outstanding operational stability with negligible activity decay after 300 h chronopotentiometry at 100 mA/cm2. Through multimodal ex situ/in situ characterizations, we conclusively identify the in situ-formed amorphous γ-FexNi1-xOOH nanosheets as the active phase, where Fe doping optimizes the electronic structure of Ni sites while the ultrathin morphology maximizes exposed active centers. This work establishes a universal precatalyst engineering strategy through controlled structural evolution of metastable precursors, applicable to diverse energy conversion systems.
2026, 37(8): 111312
doi: 10.1016/j.cclet.2025.111312
Abstract:
Transition metal phosphides (TMPs) are a promising class of functional nanomaterials with significant potential for energy-related applications. However, a universal synthesis method that is both efficient and scalable remains a challenge. This study introduces an ultrafast carbothermal shock (UCS) technique as efficient method for synthesizing various TMPs, including Rh2P, Ir2P, Pd5P2, RuP and PtP2, in just 15 s under ambient air conditions. Notably, the as synthesized Rh2P exhibits remarkable hydrogen evolution reaction (HER) performance with low overpotentials of 13 and 70 mV to reach current densities of 10 and 100 mA/cm2, respectively, coupled with excellent operational stability for over 20 h. This technique not only provides a universal platform for producing various metal phosphides, but also holds significant promise for advancing their applications in energy conversion and storage devices, catalysis, and biosensors.
Transition metal phosphides (TMPs) are a promising class of functional nanomaterials with significant potential for energy-related applications. However, a universal synthesis method that is both efficient and scalable remains a challenge. This study introduces an ultrafast carbothermal shock (UCS) technique as efficient method for synthesizing various TMPs, including Rh2P, Ir2P, Pd5P2, RuP and PtP2, in just 15 s under ambient air conditions. Notably, the as synthesized Rh2P exhibits remarkable hydrogen evolution reaction (HER) performance with low overpotentials of 13 and 70 mV to reach current densities of 10 and 100 mA/cm2, respectively, coupled with excellent operational stability for over 20 h. This technique not only provides a universal platform for producing various metal phosphides, but also holds significant promise for advancing their applications in energy conversion and storage devices, catalysis, and biosensors.
2026, 37(8): 111326
doi: 10.1016/j.cclet.2025.111326
Abstract:
The emergence of aqueous K/Zn dual-ion batteries has opened a promising new frontier in energy storage by leveraging the high energy density of zinc-ion batteries (ZIBs) and the voltage enhancement provided by cation intercalation mechanisms. However, the lifespan of these batteries has been significantly limited by dendrite growth and side reactions at the zinc negative electrode. To address this challenge, we successfully fabricated an organic framework, Zn-MOF-74, in-situ on the surface of the zinc negative electrode. The large-pore, one-dimensional channel structure of Zn-MOF-74 effectively enhances electrolyte permeability, reduces steric hindrance, and promotes efficient battery operation. Moreover, the open metal sites in Zn-MOF-74 effectively suppress side reactions, further improving battery performance. Notably, the average CE remained remarkably high at 99.43% after 1000 cycles. Furthermore, the Zn-MOF-74@Zn//ZnHCF configuration demonstrated exceptional cycling stability, retaining 88% of its initial capacity even after 1000 cycles at a current density of 1 A/g.
The emergence of aqueous K/Zn dual-ion batteries has opened a promising new frontier in energy storage by leveraging the high energy density of zinc-ion batteries (ZIBs) and the voltage enhancement provided by cation intercalation mechanisms. However, the lifespan of these batteries has been significantly limited by dendrite growth and side reactions at the zinc negative electrode. To address this challenge, we successfully fabricated an organic framework, Zn-MOF-74, in-situ on the surface of the zinc negative electrode. The large-pore, one-dimensional channel structure of Zn-MOF-74 effectively enhances electrolyte permeability, reduces steric hindrance, and promotes efficient battery operation. Moreover, the open metal sites in Zn-MOF-74 effectively suppress side reactions, further improving battery performance. Notably, the average CE remained remarkably high at 99.43% after 1000 cycles. Furthermore, the Zn-MOF-74@Zn//ZnHCF configuration demonstrated exceptional cycling stability, retaining 88% of its initial capacity even after 1000 cycles at a current density of 1 A/g.
2026, 37(8): 111327
doi: 10.1016/j.cclet.2025.111327
Abstract:
Porous single crystal (PSC) materials have a large specific surface area, higher structural stability, and more active sites by combining porosity and structural coherence, which provide a clear advantage in the field of catalysis. Platinum-based catalysts are precious metal catalysts commonly used in the dehydrogenation of low-carbon alkanes, with excellent dehydrogenation activity and good catalytic activity for the anaerobic dehydrogenation of ethane. By lattice reconstruction strategy we grow PSC MgO from the parent MgF2 single crystal and load Pt nanoparticles on its surface for growing PSC Pt/MgO. Oxygen vacancies are introduced by constructing active sites on a clear surface structure, which improve catalytic activity and durability. The PSC Pt/MgO catalyst for the direct dehydrogenation of ethane achieves an ethane conversion rate of approximately 28% and ethylene selectivity of over 97%, with good stability over 100 h. The present work offers significant value for the growth and application of porous single crystal oxides loaded with metal nanoparticles.
Porous single crystal (PSC) materials have a large specific surface area, higher structural stability, and more active sites by combining porosity and structural coherence, which provide a clear advantage in the field of catalysis. Platinum-based catalysts are precious metal catalysts commonly used in the dehydrogenation of low-carbon alkanes, with excellent dehydrogenation activity and good catalytic activity for the anaerobic dehydrogenation of ethane. By lattice reconstruction strategy we grow PSC MgO from the parent MgF2 single crystal and load Pt nanoparticles on its surface for growing PSC Pt/MgO. Oxygen vacancies are introduced by constructing active sites on a clear surface structure, which improve catalytic activity and durability. The PSC Pt/MgO catalyst for the direct dehydrogenation of ethane achieves an ethane conversion rate of approximately 28% and ethylene selectivity of over 97%, with good stability over 100 h. The present work offers significant value for the growth and application of porous single crystal oxides loaded with metal nanoparticles.
2026, 37(8): 111328
doi: 10.1016/j.cclet.2025.111328
Abstract:
Metal-organic framework (MOF) derived metal oxides and their composites have shown remarkable potential in enhancing the sensitivity and lowering the detection limits of gas sensors, emerging as promising candidates for volatile organic compound (VOC) detection. Here, the Pt-sensitized In2O3 hollow microtubes were synthesized from MIL-68 via hydrothermal and sacrificial template methods, demonstrating exceptional trace detection capability (0.01–1 ppm) to p-xylene. The 2% Pt NPs-In2O3 showed the highest response of 68.7 at 50 ppb, with a theoretical detection limit as low as 0.027 ppb. The role of Pt was elucidated through comprehensive characterization, revealing that highly dispersed Pt nanoparticles form a well-defined interface with In2O3, enhancing gas adsorption, electron transfer, and reaction kinetics, thereby significantly boosting sensor performance. By integrating in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), this study provides fundamental insights into gas-solid interfacial sensing mechanisms, elucidating how Pt modulation enhances gas sensor performance at the molecular level. Additionally, the aging mechanisms of 2% Pt NPs-In2O3 sensors were explored through in situ characterization, revealing the evolution of surface morphology and gas adsorption capacity before and after aging under different conditions: 200 ℃/0% RH, 200 ℃/50% RH, and 250 ℃/0% RH for 20 days. These findings offer valuable guidance for improving the long-term stability and reliability of Pt-modified In2O3 gas sensors.
Metal-organic framework (MOF) derived metal oxides and their composites have shown remarkable potential in enhancing the sensitivity and lowering the detection limits of gas sensors, emerging as promising candidates for volatile organic compound (VOC) detection. Here, the Pt-sensitized In2O3 hollow microtubes were synthesized from MIL-68 via hydrothermal and sacrificial template methods, demonstrating exceptional trace detection capability (0.01–1 ppm) to p-xylene. The 2% Pt NPs-In2O3 showed the highest response of 68.7 at 50 ppb, with a theoretical detection limit as low as 0.027 ppb. The role of Pt was elucidated through comprehensive characterization, revealing that highly dispersed Pt nanoparticles form a well-defined interface with In2O3, enhancing gas adsorption, electron transfer, and reaction kinetics, thereby significantly boosting sensor performance. By integrating in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), this study provides fundamental insights into gas-solid interfacial sensing mechanisms, elucidating how Pt modulation enhances gas sensor performance at the molecular level. Additionally, the aging mechanisms of 2% Pt NPs-In2O3 sensors were explored through in situ characterization, revealing the evolution of surface morphology and gas adsorption capacity before and after aging under different conditions: 200 ℃/0% RH, 200 ℃/50% RH, and 250 ℃/0% RH for 20 days. These findings offer valuable guidance for improving the long-term stability and reliability of Pt-modified In2O3 gas sensors.
2026, 37(8): 111329
doi: 10.1016/j.cclet.2025.111329
Abstract:
Graphite, the most widely used anode material in lithium-ion batteries, faces significant limitations due to sluggish lithium-ion diffusion across the conventional organic solid electrolyte interphase (SEI) during cycling. In this work, we propose the incorporation of SO3Li-grafted graphene as an ion-conducting agent (ICA) to enhance lithium-ion transport kinetics within graphite anodes. The –SO3Li functional groups regulate the Li+ solvation structure through anion-solvent dipole interactions, promoting the formation of a lithium fluoride (LiF)-rich SEI that ensures uniform lithium-ion flux and significantly extends battery cycle life. This SO3Li-grafted ICA also mitigates mechanical strain within the graphite anode during repeated cycling, improving structural integrity over long-term operation, evidenced by fiber optic sensing technology. As a result, a 3 Ah GrLiFePO4 pouch cell incorporating this functionalized ion-conducting agent achieves excellent cycling performance, retaining 86.4% of its capacity after 1200 cycles at 1 C. These findings demonstrate the effectiveness of functionalized ICAs in addressing the intrinsic limitations of graphite, providing a promising strategy for developing long-life lithium-ion batteries for practical energy storage applications.
Graphite, the most widely used anode material in lithium-ion batteries, faces significant limitations due to sluggish lithium-ion diffusion across the conventional organic solid electrolyte interphase (SEI) during cycling. In this work, we propose the incorporation of SO3Li-grafted graphene as an ion-conducting agent (ICA) to enhance lithium-ion transport kinetics within graphite anodes. The –SO3Li functional groups regulate the Li+ solvation structure through anion-solvent dipole interactions, promoting the formation of a lithium fluoride (LiF)-rich SEI that ensures uniform lithium-ion flux and significantly extends battery cycle life. This SO3Li-grafted ICA also mitigates mechanical strain within the graphite anode during repeated cycling, improving structural integrity over long-term operation, evidenced by fiber optic sensing technology. As a result, a 3 Ah GrLiFePO4 pouch cell incorporating this functionalized ion-conducting agent achieves excellent cycling performance, retaining 86.4% of its capacity after 1200 cycles at 1 C. These findings demonstrate the effectiveness of functionalized ICAs in addressing the intrinsic limitations of graphite, providing a promising strategy for developing long-life lithium-ion batteries for practical energy storage applications.
2026, 37(8): 111349
doi: 10.1016/j.cclet.2025.111349
Abstract:
Lithium−oxygen (Li−O2) batteries exhibit a superior energy density compared with any other battery currently available on the market. However, the practical application has been impeded by the insulated, insoluble discharge product (Li2O2). The limitations caused by Li2O2 are hardly to be addressed through the conventional catalyst design, which relies on the electronic structure and interfacial charge transfer characteristics. Herein, a magnetic/thermal coupling assisted Li−O2 batteries based on the thermoelectric material of MoS2 and magnetism single atom cobalt (SA−Co/MoS2) was constructed for the first time, by combing the magnetic heating and the thermoelectric catalytic effect. The spin polarization of the single atom Co may be promoted and a magnetic heating effect is generated by an external magnetic field, speeding up the oxygen evolution process (OER) and oxygen reduction reaction (ORR), as well as promoting the parallel spin arrangement of oxygen atoms. Because of its special SA−Co/MoS2 cathode, the Li−O2 battery with magnetic/thermal coupling assistance offers an ultra-low charging platform of 3.33 V and an ultra-high discharge platform of 2.90 V. The proposed novel method of sustaining the magnetic and thermal fields provides a crucial guidance for adjusting the excessive overpotential in metal−air battery systems.
Lithium−oxygen (Li−O2) batteries exhibit a superior energy density compared with any other battery currently available on the market. However, the practical application has been impeded by the insulated, insoluble discharge product (Li2O2). The limitations caused by Li2O2 are hardly to be addressed through the conventional catalyst design, which relies on the electronic structure and interfacial charge transfer characteristics. Herein, a magnetic/thermal coupling assisted Li−O2 batteries based on the thermoelectric material of MoS2 and magnetism single atom cobalt (SA−Co/MoS2) was constructed for the first time, by combing the magnetic heating and the thermoelectric catalytic effect. The spin polarization of the single atom Co may be promoted and a magnetic heating effect is generated by an external magnetic field, speeding up the oxygen evolution process (OER) and oxygen reduction reaction (ORR), as well as promoting the parallel spin arrangement of oxygen atoms. Because of its special SA−Co/MoS2 cathode, the Li−O2 battery with magnetic/thermal coupling assistance offers an ultra-low charging platform of 3.33 V and an ultra-high discharge platform of 2.90 V. The proposed novel method of sustaining the magnetic and thermal fields provides a crucial guidance for adjusting the excessive overpotential in metal−air battery systems.
2026, 37(8): 111411
doi: 10.1016/j.cclet.2025.111411
Abstract:
A composite solid-state electrolyte with a triplex ionic transport architecture (TITA) was developed by integrating nanoscale fillers, short-chain crosslinkers and polymer matrix via solution casting and in situ photopolymerization. This structure creates efficient ion-conduction pathways, reduces ion aggregation, and enhances mechanical stability. As a result, the electrolyte achieves a high ionic conductivity of 7.36 × 10−4 S/cm and demonstrates excellent cycling performance when paired with an NCM622 cathode, showing great promise for solid-state lithium battery applications.
A composite solid-state electrolyte with a triplex ionic transport architecture (TITA) was developed by integrating nanoscale fillers, short-chain crosslinkers and polymer matrix via solution casting and in situ photopolymerization. This structure creates efficient ion-conduction pathways, reduces ion aggregation, and enhances mechanical stability. As a result, the electrolyte achieves a high ionic conductivity of 7.36 × 10−4 S/cm and demonstrates excellent cycling performance when paired with an NCM622 cathode, showing great promise for solid-state lithium battery applications.
2026, 37(8): 111479
doi: 10.1016/j.cclet.2025.111479
Abstract:
The key to electrolytic water includes two half-reaction processes: hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Transition metal phosphides (TMPs) are a class of prospective bifunctional electrocatalysts, but their performances are still far from the commercial catalysts. In this work, we design several kinds of Ni2P@CoP hetero-structured catalysts by the modification of Ru atom. The 0.1Ru-Ni2P@CoP catalyst presents the overpotentials of 82.7 (HER) and 245.3 mV (OER) at 10 mA/cm2 in 1 mol/L KOH solution. Moreover, it effectively promotes water splitting under alkaline conditions (ƞ10 = 1.21 V) and seawater conditions (ƞ10 = 1.13 V). The surface self-reconfiguration also makes it remain stable under prolonged cycling in both electrolytes. Density functional theory (DFT) calculations further indicate that doping engineering and heterostructures cause electronic modulation and electron transfer thereby increasing the intrinsic activity of the catalyst.
The key to electrolytic water includes two half-reaction processes: hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Transition metal phosphides (TMPs) are a class of prospective bifunctional electrocatalysts, but their performances are still far from the commercial catalysts. In this work, we design several kinds of Ni2P@CoP hetero-structured catalysts by the modification of Ru atom. The 0.1Ru-Ni2P@CoP catalyst presents the overpotentials of 82.7 (HER) and 245.3 mV (OER) at 10 mA/cm2 in 1 mol/L KOH solution. Moreover, it effectively promotes water splitting under alkaline conditions (ƞ10 = 1.21 V) and seawater conditions (ƞ10 = 1.13 V). The surface self-reconfiguration also makes it remain stable under prolonged cycling in both electrolytes. Density functional theory (DFT) calculations further indicate that doping engineering and heterostructures cause electronic modulation and electron transfer thereby increasing the intrinsic activity of the catalyst.
2026, 37(8): 111514
doi: 10.1016/j.cclet.2025.111514
Abstract:
To mitigate the slow conversion kinetics and "shuttle effect" of polysulfides, a flexible, self-supporting Ni-nitrilotriacetic acid coordination polymer nanowires/few layer Ti3C2Tx MXene (Ni-NTA/f-Ti3C2Tx) interlayers with three-dimensional network is elaborately devised and fabricated. In this framework, the M–O–M (M = metal ion) linkages on polymer nanowires present superior catalytic activity towards the conversion of lithium polysulfides (LiPSs). Meanwhile, physical blocking and chemical trapping of LiPSs are also achieved, owing to the hierarchical porous structure and polar surface of hybrid interlayer. As a result, the lithium sulfur batteries assembled with Ni-NTA/f-Ti3C2Tx exhibit a high specific capacity of 899.5 mAh/g at 1 C and 529.6 mAh/g can be kept after 500 cycles with a decay rate of 0.08% per cycle, confirming the efficient alleviation of shuttle effect.
To mitigate the slow conversion kinetics and "shuttle effect" of polysulfides, a flexible, self-supporting Ni-nitrilotriacetic acid coordination polymer nanowires/few layer Ti3C2Tx MXene (Ni-NTA/f-Ti3C2Tx) interlayers with three-dimensional network is elaborately devised and fabricated. In this framework, the M–O–M (M = metal ion) linkages on polymer nanowires present superior catalytic activity towards the conversion of lithium polysulfides (LiPSs). Meanwhile, physical blocking and chemical trapping of LiPSs are also achieved, owing to the hierarchical porous structure and polar surface of hybrid interlayer. As a result, the lithium sulfur batteries assembled with Ni-NTA/f-Ti3C2Tx exhibit a high specific capacity of 899.5 mAh/g at 1 C and 529.6 mAh/g can be kept after 500 cycles with a decay rate of 0.08% per cycle, confirming the efficient alleviation of shuttle effect.
2026, 37(8): 111751
doi: 10.1016/j.cclet.2025.111751
Abstract:
Coinfection with severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) and influenza virus exacerbates pulmonary inflammation and tissue damage, significantly increasing the risks of respiratory failure, acute respiratory distress syndrome (ARDS), and secondary bacterial infections. Currently, there are no approved therapeutic agents specifically targeting these two viruses' coinfection. Human dihydroorotate dehydrogenase (DHODH), a key enzyme catalyzing the fourth step in the de novo pyrimidine biosynthesis pathway through the oxidation of dihydroorotate to orotate, serves as the rate-limiting enzyme in pyrimidine biosynthesis. This critical metabolic checkpoint has emerged as a promising broad-spectrum antiviral target. In this study, we designed and synthesized a series of DHODH-targeting proteolysis-targeting chimeras (PROTACs), among which PROTACs 17 and 19 connected via flexible alkyl linkers were identified as the most potent molecules. Mechanistic investigations revealed that 17 and 19 induced DHODH degradation through the proteasome- and cereblon (CRBN)-dependent pathways. Remarkably, 17 and 19 exhibited significant antiviral activities against both influenza virus and SARS-CoV-2 in vitro. These findings collectively present a novel and effective strategy for the treatment of coinfection caused by SARS-CoV-2 and influenza virus.
Coinfection with severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) and influenza virus exacerbates pulmonary inflammation and tissue damage, significantly increasing the risks of respiratory failure, acute respiratory distress syndrome (ARDS), and secondary bacterial infections. Currently, there are no approved therapeutic agents specifically targeting these two viruses' coinfection. Human dihydroorotate dehydrogenase (DHODH), a key enzyme catalyzing the fourth step in the de novo pyrimidine biosynthesis pathway through the oxidation of dihydroorotate to orotate, serves as the rate-limiting enzyme in pyrimidine biosynthesis. This critical metabolic checkpoint has emerged as a promising broad-spectrum antiviral target. In this study, we designed and synthesized a series of DHODH-targeting proteolysis-targeting chimeras (PROTACs), among which PROTACs 17 and 19 connected via flexible alkyl linkers were identified as the most potent molecules. Mechanistic investigations revealed that 17 and 19 induced DHODH degradation through the proteasome- and cereblon (CRBN)-dependent pathways. Remarkably, 17 and 19 exhibited significant antiviral activities against both influenza virus and SARS-CoV-2 in vitro. These findings collectively present a novel and effective strategy for the treatment of coinfection caused by SARS-CoV-2 and influenza virus.
2026, 37(8): 111757
doi: 10.1016/j.cclet.2025.111757
Abstract:
Genetically encoded fluorescence (FL) sensors play vital roles in monitoring cell metabolism dynamics, gene transcription, DNA repair, apoptosis, and nutrient sensing. In genetically encoded FL sensors study, microscope acquires multimodal images that contain bright-field (BF) and FL images. BF and FL images can provide different information on cell phenotypes and gray level. Here, we developed an artificial intelligence (AI)-driven system “AI-cell metabolism dynamic analyzer (AI-CMDA)” for high-throughput automatically cell division metabolism dynamics processing by fusing multimodal information. The system consists of a deep learning model based on multimodal images dedicated to division nodes extraction and an adaptive correlation filter tracker for associating cell sequences. The division extraction method enables fast filtering of dividing cells without manual selection, and the adaptive correlation filter can achieve robust, accurate tracking during cell transforms with time. We apply the system with 3 genetically encoded FL sensors for nicotinamide adenine dinucleotides (NAD+/NADH) ratio, reduced nicotinamide adenine dinucleotide phosphate (NADPH) and H2O2, respectively, to monitor the redox metabolism within cell division sequences. The results show that this system can reduce the processing time to seconds compared with several hours’ manual labeling and can achieve accuracy and fastness.
Genetically encoded fluorescence (FL) sensors play vital roles in monitoring cell metabolism dynamics, gene transcription, DNA repair, apoptosis, and nutrient sensing. In genetically encoded FL sensors study, microscope acquires multimodal images that contain bright-field (BF) and FL images. BF and FL images can provide different information on cell phenotypes and gray level. Here, we developed an artificial intelligence (AI)-driven system “AI-cell metabolism dynamic analyzer (AI-CMDA)” for high-throughput automatically cell division metabolism dynamics processing by fusing multimodal information. The system consists of a deep learning model based on multimodal images dedicated to division nodes extraction and an adaptive correlation filter tracker for associating cell sequences. The division extraction method enables fast filtering of dividing cells without manual selection, and the adaptive correlation filter can achieve robust, accurate tracking during cell transforms with time. We apply the system with 3 genetically encoded FL sensors for nicotinamide adenine dinucleotides (NAD+/NADH) ratio, reduced nicotinamide adenine dinucleotide phosphate (NADPH) and H2O2, respectively, to monitor the redox metabolism within cell division sequences. The results show that this system can reduce the processing time to seconds compared with several hours’ manual labeling and can achieve accuracy and fastness.
2026, 37(8): 111758
doi: 10.1016/j.cclet.2025.111758
Abstract:
Adenomyosis remains a poorly understood condition characterized by the limited efficacy of current pharmacotherapy. Traditional treatments using dydrogesterone (DG) for adenomyosis often yield suboptimal outcomes due to poor targeting and susceptibility to immune rejection. Therefore, there is an urgent need to identify an effective approach to enhancing the therapeutic efficacy of DG. Given the enrichment of macrophages in the uterus associated with adenomyosis, this study sought to develop a supramolecular cell-based macrophage membrane-encapsulated DG nanoparticle (MM-DG-NP) delivery system for targeted drug delivery and effective treatment of adenomyosis. The MM-DG-NP system leverages a multifaceted therapeutic mechanism by evading phagocytic clearance and enhancing targeted drug delivery efficacy. The supramolecular cell framework, constructed through dynamic non-covalent interactions, provides structural stability and biofunctional adaptability to the MM-DG-NP system, enabling precise homing to uterine macrophage-rich pathological sites. The MM-DG-NP system demonstrated therapeutic efficacy superior to that of traditional DG therapy in murine models, characterized by a pronounced reduction in endometrial invasion depth within the myometrium; effective inhibition of epithelial–mesenchymal transition (EMT) progression in the glandular epithelium; significant attenuation of local inflammatory cytokine release in the uterus, including interleukin-6 (IL-6), tumor necrosis factor-alpha (TNF-α), and interferon-gamma (IFN-γ); and notable alleviation of pain responses. These results highlight the critical role of supramolecular cell engineering in enhancing the biocompatibility and targeting precision of nanomedicines. MM-DG-NPs thus represent a promising strategy for overcoming current pharmacotherapeutic limitations in adenomyosis, warranting further investigation to explore their potential clinical translation.
Adenomyosis remains a poorly understood condition characterized by the limited efficacy of current pharmacotherapy. Traditional treatments using dydrogesterone (DG) for adenomyosis often yield suboptimal outcomes due to poor targeting and susceptibility to immune rejection. Therefore, there is an urgent need to identify an effective approach to enhancing the therapeutic efficacy of DG. Given the enrichment of macrophages in the uterus associated with adenomyosis, this study sought to develop a supramolecular cell-based macrophage membrane-encapsulated DG nanoparticle (MM-DG-NP) delivery system for targeted drug delivery and effective treatment of adenomyosis. The MM-DG-NP system leverages a multifaceted therapeutic mechanism by evading phagocytic clearance and enhancing targeted drug delivery efficacy. The supramolecular cell framework, constructed through dynamic non-covalent interactions, provides structural stability and biofunctional adaptability to the MM-DG-NP system, enabling precise homing to uterine macrophage-rich pathological sites. The MM-DG-NP system demonstrated therapeutic efficacy superior to that of traditional DG therapy in murine models, characterized by a pronounced reduction in endometrial invasion depth within the myometrium; effective inhibition of epithelial–mesenchymal transition (EMT) progression in the glandular epithelium; significant attenuation of local inflammatory cytokine release in the uterus, including interleukin-6 (IL-6), tumor necrosis factor-alpha (TNF-α), and interferon-gamma (IFN-γ); and notable alleviation of pain responses. These results highlight the critical role of supramolecular cell engineering in enhancing the biocompatibility and targeting precision of nanomedicines. MM-DG-NPs thus represent a promising strategy for overcoming current pharmacotherapeutic limitations in adenomyosis, warranting further investigation to explore their potential clinical translation.
2026, 37(8): 111760
doi: 10.1016/j.cclet.2025.111760
Abstract:
Deubiquitinases (DUBs) that remove conjugated ubiquitin from substrates are critical regulators of protein homeostasis and cellular signaling. Understanding the spatial distribution of DUBs in subcellular compartments is essential for uncovering their roles in stress responses and disease pathogenesis. Herein, we developed an Escherichia coli (E. coli)-based biosynthetic strategy for the expedient generation of biotin-labeled ubiquitin probe (Biotin-Ub-PA) through co-expression of Avi-Ub and BirA in E. coli, thus bypassing tedious chemical synthesis. Combined with affinity purification and proteomics, we utilized the biosynthetic probe to covalently capture active DUBs in subcellular compartments and revealed the distribution of DUBs in the cytoplasm and nucleus. As a proof of concept, hydrogen peroxide-induced activity changes of DUBs in the cytoplasm and nucleus were analyzed by the same probe. The results suggest that some DUBs, such as ubiquitin-specific protease 36 (USP36) and USP16, may undergo subcellular translocation and activity alterations under oxidative stress. Our study presents a reliable workflow for the spatial distribution analysis of DUBs under different stimuli or disease conditions.
Deubiquitinases (DUBs) that remove conjugated ubiquitin from substrates are critical regulators of protein homeostasis and cellular signaling. Understanding the spatial distribution of DUBs in subcellular compartments is essential for uncovering their roles in stress responses and disease pathogenesis. Herein, we developed an Escherichia coli (E. coli)-based biosynthetic strategy for the expedient generation of biotin-labeled ubiquitin probe (Biotin-Ub-PA) through co-expression of Avi-Ub and BirA in E. coli, thus bypassing tedious chemical synthesis. Combined with affinity purification and proteomics, we utilized the biosynthetic probe to covalently capture active DUBs in subcellular compartments and revealed the distribution of DUBs in the cytoplasm and nucleus. As a proof of concept, hydrogen peroxide-induced activity changes of DUBs in the cytoplasm and nucleus were analyzed by the same probe. The results suggest that some DUBs, such as ubiquitin-specific protease 36 (USP36) and USP16, may undergo subcellular translocation and activity alterations under oxidative stress. Our study presents a reliable workflow for the spatial distribution analysis of DUBs under different stimuli or disease conditions.
2026, 37(8): 111771
doi: 10.1016/j.cclet.2025.111771
Abstract:
Triggering mitochondria-targeted ferroptosis is the effective way to bypass apoptotic resistance of sonodynamic therapy (SDT), but it suffers from discounted therapeutic efficacy due to the anti-ferroptosis mechanism via mitochondrial dihydroorotate dehydrogenase (DHODH). Herein, iron porphyrin-based nanometal organic frameworks (PCN-600) were synthesized by hydrothermal method for loading the ferroptosis inducer sulfasalazine (SAS) and DHODH inhibitor brequinar (BQR), and finally surface-modified with short chains of mitochondria-targeting triphenylphosphine (TPP) and long chains contained tumor-targeting groups of biotin that can be cleaved by intratumoral glutathione (GSH) to re-expose TPP. The nanosystem could be successfully delivered into the mitochondria of cancer cells which was an important location of cell apoptosis and ferroptosis, released SAS/BQR, and produced amounts of ROS under ultrasound activation to induce ferroptosis and overcome ferroptosis resistance for dual-synergism with apoptosis to enhance the anti-tumor efficacy of SDT both in vitro and in vivo. The GSH-activated mitochondria-targeting nanosystem for devasting mitochondrial anti-ferroptosis provides a novel method for ferroptosis-based enhancement of anti-tumor efficacy of SDT.
Triggering mitochondria-targeted ferroptosis is the effective way to bypass apoptotic resistance of sonodynamic therapy (SDT), but it suffers from discounted therapeutic efficacy due to the anti-ferroptosis mechanism via mitochondrial dihydroorotate dehydrogenase (DHODH). Herein, iron porphyrin-based nanometal organic frameworks (PCN-600) were synthesized by hydrothermal method for loading the ferroptosis inducer sulfasalazine (SAS) and DHODH inhibitor brequinar (BQR), and finally surface-modified with short chains of mitochondria-targeting triphenylphosphine (TPP) and long chains contained tumor-targeting groups of biotin that can be cleaved by intratumoral glutathione (GSH) to re-expose TPP. The nanosystem could be successfully delivered into the mitochondria of cancer cells which was an important location of cell apoptosis and ferroptosis, released SAS/BQR, and produced amounts of ROS under ultrasound activation to induce ferroptosis and overcome ferroptosis resistance for dual-synergism with apoptosis to enhance the anti-tumor efficacy of SDT both in vitro and in vivo. The GSH-activated mitochondria-targeting nanosystem for devasting mitochondrial anti-ferroptosis provides a novel method for ferroptosis-based enhancement of anti-tumor efficacy of SDT.
2026, 37(8): 111772
doi: 10.1016/j.cclet.2025.111772
Abstract:
The clinical application of photodynamic therapy (PDT) is usually limited by the low penetration depth of light and the hypoxic condition of tumor microenvironment. Therefore, it is urgent to develop a drug system that can activate photosensitizers (PSs) in deeply seated tumors and spontaneously generate O2 to enhance the efficacy of PDT. Herein, we design a liquid polyethylene glycol (PEG) 200 (PEG200)-based drug depot containing calcium peroxide (CaO2) nanoparticles, bis[2,4,5-trichloro-6-(pentyloxycarbonyl)phenyl]oxalate (CPPO, a high-energy compound), and chlorin e6 (Ce6, a PS) for achieving O2/H2O2 self-supplied chemiexcited (light irradiation-free) PDT and immunotherapy. By injecting the drug depot into the tumor, CaO2 can react with water to produce H2O2, which can activate CPPO to generate chemical energy, further stimulating Ce6 to produce 1O2. Meanwhile, CaO2 can also generate O2 to enhance PDT. Besides, CaO2 can neutralize the acidic tumor microenvironment by the formation of Ca(OH)2, cause calcium overload in tumor cells, and lead to tumor calcification. Further experiments show that CaO2, CPPO, and Ce6 can cause mitochondrial damage, trigger immunogenic cell death, and significantly improve the therapeutic effect of programmed death-1 (PD-1) monoclonal antibody. This work highlights the application potential of the rational combination of CaO2, CPPO, and Ce6 for realizing light irradiation-free PDT and immunotherapy.
The clinical application of photodynamic therapy (PDT) is usually limited by the low penetration depth of light and the hypoxic condition of tumor microenvironment. Therefore, it is urgent to develop a drug system that can activate photosensitizers (PSs) in deeply seated tumors and spontaneously generate O2 to enhance the efficacy of PDT. Herein, we design a liquid polyethylene glycol (PEG) 200 (PEG200)-based drug depot containing calcium peroxide (CaO2) nanoparticles, bis[2,4,5-trichloro-6-(pentyloxycarbonyl)phenyl]oxalate (CPPO, a high-energy compound), and chlorin e6 (Ce6, a PS) for achieving O2/H2O2 self-supplied chemiexcited (light irradiation-free) PDT and immunotherapy. By injecting the drug depot into the tumor, CaO2 can react with water to produce H2O2, which can activate CPPO to generate chemical energy, further stimulating Ce6 to produce 1O2. Meanwhile, CaO2 can also generate O2 to enhance PDT. Besides, CaO2 can neutralize the acidic tumor microenvironment by the formation of Ca(OH)2, cause calcium overload in tumor cells, and lead to tumor calcification. Further experiments show that CaO2, CPPO, and Ce6 can cause mitochondrial damage, trigger immunogenic cell death, and significantly improve the therapeutic effect of programmed death-1 (PD-1) monoclonal antibody. This work highlights the application potential of the rational combination of CaO2, CPPO, and Ce6 for realizing light irradiation-free PDT and immunotherapy.
2026, 37(8): 111773
doi: 10.1016/j.cclet.2025.111773
Abstract:
Accumulating evidence highlights the therapeutic potential of soluble epoxide hydrolase (sEH) inhibitors with anti-inflammatory and neuroprotective properties for Alzheimer’s disease (AD). In this work, an ent–atisane diterpenoid J12 was identified as a hit compound against sEH with moderate inhibitory activity from five distinct series of compounds (J1–J44) isolated from Excoecaria agallocha L. After rational structural modification, a novel sEH inhibitor HXY14 with improved sEH inhibitory activity (half maximal inhibitory concentration (IC50) = 1.6 µmol/L, 10-fold compared to J12) was obtained. The cellular thermal shift assay (CETSA) demonstrated direct binding of HXY14 to sEH. In an Aβ-induced neuroinflammation cell model, treatment with HXY14 increased epoxyeicosatrienoic acids (EETs) levels, leading to reduced neuroinflammation and concomitant neuroprotection. HXY14 could ameliorate memory impairment and exhibited cognitive improvement in Aβ1–42-induced AD model and exhibited preferable safety in vivo. Treatment with HXY14 significantly decreased the expression levels of inflammatory factors and attenuated microglia activation, thereby inhibiting neuroinflammation. Furthermore, HXY14 could promote neuroprotection and alleviate synaptic dysfunction in AD model mice. This study expands the discovery of novel naturally derived sEH inhibitors and provides evidence for the utility of sEH inhibitors for AD therapy.
Accumulating evidence highlights the therapeutic potential of soluble epoxide hydrolase (sEH) inhibitors with anti-inflammatory and neuroprotective properties for Alzheimer’s disease (AD). In this work, an ent–atisane diterpenoid J12 was identified as a hit compound against sEH with moderate inhibitory activity from five distinct series of compounds (J1–J44) isolated from Excoecaria agallocha L. After rational structural modification, a novel sEH inhibitor HXY14 with improved sEH inhibitory activity (half maximal inhibitory concentration (IC50) = 1.6 µmol/L, 10-fold compared to J12) was obtained. The cellular thermal shift assay (CETSA) demonstrated direct binding of HXY14 to sEH. In an Aβ-induced neuroinflammation cell model, treatment with HXY14 increased epoxyeicosatrienoic acids (EETs) levels, leading to reduced neuroinflammation and concomitant neuroprotection. HXY14 could ameliorate memory impairment and exhibited cognitive improvement in Aβ1–42-induced AD model and exhibited preferable safety in vivo. Treatment with HXY14 significantly decreased the expression levels of inflammatory factors and attenuated microglia activation, thereby inhibiting neuroinflammation. Furthermore, HXY14 could promote neuroprotection and alleviate synaptic dysfunction in AD model mice. This study expands the discovery of novel naturally derived sEH inhibitors and provides evidence for the utility of sEH inhibitors for AD therapy.
2026, 37(8): 111780
doi: 10.1016/j.cclet.2025.111780
Abstract:
Two novel anthrone–macrolide hybrids, neonectones A and B (1 and 2), one new 10-membered macrolide neonectone C (3), and one new oxaphenalenone derivative, (±)-neonectone D (4), together with five known compounds (5–9) were isolated from the crude extract of the ascomycete fungus Neonectria sp. Compounds 1 and 2 represent the first example of anthrone–ten-membered lactone heterodimers, possessing an unprecedented 5-(10-oxo-9,10-dihydroanthracen-9-yl)oxecane-2,7-dione skeleton. Their structures and absolute configurations were established by a combination of extensive spectroscopic analysis, 13C nuclear magnetic resonance spectroscopy (NMR) chemical shifts calculations with DP4+ probability analysis and electronic circular dichroism (ECD) calculations. Bioactivity evaluation revealed that compounds 1, 2 and 9 exhibited anti-methicillin-resistant Staphylococcus aureus (MRSA) activity. Compound 9 exhibited anti-MRSA activity through disrupting membrane integrity, suppressing energy and nucleotide metabolism, modulating membrane transport and transcription/translation regulatory factors, as well as inhibiting quorum sensing and biofilm formation.
Two novel anthrone–macrolide hybrids, neonectones A and B (1 and 2), one new 10-membered macrolide neonectone C (3), and one new oxaphenalenone derivative, (±)-neonectone D (4), together with five known compounds (5–9) were isolated from the crude extract of the ascomycete fungus Neonectria sp. Compounds 1 and 2 represent the first example of anthrone–ten-membered lactone heterodimers, possessing an unprecedented 5-(10-oxo-9,10-dihydroanthracen-9-yl)oxecane-2,7-dione skeleton. Their structures and absolute configurations were established by a combination of extensive spectroscopic analysis, 13C nuclear magnetic resonance spectroscopy (NMR) chemical shifts calculations with DP4+ probability analysis and electronic circular dichroism (ECD) calculations. Bioactivity evaluation revealed that compounds 1, 2 and 9 exhibited anti-methicillin-resistant Staphylococcus aureus (MRSA) activity. Compound 9 exhibited anti-MRSA activity through disrupting membrane integrity, suppressing energy and nucleotide metabolism, modulating membrane transport and transcription/translation regulatory factors, as well as inhibiting quorum sensing and biofilm formation.
2026, 37(8): 111786
doi: 10.1016/j.cclet.2025.111786
Abstract:
Inhibiting the contraction of cardiac myosin is an important strategy for treating hypertrophic cardiomyopathy (HCM). However, currently only MYK-461 has been approved for market, and its safety and pharmacokinetic (PK) properties still have deficiencies. Herein, we reported the discovery of a novel and potent cardiac myosin inhibitor Z5–11 through rational structural optimization of MYK-461. Compared with MYK-461, Z5–11 exhibited stronger inhibitory activity against myosin ATPase and could significantly inhibit myocardial cell contraction, as well as alleviate Ang Ⅱ-induced cardiac hypertrophy. The cytotoxicity assessment on rat myocardial cells showed that Z5–11 exhibited better safety than MYK-461. The PK study revealed that Z5–11 had reasonable half-life time (t1/2 = 2.74 h), and excellent oral bioavailability (F = 105.2%). More importantly, Z5–11 can effectively ameliorate transverse aortic constriction (TAC)-induced cardiac dysfunction and cardiac hypertrophy and remodeling in mice. These findings suggest that Z5–11 can be developed as a promising drug candidate for treating HCM.
Inhibiting the contraction of cardiac myosin is an important strategy for treating hypertrophic cardiomyopathy (HCM). However, currently only MYK-461 has been approved for market, and its safety and pharmacokinetic (PK) properties still have deficiencies. Herein, we reported the discovery of a novel and potent cardiac myosin inhibitor Z5–11 through rational structural optimization of MYK-461. Compared with MYK-461, Z5–11 exhibited stronger inhibitory activity against myosin ATPase and could significantly inhibit myocardial cell contraction, as well as alleviate Ang Ⅱ-induced cardiac hypertrophy. The cytotoxicity assessment on rat myocardial cells showed that Z5–11 exhibited better safety than MYK-461. The PK study revealed that Z5–11 had reasonable half-life time (t1/2 = 2.74 h), and excellent oral bioavailability (F = 105.2%). More importantly, Z5–11 can effectively ameliorate transverse aortic constriction (TAC)-induced cardiac dysfunction and cardiac hypertrophy and remodeling in mice. These findings suggest that Z5–11 can be developed as a promising drug candidate for treating HCM.
2026, 37(8): 111794
doi: 10.1016/j.cclet.2025.111794
Abstract:
Methamphetamine (METH) addiction represents a severe global public health crisis with currently limited therapeutic options, highlighting an urgent need for innovative approaches. Emerging evidence indicates that neuroinflammation, particularly microglial activation and subsequent cytokine release, significantly contributes to the neuropathology associated with METH use. Cannabidiol (CBD), a phytocannabinoid with promising anti-inflammatory and neuroprotective properties, has demonstrated therapeutic potential in mitigating METH-related neuroimmune responses. However, its clinical translation is severely restricted due to low bioavailability, rapid hepatic metabolism, and limited blood-brain barrier (BBB) penetration. To address these challenges, we developed a novel therapeutic platform utilizing exosomes derived from hypoxia-preconditioned human umbilical vein endothelial cells. These exosomes were loaded with CBD and surface-functionalized with the transcriptional activator protein (TAT) peptide, generating HP-Exo-CBD-TAT, to enhance brain targeting. Intranasal administration of HP-Exo-CBD-TAT significantly improved BBB penetration and brain accumulation compared to unmodified CBD-loaded exosomes (HP-Exo-CBD). In mouse models of METH addiction, treatment with HP-Exo-CBD-TAT markedly attenuated behavioral sensitization and conditioned place preference (CPP), two key indicators of addiction-like behaviors. The observed therapeutic effects correlated strongly with reductions in microglial activation and pro-inflammatory cytokine expression (interleukin-1β (IL-1β), IL-6, tumor necrosis factor-α (TNF-α)) in critical addiction-associated brain regions, such as the medial prefrontal cortex and ventral tegmental area. Importantly, even the carrier alone (HP-Exo-TAT) exhibited intrinsic immunomodulatory effects, underscoring the dual therapeutic action of this delivery system. Our findings highlight HP-Exo-CBD-TAT as a highly efficient, biocompatible, and non-invasive strategy that effectively targets neuroinflammation and addictive behaviors. This intranasal exosomal platform demonstrates significant translational promise for the clinical management of METH addiction.
Methamphetamine (METH) addiction represents a severe global public health crisis with currently limited therapeutic options, highlighting an urgent need for innovative approaches. Emerging evidence indicates that neuroinflammation, particularly microglial activation and subsequent cytokine release, significantly contributes to the neuropathology associated with METH use. Cannabidiol (CBD), a phytocannabinoid with promising anti-inflammatory and neuroprotective properties, has demonstrated therapeutic potential in mitigating METH-related neuroimmune responses. However, its clinical translation is severely restricted due to low bioavailability, rapid hepatic metabolism, and limited blood-brain barrier (BBB) penetration. To address these challenges, we developed a novel therapeutic platform utilizing exosomes derived from hypoxia-preconditioned human umbilical vein endothelial cells. These exosomes were loaded with CBD and surface-functionalized with the transcriptional activator protein (TAT) peptide, generating HP-Exo-CBD-TAT, to enhance brain targeting. Intranasal administration of HP-Exo-CBD-TAT significantly improved BBB penetration and brain accumulation compared to unmodified CBD-loaded exosomes (HP-Exo-CBD). In mouse models of METH addiction, treatment with HP-Exo-CBD-TAT markedly attenuated behavioral sensitization and conditioned place preference (CPP), two key indicators of addiction-like behaviors. The observed therapeutic effects correlated strongly with reductions in microglial activation and pro-inflammatory cytokine expression (interleukin-1β (IL-1β), IL-6, tumor necrosis factor-α (TNF-α)) in critical addiction-associated brain regions, such as the medial prefrontal cortex and ventral tegmental area. Importantly, even the carrier alone (HP-Exo-TAT) exhibited intrinsic immunomodulatory effects, underscoring the dual therapeutic action of this delivery system. Our findings highlight HP-Exo-CBD-TAT as a highly efficient, biocompatible, and non-invasive strategy that effectively targets neuroinflammation and addictive behaviors. This intranasal exosomal platform demonstrates significant translational promise for the clinical management of METH addiction.
2026, 37(8): 111799
doi: 10.1016/j.cclet.2025.111799
Abstract:
Prostate cancer poses a severe threat to the health of middle-aged and elderly males. In recent years, the development and clinical utilization of prostate-specific membrane antigen (PSMA)-targeted agents have significantly expanded diagnostic options for this malignancy. However, tumor heterogeneity substantially compromises the efficacy of radionuclide therapy, necessitating the exploration of multi-target strategies as potential solutions. This study presents a novel heterodimeric construct engineered for prostate cancer management, labeled with both diagnostic and therapeutic radionuclides to enable concurrent application in positron emission computed tomography (PET) imaging and radionuclide therapy. Our investigation primarily evaluates the therapeutic efficacy of ultra-low-dose (3.7 MBq) radionuclide therapy combined with anti-programmed cell death protein-1 (PD-1) antibody immunotherapy. In the RM-1 prostate cancer model with elevated PSMA expression, we have validated that the combination of ultra-low-dose radionuclide treatment and anti-PD-1 antibody immunotherapy yields superior therapeutic outcomes. Notably, compared to the immunotherapy-only group, the combination regimen elicited a significant increase in dendritic cells (DCs) and natural killer (NK) cells populations, with enhancements ranging from 32% to 103%. This ultra-low-dose radioimmunotherapy strategy offers a valuable theoretical framework for clinical translation, holding promise for further enhancing therapeutic efficacy in prostate cancer treatment.
Prostate cancer poses a severe threat to the health of middle-aged and elderly males. In recent years, the development and clinical utilization of prostate-specific membrane antigen (PSMA)-targeted agents have significantly expanded diagnostic options for this malignancy. However, tumor heterogeneity substantially compromises the efficacy of radionuclide therapy, necessitating the exploration of multi-target strategies as potential solutions. This study presents a novel heterodimeric construct engineered for prostate cancer management, labeled with both diagnostic and therapeutic radionuclides to enable concurrent application in positron emission computed tomography (PET) imaging and radionuclide therapy. Our investigation primarily evaluates the therapeutic efficacy of ultra-low-dose (3.7 MBq) radionuclide therapy combined with anti-programmed cell death protein-1 (PD-1) antibody immunotherapy. In the RM-1 prostate cancer model with elevated PSMA expression, we have validated that the combination of ultra-low-dose radionuclide treatment and anti-PD-1 antibody immunotherapy yields superior therapeutic outcomes. Notably, compared to the immunotherapy-only group, the combination regimen elicited a significant increase in dendritic cells (DCs) and natural killer (NK) cells populations, with enhancements ranging from 32% to 103%. This ultra-low-dose radioimmunotherapy strategy offers a valuable theoretical framework for clinical translation, holding promise for further enhancing therapeutic efficacy in prostate cancer treatment.
2026, 37(8): 111800
doi: 10.1016/j.cclet.2025.111800
Abstract:
Hydrogen sulfide (H2S), a gaseous signaling molecule with diverse biological functions, exhibits abnormal concentrations that are closely associated with arthritic pathogenesis and serve as a characteristic indicator of protein-rich food spoilage. To address the need for reliable H2S detection, this study developed a novel fluorescent probe, BHP-PC, by rationally integrating methylene blue and benzothiazole fluorophores. The probe demonstrates remarkable spectral separation (215 nm) and high selectivity, enabling simultaneous monitoring of fluorescence signals in both blue (detection limit: 12.5 nmol/L) and red (detection limit: 22.6 nmol/L) channels for highly sensitive H2S quantification. BHP-PC exhibits excellent dual-color imaging capabilities in both cellular and zebrafish models. The distinct colorimetric response facilitated the successful development of test strips for practical H2S detection in spoiled proteinaceous samples. Furthermore, the probe’s application in a λ-carrageenan-induced murine arthritis model enabled real-time H2S visualization, demonstrating its potential as an analytical tool for arthritis diagnosis and therapeutic monitoring.
Hydrogen sulfide (H2S), a gaseous signaling molecule with diverse biological functions, exhibits abnormal concentrations that are closely associated with arthritic pathogenesis and serve as a characteristic indicator of protein-rich food spoilage. To address the need for reliable H2S detection, this study developed a novel fluorescent probe, BHP-PC, by rationally integrating methylene blue and benzothiazole fluorophores. The probe demonstrates remarkable spectral separation (215 nm) and high selectivity, enabling simultaneous monitoring of fluorescence signals in both blue (detection limit: 12.5 nmol/L) and red (detection limit: 22.6 nmol/L) channels for highly sensitive H2S quantification. BHP-PC exhibits excellent dual-color imaging capabilities in both cellular and zebrafish models. The distinct colorimetric response facilitated the successful development of test strips for practical H2S detection in spoiled proteinaceous samples. Furthermore, the probe’s application in a λ-carrageenan-induced murine arthritis model enabled real-time H2S visualization, demonstrating its potential as an analytical tool for arthritis diagnosis and therapeutic monitoring.
2026, 37(8): 111812
doi: 10.1016/j.cclet.2025.111812
Abstract:
Ovarian cancer (OC) manifests the second deadliest gynecologic malignancy and shows severe conventional therapies-resistance, underscoring the urgent need for new therapeutic interventions. Disulfidptosis, caused in solute carrier family 7 member 11 (SLC7A11)-overexpressing (SLC7A11high) cancer cells under glucose deficiency, has emerged as an appealing alternative approach. Herein we identified the significantly high expression of SLC7A11 in OC, and demonstrated that disulfidptosis induced by 6-aminonicotinamide (6-AN) effectively kill SLC7A11high OC cells. Hence, to enhance the therapeutic effect of 6-AN, we engineered a novel nanodrug, FA-L@AI, utilizing folic acid (FA)-modified liposome, and also illustrated the detailed therapeutic mechanism. Upon exposed to FA-L@AI, SLC7A11high OC cells endured internal nicotinamide adenine dinucleotide phosphate (NADPH) pools deleting, which leads to cystine accumulations. The elevated cystine levels resulted in disulfide bonds formation in actin cytoskeletal protein, ultimately triggering disulfidptosis. FA-L@AI nanoparticles exhibited an impactful suppression of tumor cells growth through 6-AN-induced disulfidptosis both in vitro and in vivo. Consistently, mRNA transcriptomic analysis further elucidated the underlying mechanism of disulfidptosis. Altogether, our work displays a unique strategy mediating disulfidptosis for OC specific therapy.
Ovarian cancer (OC) manifests the second deadliest gynecologic malignancy and shows severe conventional therapies-resistance, underscoring the urgent need for new therapeutic interventions. Disulfidptosis, caused in solute carrier family 7 member 11 (SLC7A11)-overexpressing (SLC7A11high) cancer cells under glucose deficiency, has emerged as an appealing alternative approach. Herein we identified the significantly high expression of SLC7A11 in OC, and demonstrated that disulfidptosis induced by 6-aminonicotinamide (6-AN) effectively kill SLC7A11high OC cells. Hence, to enhance the therapeutic effect of 6-AN, we engineered a novel nanodrug, FA-L@AI, utilizing folic acid (FA)-modified liposome, and also illustrated the detailed therapeutic mechanism. Upon exposed to FA-L@AI, SLC7A11high OC cells endured internal nicotinamide adenine dinucleotide phosphate (NADPH) pools deleting, which leads to cystine accumulations. The elevated cystine levels resulted in disulfide bonds formation in actin cytoskeletal protein, ultimately triggering disulfidptosis. FA-L@AI nanoparticles exhibited an impactful suppression of tumor cells growth through 6-AN-induced disulfidptosis both in vitro and in vivo. Consistently, mRNA transcriptomic analysis further elucidated the underlying mechanism of disulfidptosis. Altogether, our work displays a unique strategy mediating disulfidptosis for OC specific therapy.
2026, 37(8): 111818
doi: 10.1016/j.cclet.2025.111818
Abstract:
Calcitonin (CT), a 32-amino acid polypeptide drug, is crucial in regulating calcium homeostasis and inhibiting osteoclast activity. CT is primarily administered via injections and nasal sprays. However, injections usually suffer from poor patient compliance, while nasal sprays may cause side effects such as epistaxis, rhinitis, and nasal mucosal ulcers, coupled with low bioavailability. Deep eutectic solvents (DESs), formed by hydrogen-bond donors and acceptors, have shown potential in overcoming intestinal permeability barriers and facilitating the oral delivery of peptide drugs. Herein, we developed an intestinal drug delivery system for CT using DESs, which is expected to facilitate the subsequent development of oral preparations. We first prepared and characterized DESs with different stoichiometric ratios of choline (Ch) and geranate (Ge), followed by the investigation of the interaction between CT and Ch-Ge-based DESs (CAGE). Intestinal transport studies revealed that CAGE significantly promoted the jejunal absorption of CT-CAGE 1:2 (Ch and Ge in a 1:2 ratio), exhibiting the most pronounced pro-permeability effect. In vivo pharmacokinetic and pharmacodynamic results indicated that, compared with the aqueous CT solution, the CT-CAGE formulation increased bioavailability to 3.53%, with a significant hypocalcemic effect. In vitro studies further demonstrated that CAGE increased the transmembrane transport and membrane permeability of CT. The pro-permeability mechanism of CAGE may be related to the opening of tight junctions between intestinal cells and the improvement of paracellular transport efficiency. This DES-based drug delivery system offers a novel and promising approach for the oral delivery design of CT, addressing the limitations of administration routes.
Calcitonin (CT), a 32-amino acid polypeptide drug, is crucial in regulating calcium homeostasis and inhibiting osteoclast activity. CT is primarily administered via injections and nasal sprays. However, injections usually suffer from poor patient compliance, while nasal sprays may cause side effects such as epistaxis, rhinitis, and nasal mucosal ulcers, coupled with low bioavailability. Deep eutectic solvents (DESs), formed by hydrogen-bond donors and acceptors, have shown potential in overcoming intestinal permeability barriers and facilitating the oral delivery of peptide drugs. Herein, we developed an intestinal drug delivery system for CT using DESs, which is expected to facilitate the subsequent development of oral preparations. We first prepared and characterized DESs with different stoichiometric ratios of choline (Ch) and geranate (Ge), followed by the investigation of the interaction between CT and Ch-Ge-based DESs (CAGE). Intestinal transport studies revealed that CAGE significantly promoted the jejunal absorption of CT-CAGE 1:2 (Ch and Ge in a 1:2 ratio), exhibiting the most pronounced pro-permeability effect. In vivo pharmacokinetic and pharmacodynamic results indicated that, compared with the aqueous CT solution, the CT-CAGE formulation increased bioavailability to 3.53%, with a significant hypocalcemic effect. In vitro studies further demonstrated that CAGE increased the transmembrane transport and membrane permeability of CT. The pro-permeability mechanism of CAGE may be related to the opening of tight junctions between intestinal cells and the improvement of paracellular transport efficiency. This DES-based drug delivery system offers a novel and promising approach for the oral delivery design of CT, addressing the limitations of administration routes.
2026, 37(8): 111835
doi: 10.1016/j.cclet.2025.111835
Abstract:
Colorectal cancer (CRC) is one of the most prevalent malignancies worldwide, frequently presenting with metastatic progression to the liver. A hallmark of CRC is redox dysregulation, characterized by elevated levels of γ-glutamyl transferase (GGT) and hypochlorite (ClO−). However, bioluminescent probes capable of simultaneously detecting GGT and ClO− for sensitive in vivo CRC diagnosis and ex vivo fecal analysis remain lacking. Herein, we report a novel dual-locked bioluminescent probe, GClO-luc, designed for the simultaneous detection of GGT and ClO− in CRC and stool testing. GClO-luc remains silent until sequentially activated by GGT and ClO−, generating a turn-on bioluminescence response in both aqueous solution and fLuc-transfected CT26 cells. Notably, this probe enabled real-time visualization of small tumors in both CRC and colorectal cancer liver metastasis (CRLM) mouse models, achieving high signal-to-background ratios of 65:1 and 41:1, respectively. Moreover, GClO-luc was successfully applied to fecal analysis, showing significantly higher bioluminescence intensity in the feces from CRC and CRLM mice. These findings demonstrate that GClO-luc represents a powerful dual-responsive diagnostic tool for cancer diagnosis and stool examinations.
Colorectal cancer (CRC) is one of the most prevalent malignancies worldwide, frequently presenting with metastatic progression to the liver. A hallmark of CRC is redox dysregulation, characterized by elevated levels of γ-glutamyl transferase (GGT) and hypochlorite (ClO−). However, bioluminescent probes capable of simultaneously detecting GGT and ClO− for sensitive in vivo CRC diagnosis and ex vivo fecal analysis remain lacking. Herein, we report a novel dual-locked bioluminescent probe, GClO-luc, designed for the simultaneous detection of GGT and ClO− in CRC and stool testing. GClO-luc remains silent until sequentially activated by GGT and ClO−, generating a turn-on bioluminescence response in both aqueous solution and fLuc-transfected CT26 cells. Notably, this probe enabled real-time visualization of small tumors in both CRC and colorectal cancer liver metastasis (CRLM) mouse models, achieving high signal-to-background ratios of 65:1 and 41:1, respectively. Moreover, GClO-luc was successfully applied to fecal analysis, showing significantly higher bioluminescence intensity in the feces from CRC and CRLM mice. These findings demonstrate that GClO-luc represents a powerful dual-responsive diagnostic tool for cancer diagnosis and stool examinations.
2026, 37(8): 111836
doi: 10.1016/j.cclet.2025.111836
Abstract:
Inflammatory bowel disease (IBD) exhibits pathological heterogeneity driven by multifactorial origins and patient variability, posing therapeutic challenges due to divergent immune microenvironment dynamics. Notably, neutrophils and macrophages showed prominent heterogeneity in IBD patients and underwent different reprogramming during the acute and chronic inflammatory phases. To address this pathological complexity, an orally administered TH@PVP-gel system integrating tanshinone IIA (Tan) and hemin (Hem) was engineered to address the heterogeneity of IBD pathology with the aim of achieving multi-targeted modulation of IBD. TH@PVP-gel specifically promoted neutrophil apoptosis and facilitated macrophage M2 polarization in the inflamed environment of the colon, targeting inflammatory heterogeneity and remodeling the inflammatory environment. In addition, the TH@PVP-gel efficiently scavenged reactive oxygen species (ROS), inhibited the death of colonic epithelial cells, and restored the intestinal barrier. Ultimately, the TH@PVP-gel demonstrated excellent therapeutic efficacy in both acute and chronic colitis, providing a potential strategy for the broad-spectrum treatment of IBD.
Inflammatory bowel disease (IBD) exhibits pathological heterogeneity driven by multifactorial origins and patient variability, posing therapeutic challenges due to divergent immune microenvironment dynamics. Notably, neutrophils and macrophages showed prominent heterogeneity in IBD patients and underwent different reprogramming during the acute and chronic inflammatory phases. To address this pathological complexity, an orally administered TH@PVP-gel system integrating tanshinone IIA (Tan) and hemin (Hem) was engineered to address the heterogeneity of IBD pathology with the aim of achieving multi-targeted modulation of IBD. TH@PVP-gel specifically promoted neutrophil apoptosis and facilitated macrophage M2 polarization in the inflamed environment of the colon, targeting inflammatory heterogeneity and remodeling the inflammatory environment. In addition, the TH@PVP-gel efficiently scavenged reactive oxygen species (ROS), inhibited the death of colonic epithelial cells, and restored the intestinal barrier. Ultimately, the TH@PVP-gel demonstrated excellent therapeutic efficacy in both acute and chronic colitis, providing a potential strategy for the broad-spectrum treatment of IBD.
2026, 37(8): 111837
doi: 10.1016/j.cclet.2025.111837
Abstract:
The combination of sonodynamic therapy (SDT) and immunotherapy exhibits potent anticancer efficacy. However, most sonosensitizers produce reactive oxygen species (ROS) with low efficiency under ultrasound (US). Chemotherapy-induced immunogenic cell death (ICD) is also plagued by toxic side effects, suboptimal efficacy, and immune escape. Herein, we developed a cancer therapy platform based on a sonosensitizer, iron porphyrin (Fe(Ⅲ) meso-tetra(4-carboxyphenyl)porphine chloride, FeTCPPCl), which self-assembles into a hydrogen-bonded organic framework (PHOF-1). This platform enables precise activation and spatiotemporal controlled release of prodrugs, thereby inducing ICD efficiently and safely. Specifically, PHOF-1 bioorthogonally activates the doxorubicin prodrug (pro-DOX) in situ, synergizing with sonodynamic immunotherapy. This strategy, which combines SDT with in situ prodrug activation, minimizes drug side effects and maximizes therapeutic effects. Additionally, this system activates the metformin (Glucophage) prodrug (pro-MET), with ATP depletion leading to upregulated adenosine monophosphate activated protein kinase (AMPK) expression, increased programmed death-ligand 1 (PD-L1) degradation, and reversal of tumor immunosuppression. Remarkably, SDT combined with bioorthogonal in situ immune activation represents a novel approach to enhance cancer immunotherapy. This synergy effectively converts "cold" tumors into "hot" tumors by promoting ICD and reducing PD-L1 expression, thereby improving immunotherapy efficacy. The integration of SDT and bioorthogonal chemistry offers a controllable therapeutic strategy with reduced immune-related adverse effects, providing a promising avenue for safer and more effective cancer immunotherapy through the induction of adaptive antitumor immunity.
The combination of sonodynamic therapy (SDT) and immunotherapy exhibits potent anticancer efficacy. However, most sonosensitizers produce reactive oxygen species (ROS) with low efficiency under ultrasound (US). Chemotherapy-induced immunogenic cell death (ICD) is also plagued by toxic side effects, suboptimal efficacy, and immune escape. Herein, we developed a cancer therapy platform based on a sonosensitizer, iron porphyrin (Fe(Ⅲ) meso-tetra(4-carboxyphenyl)porphine chloride, FeTCPPCl), which self-assembles into a hydrogen-bonded organic framework (PHOF-1). This platform enables precise activation and spatiotemporal controlled release of prodrugs, thereby inducing ICD efficiently and safely. Specifically, PHOF-1 bioorthogonally activates the doxorubicin prodrug (pro-DOX) in situ, synergizing with sonodynamic immunotherapy. This strategy, which combines SDT with in situ prodrug activation, minimizes drug side effects and maximizes therapeutic effects. Additionally, this system activates the metformin (Glucophage) prodrug (pro-MET), with ATP depletion leading to upregulated adenosine monophosphate activated protein kinase (AMPK) expression, increased programmed death-ligand 1 (PD-L1) degradation, and reversal of tumor immunosuppression. Remarkably, SDT combined with bioorthogonal in situ immune activation represents a novel approach to enhance cancer immunotherapy. This synergy effectively converts "cold" tumors into "hot" tumors by promoting ICD and reducing PD-L1 expression, thereby improving immunotherapy efficacy. The integration of SDT and bioorthogonal chemistry offers a controllable therapeutic strategy with reduced immune-related adverse effects, providing a promising avenue for safer and more effective cancer immunotherapy through the induction of adaptive antitumor immunity.
2026, 37(8): 111841
doi: 10.1016/j.cclet.2025.111841
Abstract:
Rapid hemostasis is a paramount issue in tissue wound repair treatment. Currently, hydrophilic hemostatic materials are favored for their absorption concentration capabilities in achieving swift hemostasis. However, the subsequent adherence of these materials to the wound presents another challenge, impacting the overall therapeutic outcome. Here, we reported a flexible electrospinning membrane (75D-P) composed of polyacrylonitrile (PAN) and diatom biosilica (DB), which integrated the submicron-sized pores of fiber membranes with the hierarchical porous structure of DB. It exhibited weak interfacial hydrophobicity, enabling rapid plasma protein adsorption capacity and accelerating blood coagulation at the material interface. The clotting time of kaolin commercial hemostatic agent-QuikClot® (QC) was 200 s, and that of 75D-P was 100 s, with the minimum tissue adhesion (0.06 N). Importantly, in the rabbit injury models, the dosage of the 75D-P was far below that of the QC group, yet it maintained comparable clotting time (about 400 s) and blood loss (4 g). We have integrated DB and PAN in electrospinning membrane could achieve a distinct water repellenting separation effect on blood components, promoting efficient interfacial blood coagulation. These offer insights into facilitating the blood clots formation at interfacial, thereby mitigating excessive material blood absorption and tissue adhesion.
Rapid hemostasis is a paramount issue in tissue wound repair treatment. Currently, hydrophilic hemostatic materials are favored for their absorption concentration capabilities in achieving swift hemostasis. However, the subsequent adherence of these materials to the wound presents another challenge, impacting the overall therapeutic outcome. Here, we reported a flexible electrospinning membrane (75D-P) composed of polyacrylonitrile (PAN) and diatom biosilica (DB), which integrated the submicron-sized pores of fiber membranes with the hierarchical porous structure of DB. It exhibited weak interfacial hydrophobicity, enabling rapid plasma protein adsorption capacity and accelerating blood coagulation at the material interface. The clotting time of kaolin commercial hemostatic agent-QuikClot® (QC) was 200 s, and that of 75D-P was 100 s, with the minimum tissue adhesion (0.06 N). Importantly, in the rabbit injury models, the dosage of the 75D-P was far below that of the QC group, yet it maintained comparable clotting time (about 400 s) and blood loss (4 g). We have integrated DB and PAN in electrospinning membrane could achieve a distinct water repellenting separation effect on blood components, promoting efficient interfacial blood coagulation. These offer insights into facilitating the blood clots formation at interfacial, thereby mitigating excessive material blood absorption and tissue adhesion.
2026, 37(8): 111852
doi: 10.1016/j.cclet.2025.111852
Abstract:
Synergistic strategy of cationic antibacterial and nanoparticle mediated photothermal conversion provides new opportunities to address bacterial infections. However, the conventional post-modification and lack of precise structural regulation, leads to the complexity of operation and unsatisfying synergistic effect on antibacterial performance. To address these challenges, herein, a novel "selective extraction and domain-restricted growth" approach has been proposed to successfully synthesize quaternized mesoporous silica nanosphere (QMSN) encapsulating gold nanorods (GNRs) inside the pore channel (GNRs@QMSN) for the treatment of bacterial infected diabetic wound. The strategy exhibits extensive convenience, enabling the ultra-uniform microporous core-mesoporous shell structure with positive charges. Most importantly, GNRs@QMSN demonstrated an excellent photothermal conversion efficiency up to 63.73%, due to the unique pore-domain-limited effect. Under the synergistic effect of positive charge surface for enhanced bacteria adhesion, intrinsic antibacterial quaternization and GNRs-mediated photothermal conversion, GNRs@QMSN exhibited excellent antibacterial and antibiofilm performance in vitro. The feasibility of GNRs@QMSN was further validated in a mouse diabetic wound infection model. This novel QMSN encapsulating GNRs is expected to be a promising paradigm for bacterial infected wound healing.
Synergistic strategy of cationic antibacterial and nanoparticle mediated photothermal conversion provides new opportunities to address bacterial infections. However, the conventional post-modification and lack of precise structural regulation, leads to the complexity of operation and unsatisfying synergistic effect on antibacterial performance. To address these challenges, herein, a novel "selective extraction and domain-restricted growth" approach has been proposed to successfully synthesize quaternized mesoporous silica nanosphere (QMSN) encapsulating gold nanorods (GNRs) inside the pore channel (GNRs@QMSN) for the treatment of bacterial infected diabetic wound. The strategy exhibits extensive convenience, enabling the ultra-uniform microporous core-mesoporous shell structure with positive charges. Most importantly, GNRs@QMSN demonstrated an excellent photothermal conversion efficiency up to 63.73%, due to the unique pore-domain-limited effect. Under the synergistic effect of positive charge surface for enhanced bacteria adhesion, intrinsic antibacterial quaternization and GNRs-mediated photothermal conversion, GNRs@QMSN exhibited excellent antibacterial and antibiofilm performance in vitro. The feasibility of GNRs@QMSN was further validated in a mouse diabetic wound infection model. This novel QMSN encapsulating GNRs is expected to be a promising paradigm for bacterial infected wound healing.
2026, 37(8): 111868
doi: 10.1016/j.cclet.2025.111868
Abstract:
Aqueous Zn//MnO2 batteries with Mn2+/MnO2 conversion reactions are highly promising due to their high redox potential and low cost. Typically, the conversion of Mn2+/MnO2 occurs at a strong acidic environment to ensure sufficient proton participation in the reaction, which will lead to Zn anode corrosion and electrolyte decomposition. Here, an acid-free mild electrolyte with Al2(SO4)3 as the additive to trigger Mn2+/MnO2 conversion through the hydrolysis of Al3+. This approach not only provides protons to enhance the two-electron transfer reaction but also utilizes the electrostatic shielding effect of Al3+ effectively inhibiting the formation of Zn dendrites and protecting the Zn anode. As a result, the assembled aqueous Zn//MnO2 battery exhibits high discharge voltage (1.6 V), long cycling stability (1900 cycles without decay) and excellent rate performance. Meanwhile, the anode-friendly electrolyte facilitates stable Zn plating/stripping and high Coulombic efficiency. This work proposes an effective strategy for enabling the two-electron process of MnO2 in mild aqueous Zn batteries.
Aqueous Zn//MnO2 batteries with Mn2+/MnO2 conversion reactions are highly promising due to their high redox potential and low cost. Typically, the conversion of Mn2+/MnO2 occurs at a strong acidic environment to ensure sufficient proton participation in the reaction, which will lead to Zn anode corrosion and electrolyte decomposition. Here, an acid-free mild electrolyte with Al2(SO4)3 as the additive to trigger Mn2+/MnO2 conversion through the hydrolysis of Al3+. This approach not only provides protons to enhance the two-electron transfer reaction but also utilizes the electrostatic shielding effect of Al3+ effectively inhibiting the formation of Zn dendrites and protecting the Zn anode. As a result, the assembled aqueous Zn//MnO2 battery exhibits high discharge voltage (1.6 V), long cycling stability (1900 cycles without decay) and excellent rate performance. Meanwhile, the anode-friendly electrolyte facilitates stable Zn plating/stripping and high Coulombic efficiency. This work proposes an effective strategy for enabling the two-electron process of MnO2 in mild aqueous Zn batteries.
2026, 37(8): 111877
doi: 10.1016/j.cclet.2025.111877
Abstract:
Vitiligo is a chronic autoimmune disorder characterized by progressive melanocyte loss. Conventional narrowband ultraviolet B (NB-UVB) phototherapy for vitiligo faces limitations due to reactive oxygen species (ROS)-induced phototoxicity and insufficient melanocyte regeneration in chronic applications. In this study, we propose a differential dual-release bilayer microneedle loaded with two natural plant-derived polyphenols nanoparticles, which integrates rapid antioxidant defense and sustained melanogenic reprogramming for precision vitiligo phototherapy. The upper layer, composed of hyaluronic acid (HA), encapsulates curcumin-fructose self-assembled nanomicelles (CF NMs) for rapid ROS scavenging (68.50% within 15 min), to prevent photodamage and nuclear factor kappa-light-chain-enhancer of activated B cells (NF-κB)-mediated inflammation. The lower gelatin methacryloyl (GelMA) hydrogel layer sustains the release of psoralen-loaded melanin-mimetic mesoporous polydopamine nanoparticles (PMPN), which persistently inhibits the Janus kinase-signal transducer and activator of transcription (JAK-STAT) signaling pathway and reduces autophagy-induced apoptosis, while enhancing tyrosinase activity (0.47-fold increase) to promote melanogenesis. In monobenzone-induced vitiligo mice, the CF/HA-PMPN/GelMA-MNs combined with NB-UVB demonstrated superior outcomes with 80.55% repigmentation at day 14 (vs. 25.90% in NB-UVB alone). This "rapid defense-sustained regeneration" paradigm provides a clinically translatable strategy to enhance efficacy and safety in vitiligo phototherapy.
Vitiligo is a chronic autoimmune disorder characterized by progressive melanocyte loss. Conventional narrowband ultraviolet B (NB-UVB) phototherapy for vitiligo faces limitations due to reactive oxygen species (ROS)-induced phototoxicity and insufficient melanocyte regeneration in chronic applications. In this study, we propose a differential dual-release bilayer microneedle loaded with two natural plant-derived polyphenols nanoparticles, which integrates rapid antioxidant defense and sustained melanogenic reprogramming for precision vitiligo phototherapy. The upper layer, composed of hyaluronic acid (HA), encapsulates curcumin-fructose self-assembled nanomicelles (CF NMs) for rapid ROS scavenging (68.50% within 15 min), to prevent photodamage and nuclear factor kappa-light-chain-enhancer of activated B cells (NF-κB)-mediated inflammation. The lower gelatin methacryloyl (GelMA) hydrogel layer sustains the release of psoralen-loaded melanin-mimetic mesoporous polydopamine nanoparticles (PMPN), which persistently inhibits the Janus kinase-signal transducer and activator of transcription (JAK-STAT) signaling pathway and reduces autophagy-induced apoptosis, while enhancing tyrosinase activity (0.47-fold increase) to promote melanogenesis. In monobenzone-induced vitiligo mice, the CF/HA-PMPN/GelMA-MNs combined with NB-UVB demonstrated superior outcomes with 80.55% repigmentation at day 14 (vs. 25.90% in NB-UVB alone). This "rapid defense-sustained regeneration" paradigm provides a clinically translatable strategy to enhance efficacy and safety in vitiligo phototherapy.
2026, 37(8): 111878
doi: 10.1016/j.cclet.2025.111878
Abstract:
Current immunotherapy for melanoma remains limited by low immunogenicity, immune-related toxicity, and an immunosuppressive tumor microenvironment (TME), necessitating more effective strategies to enhance treatment outcomes. Enhancing immunogenic cell death (ICD) induction with immune remodelling offers a promising approach to boost antitumor immunity. Here, we develop a transdermal microneedle (MN) system co-delivering garlic-derived nanovesicles (Ve) and immunomodulatory garlic polysaccharides (GP) to synergistically activate a self-reinforcing cell death pathway and reprogram the immunosuppressive TME. The dissolving MN platform enables efficient intratumoral delivery of Ve-fused thermosensitive liposomes (TSVL@PTX/ICG), loaded with paclitaxel (PTX) and the photosensitizer indocyanine green (ICG). Upon near-infrared (NIR) irradiation, ICG-mediated photothermal heating triggers rapid drug release, inducing pyroptosis via gasdermin E (GSDME) cleavage while amplifying photodynamic therapy (PDT)-driven mitochondrial damage. This dual cell death mechanism elicits robust ICD, releasing tumor antigens and damage-associated molecular patterns (DAMPs) to enhance dendritic cell activation and cytotoxic T-cell infiltration. Concurrently, GP reprograms tumor-associated macrophages (TAMs) from immunosuppressive M2 to pro-inflammatory M1 phenotypes, reshaping the TME into an immunostimulatory niche. This multi-modal approach, combining pyroptosis-driven ICD, PDT, and immune remodelling achieves potent antitumor immunity and melanoma suppression, highlighting the potential of plant-derived therapeutics in cancer immunotherapy.
Current immunotherapy for melanoma remains limited by low immunogenicity, immune-related toxicity, and an immunosuppressive tumor microenvironment (TME), necessitating more effective strategies to enhance treatment outcomes. Enhancing immunogenic cell death (ICD) induction with immune remodelling offers a promising approach to boost antitumor immunity. Here, we develop a transdermal microneedle (MN) system co-delivering garlic-derived nanovesicles (Ve) and immunomodulatory garlic polysaccharides (GP) to synergistically activate a self-reinforcing cell death pathway and reprogram the immunosuppressive TME. The dissolving MN platform enables efficient intratumoral delivery of Ve-fused thermosensitive liposomes (TSVL@PTX/ICG), loaded with paclitaxel (PTX) and the photosensitizer indocyanine green (ICG). Upon near-infrared (NIR) irradiation, ICG-mediated photothermal heating triggers rapid drug release, inducing pyroptosis via gasdermin E (GSDME) cleavage while amplifying photodynamic therapy (PDT)-driven mitochondrial damage. This dual cell death mechanism elicits robust ICD, releasing tumor antigens and damage-associated molecular patterns (DAMPs) to enhance dendritic cell activation and cytotoxic T-cell infiltration. Concurrently, GP reprograms tumor-associated macrophages (TAMs) from immunosuppressive M2 to pro-inflammatory M1 phenotypes, reshaping the TME into an immunostimulatory niche. This multi-modal approach, combining pyroptosis-driven ICD, PDT, and immune remodelling achieves potent antitumor immunity and melanoma suppression, highlighting the potential of plant-derived therapeutics in cancer immunotherapy.
2026, 37(8): 111883
doi: 10.1016/j.cclet.2025.111883
Abstract:
Lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation energy storage systems owing to their high theoretical capacity and energy density. However, conventional polyolefin-based separators suffer from randomly distributed pores with broad size distributions, which are ineffective in suppressing the polysulfide shuttle effect. Moreover, they lack functional groups for catalyzing polysulfides conversion and promoting uniform lithium-ion deposition. Herein, we synthesized a hybrid material (denoted as DAAQ-TFP/MXene) via in situ growth of redox-active covalent organic frameworks (DAAQ-TFP) on amine-functionalized MXene nanosheets. The resulting DAAQ-TFP/MXene hybrid features a porous architecture and dual binding/catalytic sites, enabling efficient polysulfides adsorption and catalytic conversion, enhanced lithium-ion transport, and uniform lithium deposition. Consequently, the DAAQ-TFP/MXene-coated PP separator exhibits a high lithium-ion transference number (0.53). The LiLi symmetric cell incorporating this separator operates stably for 3800 h at 5 mA/cm2 and 1 mAh/cm2. Furthermore, Li-S full cells using DAAQ-TFP/MXene@PP separator delivers a high specific capacity (1224 mAh/g at 0.1 C), excellent rate performance (631 mAh/g at 5 C), and long-term cycling stability (71.3% capacity retention after 300 cycles at 1 C). This study provides a promising strategy for designing MXene-COF hybrid materials as functional coatings to improve the performance of Li-S batteries.
Lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation energy storage systems owing to their high theoretical capacity and energy density. However, conventional polyolefin-based separators suffer from randomly distributed pores with broad size distributions, which are ineffective in suppressing the polysulfide shuttle effect. Moreover, they lack functional groups for catalyzing polysulfides conversion and promoting uniform lithium-ion deposition. Herein, we synthesized a hybrid material (denoted as DAAQ-TFP/MXene) via in situ growth of redox-active covalent organic frameworks (DAAQ-TFP) on amine-functionalized MXene nanosheets. The resulting DAAQ-TFP/MXene hybrid features a porous architecture and dual binding/catalytic sites, enabling efficient polysulfides adsorption and catalytic conversion, enhanced lithium-ion transport, and uniform lithium deposition. Consequently, the DAAQ-TFP/MXene-coated PP separator exhibits a high lithium-ion transference number (0.53). The LiLi symmetric cell incorporating this separator operates stably for 3800 h at 5 mA/cm2 and 1 mAh/cm2. Furthermore, Li-S full cells using DAAQ-TFP/MXene@PP separator delivers a high specific capacity (1224 mAh/g at 0.1 C), excellent rate performance (631 mAh/g at 5 C), and long-term cycling stability (71.3% capacity retention after 300 cycles at 1 C). This study provides a promising strategy for designing MXene-COF hybrid materials as functional coatings to improve the performance of Li-S batteries.
2026, 37(8): 111908
doi: 10.1016/j.cclet.2025.111908
Abstract:
The rational design of high-performance electrocatalysts for hydrogen evolution reaction (HER) through real-time tracking of dynamic active site evolution is both challenging and essential for the progress of sustainable energy technologies. Herein, NixCo1-xMoO4 solid solution nanotubes have been synthesized via electrospinning followed by calcination for electrocatalytic HER in a 1.0 mol/L KOH electrolyte. Optimized Ni0.25Co0.75MoO4 (denoted as NCMO-1) demonstrates high specific surface area, enhances charge transfer kinetics, and improves HER activity, achieving a low overpotential of 123 mV at 10 mA/cm2. Based on the inherent structural stability, the surface reconstruction relies on the reaction potential and the pH electrolyte via integrated approach, which involves hydroxide ion can etch the Mo species into the electrolyte accompanied by collapse and transformation from MO6 polyhedrons to amorphous cobalt-nickel hydroxides (M(OH)x (M = Co and Ni) with the electron transfer from Co to Ni sites via the oxygen-bridged cobalt-nickel bond (Co-O-Ni). Meanwhile, the dissolution of Mo enhances the hydroxylation at Co/Ni sites by revealing additional defect sites, while the formation of Co(OH)x and Ni(OH)x alters the local electronic environment. Due to the amorphous nature and structural complexity of the reconstructed sites, theoretical calculations indicate that the interaction between Co and Ni sites in NCMO-1 enhances charge transfer, strengthens adsorption, and accelerates the conversion of hydrogen and the key intermediate (*H···OH). This study provides fundamental insights into surface reconstruction behavior through the strategic integration of multi-scale in-situ characterization techniques and offers guidance for the rational design of advanced HER electrocatalysts.
The rational design of high-performance electrocatalysts for hydrogen evolution reaction (HER) through real-time tracking of dynamic active site evolution is both challenging and essential for the progress of sustainable energy technologies. Herein, NixCo1-xMoO4 solid solution nanotubes have been synthesized via electrospinning followed by calcination for electrocatalytic HER in a 1.0 mol/L KOH electrolyte. Optimized Ni0.25Co0.75MoO4 (denoted as NCMO-1) demonstrates high specific surface area, enhances charge transfer kinetics, and improves HER activity, achieving a low overpotential of 123 mV at 10 mA/cm2. Based on the inherent structural stability, the surface reconstruction relies on the reaction potential and the pH electrolyte via integrated approach, which involves hydroxide ion can etch the Mo species into the electrolyte accompanied by collapse and transformation from MO6 polyhedrons to amorphous cobalt-nickel hydroxides (M(OH)x (M = Co and Ni) with the electron transfer from Co to Ni sites via the oxygen-bridged cobalt-nickel bond (Co-O-Ni). Meanwhile, the dissolution of Mo enhances the hydroxylation at Co/Ni sites by revealing additional defect sites, while the formation of Co(OH)x and Ni(OH)x alters the local electronic environment. Due to the amorphous nature and structural complexity of the reconstructed sites, theoretical calculations indicate that the interaction between Co and Ni sites in NCMO-1 enhances charge transfer, strengthens adsorption, and accelerates the conversion of hydrogen and the key intermediate (*H···OH). This study provides fundamental insights into surface reconstruction behavior through the strategic integration of multi-scale in-situ characterization techniques and offers guidance for the rational design of advanced HER electrocatalysts.
2026, 37(8): 112001
doi: 10.1016/j.cclet.2025.112001
Abstract:
Aptamers as synthetic oligonucleotide, exhibit exceptional target specificity and are increasingly employed in the development of high-performance aptamer-based sensors (aptasensors). Dye-displacement-based aptasensors have emerged as a label-free strategy, wherein between the aptamer and its cognate target displaces a pre-associated dye, eliciting an optical response. Despite this, conventional aptasensors rely on a single output signal, which constrains both sensitivity and detection robustness. Herein, we present a dual-mode aptasensor (DMApt) platform with fluorescence and colorimetric signal outputs derived from a systematic screening of a cyanine dye library, with CyFluor-8 identified as an optimal reporter. Notably, the DMApt features an ultrafast response time (5 s), making it highly suited for rapid, on-site detection applications. This approach leverages the superior binding affinity of native aptamers, avoiding the need for modification and ensuring high sensitivity. Mechanistically, signal generation arises from the concerted contributions of disaggregation-induced emission (DIE) and the attenuation of twisted intramolecular charge-transfer (TICT) through its application to a range of small-molecule and ionic targets, as well as its compatibility with aptamers exhibiting diverse secondary structures. This work establishes a modular, label-free framework for high-sensitivity small-molecule sensing, offering rapid response and excellent practicality for on-site biochemical, environmental, and diagnostic monitoring.
Aptamers as synthetic oligonucleotide, exhibit exceptional target specificity and are increasingly employed in the development of high-performance aptamer-based sensors (aptasensors). Dye-displacement-based aptasensors have emerged as a label-free strategy, wherein between the aptamer and its cognate target displaces a pre-associated dye, eliciting an optical response. Despite this, conventional aptasensors rely on a single output signal, which constrains both sensitivity and detection robustness. Herein, we present a dual-mode aptasensor (DMApt) platform with fluorescence and colorimetric signal outputs derived from a systematic screening of a cyanine dye library, with CyFluor-8 identified as an optimal reporter. Notably, the DMApt features an ultrafast response time (5 s), making it highly suited for rapid, on-site detection applications. This approach leverages the superior binding affinity of native aptamers, avoiding the need for modification and ensuring high sensitivity. Mechanistically, signal generation arises from the concerted contributions of disaggregation-induced emission (DIE) and the attenuation of twisted intramolecular charge-transfer (TICT) through its application to a range of small-molecule and ionic targets, as well as its compatibility with aptamers exhibiting diverse secondary structures. This work establishes a modular, label-free framework for high-sensitivity small-molecule sensing, offering rapid response and excellent practicality for on-site biochemical, environmental, and diagnostic monitoring.
2026, 37(8): 112016
doi: 10.1016/j.cclet.2025.112016
Abstract:
Mimicking natural energy conversion processes, the pursuit of metal-free porous organic polymers (POPs) as heterogeneous catalysts for photocatalytic oxidation is a major driving force in materials science, seeking to achieve high-performance artificial photochemical systems. In this work, we report the bottom-up synthesis of a hydrazone-linked pillararene POP in its keto form. The inherent pillararene cavities provide a unique nanoconfinement environment, enabling effective substrate recognition and electron enrichment, thereby facilitating sensitive photo-response and efficient photoenergy-to-chemical energy conversion for photocatalytic oxidation coupling of primary amines (up to 99% conversion). Crucially, the framework’s tautomeric state is precisely modulated via an irreversible keto-to-enol conversion using sodium borohydride reduction. This controlled tautomerism permanently tunes the nanoconfinement microenvironment, amplifying the polymer’s electron-rich character and optimizing pore electrostatic properties. Leveraging this tunable nanoconfinement, the resulting enol form framework achieves highly efficient adsorption of cationic pollutants (up to 95% removal for Rhodamine B). This work establishes tautomerism as a chemical tool to engineer nanoconfinement in macrocycle-based POPs, expanding the toolbox for advanced porous materials with tailored functionalities for diverse applications like photocatalysis and adsorption.
Mimicking natural energy conversion processes, the pursuit of metal-free porous organic polymers (POPs) as heterogeneous catalysts for photocatalytic oxidation is a major driving force in materials science, seeking to achieve high-performance artificial photochemical systems. In this work, we report the bottom-up synthesis of a hydrazone-linked pillararene POP in its keto form. The inherent pillararene cavities provide a unique nanoconfinement environment, enabling effective substrate recognition and electron enrichment, thereby facilitating sensitive photo-response and efficient photoenergy-to-chemical energy conversion for photocatalytic oxidation coupling of primary amines (up to 99% conversion). Crucially, the framework’s tautomeric state is precisely modulated via an irreversible keto-to-enol conversion using sodium borohydride reduction. This controlled tautomerism permanently tunes the nanoconfinement microenvironment, amplifying the polymer’s electron-rich character and optimizing pore electrostatic properties. Leveraging this tunable nanoconfinement, the resulting enol form framework achieves highly efficient adsorption of cationic pollutants (up to 95% removal for Rhodamine B). This work establishes tautomerism as a chemical tool to engineer nanoconfinement in macrocycle-based POPs, expanding the toolbox for advanced porous materials with tailored functionalities for diverse applications like photocatalysis and adsorption.
2026, 37(8): 112017
doi: 10.1016/j.cclet.2025.112017
Abstract:
A significant challenge in organic synthesis has been the direct transformation of azaarenes into synthetically important aromatic aldehydes via formal nitrogen extrusion and carbon insertion. In this study, we present an efficient approach to reshape easily accessible azaarene-based onium salts, such as isoquinoliniums, pyridiniums, and pyrimidiniums, into functionalized multi-substituted aromatic aldehydes. This strategy relies on the strategic use of an inverse-electron-demand [4 + 2] cycloaddition-inspired cascade process with a wide tolerance of allenes, alkynes or alkenes as dienophiles. DFT calculations were conducted to gain insight into the reaction mechanism, revealing the significant catalytic roles of Na2CO3 and H2O for aldehyde formation and deamination. The operational simplicity enables widespread application of this strategy which has successfully been expanded towards the direct transformation of fused pyridinium and isoquinolinium salts as well as naturally occurring pharmaceuticals berberine sulfate and palmatine chloride into structurally novel atropisomeric N/P compounds. The resultant N/P compounds have demonstrated their potential application as ligands.
A significant challenge in organic synthesis has been the direct transformation of azaarenes into synthetically important aromatic aldehydes via formal nitrogen extrusion and carbon insertion. In this study, we present an efficient approach to reshape easily accessible azaarene-based onium salts, such as isoquinoliniums, pyridiniums, and pyrimidiniums, into functionalized multi-substituted aromatic aldehydes. This strategy relies on the strategic use of an inverse-electron-demand [4 + 2] cycloaddition-inspired cascade process with a wide tolerance of allenes, alkynes or alkenes as dienophiles. DFT calculations were conducted to gain insight into the reaction mechanism, revealing the significant catalytic roles of Na2CO3 and H2O for aldehyde formation and deamination. The operational simplicity enables widespread application of this strategy which has successfully been expanded towards the direct transformation of fused pyridinium and isoquinolinium salts as well as naturally occurring pharmaceuticals berberine sulfate and palmatine chloride into structurally novel atropisomeric N/P compounds. The resultant N/P compounds have demonstrated their potential application as ligands.
2026, 37(8): 112033
doi: 10.1016/j.cclet.2025.112033
Abstract:
Reductive amination between glycolaldehyde derivatives and lysine residues is a widely used strategy for constructing neoglycoproteins in biomedical applications. Here, α- and β-glycolaldehyde glycosides of five biologically relevant monosaccharides (Glc, Gal, Man, GlcNAc, GalNAc) were synthesized and conjugated to protein at a fixed sugar-to-protein ratio. Continuous kinetic monitoring revealed that anomeric configuration markedly influences both reaction rates and final sugar loading: α-Man > β-Man; β-Gal/GalNAc > their α-counterparts; Glc and GlcNAc showed no significant anomeric preferences. NMR analysis identified cyclic intermediates that reduce the effective concentration of reactive aldehyde, while DFT calculations provided complementary insight into anomer-specific electrophilic character. These findings offer a mechanistic rationale for selecting anomeric configuration in glycoconjugate design.
Reductive amination between glycolaldehyde derivatives and lysine residues is a widely used strategy for constructing neoglycoproteins in biomedical applications. Here, α- and β-glycolaldehyde glycosides of five biologically relevant monosaccharides (Glc, Gal, Man, GlcNAc, GalNAc) were synthesized and conjugated to protein at a fixed sugar-to-protein ratio. Continuous kinetic monitoring revealed that anomeric configuration markedly influences both reaction rates and final sugar loading: α-Man > β-Man; β-Gal/GalNAc > their α-counterparts; Glc and GlcNAc showed no significant anomeric preferences. NMR analysis identified cyclic intermediates that reduce the effective concentration of reactive aldehyde, while DFT calculations provided complementary insight into anomer-specific electrophilic character. These findings offer a mechanistic rationale for selecting anomeric configuration in glycoconjugate design.
2026, 37(8): 112034
doi: 10.1016/j.cclet.2025.112034
Abstract:
Precise control over the dimensionality and morphology of supramolecular assemblies remains a key challenge in hybrid material design. Here we report a directional assembly strategy that exploits synergistic portal-specific hydrogen bonding and ion–dipole interactions between cucurbit[5]uril (CB[5]) and an Anderson-type polyoxometalate (POM) functionalized with terminal protonated amines. This tailored interaction drives the formation of elongated two-dimensional hybrid sheets with spatial confinement and anisotropic growth. The resulting CB[5]-NH2POM hybrids exhibit high thermal stability and surface-accessible CB[5] units, enabling hierarchical integration with gold nanorods (AuNRs). These AuNRs@CB[5]-NH2POM hybrids demonstrate efficient photothermal conversion (37.8%) and enable near-quantitative catalytic conversion (>99%) in NIR-triggered sulfide oxidation. Comparative controls confirm the critical role of CB[5]-mediated portal interactions in both structural definition and functional performance. This study highlights a transferable supramolecular design principle for dimensional control and modular interface engineering, offering a promising platform for developing adaptive hybrid materials in photothermal catalysis and related applications.
Precise control over the dimensionality and morphology of supramolecular assemblies remains a key challenge in hybrid material design. Here we report a directional assembly strategy that exploits synergistic portal-specific hydrogen bonding and ion–dipole interactions between cucurbit[5]uril (CB[5]) and an Anderson-type polyoxometalate (POM) functionalized with terminal protonated amines. This tailored interaction drives the formation of elongated two-dimensional hybrid sheets with spatial confinement and anisotropic growth. The resulting CB[5]-NH2POM hybrids exhibit high thermal stability and surface-accessible CB[5] units, enabling hierarchical integration with gold nanorods (AuNRs). These AuNRs@CB[5]-NH2POM hybrids demonstrate efficient photothermal conversion (37.8%) and enable near-quantitative catalytic conversion (>99%) in NIR-triggered sulfide oxidation. Comparative controls confirm the critical role of CB[5]-mediated portal interactions in both structural definition and functional performance. This study highlights a transferable supramolecular design principle for dimensional control and modular interface engineering, offering a promising platform for developing adaptive hybrid materials in photothermal catalysis and related applications.
2026, 37(8): 112035
doi: 10.1016/j.cclet.2025.112035
Abstract:
Site-selective deuterated reduction of quinoline to deuterium-labelled 1,2,3,4-tetrahydroquinoline scaffold can offer a powerful strategy for drug development, mechanistic studies, and synthesis of isotopically labeled standards. Existing deuterated reduction methods predominantly produce fully deuterated piperidines, lacking control over regioselectivity and deuterium stoichiometry. Herein, we report a Ni-catalyzed sequential deuteration protocol that enables regio- and multiplicity-controlled synthesis of mono-, di-, and tri-deuterated tetrahydroquinolines with simple deuterating reagents. Nucleophilic and electrophilic deuterating sources were combined to achieve site-selective reductive deuteration at 2-, 3- and 4-positions of quinolines. The method features broad functional group compatibility and delivers D-labeled tetrahydroquinolines in high yields with excellent positional deuterium incorporation. The protocol was further extended to the double-deuteration of different classes of olefins, quinoxalines and acridines, thus providing a unified platform for efficient synthesis of selectively D-labeled N-containing heterocycles and alkenes derivatives.
Site-selective deuterated reduction of quinoline to deuterium-labelled 1,2,3,4-tetrahydroquinoline scaffold can offer a powerful strategy for drug development, mechanistic studies, and synthesis of isotopically labeled standards. Existing deuterated reduction methods predominantly produce fully deuterated piperidines, lacking control over regioselectivity and deuterium stoichiometry. Herein, we report a Ni-catalyzed sequential deuteration protocol that enables regio- and multiplicity-controlled synthesis of mono-, di-, and tri-deuterated tetrahydroquinolines with simple deuterating reagents. Nucleophilic and electrophilic deuterating sources were combined to achieve site-selective reductive deuteration at 2-, 3- and 4-positions of quinolines. The method features broad functional group compatibility and delivers D-labeled tetrahydroquinolines in high yields with excellent positional deuterium incorporation. The protocol was further extended to the double-deuteration of different classes of olefins, quinoxalines and acridines, thus providing a unified platform for efficient synthesis of selectively D-labeled N-containing heterocycles and alkenes derivatives.
Metal-free carbon quantum dots as photocatalyst for phosphonation of undirected heteroaryl compounds
2026, 37(8): 112050
doi: 10.1016/j.cclet.2025.112050
Abstract:
Nitrogen-doped carbon dots (N-CDs) were synthesized via a hydrothermal method, utilizing citric acid and urea as precursor materials. Through a systematic characterization and evaluation process, the N-CDs variant with the highest amino group density was identified as an outstanding metal-free photocatalyst. Under ambient conditions, this photocatalyst exhibited remarkable catalytic performance in promoting visible-light-driven cross-dehydrogenative coupling (CDC) reactions between heteroaryl substrates and a wide range of H-phosphine oxide derivatives. This methodology presents several noteworthy advantages, such as operational stability and recyclability of the photocatalyst system, compatibility with various functional groups, mild reaction parameters, scalability for practical applications, and eco-friendly implementation using a mixed solvent system composed of 2-methyl tetrahydrofuran (2-Me THF) and water as the solvent medium. The developed protocol demonstrates enhanced process sustainability through its combination of environmental benignity and technical practicality.
Nitrogen-doped carbon dots (N-CDs) were synthesized via a hydrothermal method, utilizing citric acid and urea as precursor materials. Through a systematic characterization and evaluation process, the N-CDs variant with the highest amino group density was identified as an outstanding metal-free photocatalyst. Under ambient conditions, this photocatalyst exhibited remarkable catalytic performance in promoting visible-light-driven cross-dehydrogenative coupling (CDC) reactions between heteroaryl substrates and a wide range of H-phosphine oxide derivatives. This methodology presents several noteworthy advantages, such as operational stability and recyclability of the photocatalyst system, compatibility with various functional groups, mild reaction parameters, scalability for practical applications, and eco-friendly implementation using a mixed solvent system composed of 2-methyl tetrahydrofuran (2-Me THF) and water as the solvent medium. The developed protocol demonstrates enhanced process sustainability through its combination of environmental benignity and technical practicality.
2026, 37(8): 112104
doi: 10.1016/j.cclet.2025.112104
Abstract:
The development of recyclable materials has been the key to designing sustainable materials. Dynamic supramolecular polymers, taking advantages of the reversibility of noncovalent and dynamic covalent bonds, offer many opportunities for constructing responsive and recyclable material. Here, we report dynamic supramolecular network polymers based on the cooperation between hydrogen bond and the pillar[5]arene-based host–guest interaction. The backbones of the polymer network are constructed by poly(disulfides) and the side chains are cross-linked by hydrogen bond and the pillar[5]arene-based host–guest interaction. The introduction of host-guest interaction renders the resulting network with enhanced mechanical performances. The dynamic performance of poly(disulfides) backbones and the noncovalent side chain endow the polymer materials with depolymerization ability into monomer in a closed-loop manner. We foresee this dynamic supramolecular polymer system will show widespread potential toward developing sustainable materials.
The development of recyclable materials has been the key to designing sustainable materials. Dynamic supramolecular polymers, taking advantages of the reversibility of noncovalent and dynamic covalent bonds, offer many opportunities for constructing responsive and recyclable material. Here, we report dynamic supramolecular network polymers based on the cooperation between hydrogen bond and the pillar[5]arene-based host–guest interaction. The backbones of the polymer network are constructed by poly(disulfides) and the side chains are cross-linked by hydrogen bond and the pillar[5]arene-based host–guest interaction. The introduction of host-guest interaction renders the resulting network with enhanced mechanical performances. The dynamic performance of poly(disulfides) backbones and the noncovalent side chain endow the polymer materials with depolymerization ability into monomer in a closed-loop manner. We foresee this dynamic supramolecular polymer system will show widespread potential toward developing sustainable materials.
2026, 37(8): 112105
doi: 10.1016/j.cclet.2025.112105
Abstract:
Lactic acid plays a crucial role in tumor growth, maintenance, and metastasis. Given its significant impact on tumorigenesis, modulating lactic acid levels within the tumor microenvironment (TME) presents new opportunities for cancer therapy. Herein we developed a supramolecularly engineered bacterial reactor using a strong host-guest interaction between cucurbit[7]uril (CB[7])-modified attenuated Salmonella typhimurium VNP20009 (VNP) and adamantane (ADA)-functionalized lactate oxidase (LOX)-loaded liposomes. The VNP-mediated tumor colonization of these reactors facilitated LOX-driven lactic acid depletion in the hypoxic TME, simultaneously producing hydrogen peroxide (H2O2). The presence of H2O2 triggered the expression of catalase in VNP, which, in turn, catalyzed the conversion of H2O2 to oxygen (O2). This cyclic cascade reactor thus provided a continuous and stable oxygen source, promoting sustained lactic acid consumption for metabolic treatment, ultimately leading to tumor growth suppression and an enhanced anticancer effect.
Lactic acid plays a crucial role in tumor growth, maintenance, and metastasis. Given its significant impact on tumorigenesis, modulating lactic acid levels within the tumor microenvironment (TME) presents new opportunities for cancer therapy. Herein we developed a supramolecularly engineered bacterial reactor using a strong host-guest interaction between cucurbit[7]uril (CB[7])-modified attenuated Salmonella typhimurium VNP20009 (VNP) and adamantane (ADA)-functionalized lactate oxidase (LOX)-loaded liposomes. The VNP-mediated tumor colonization of these reactors facilitated LOX-driven lactic acid depletion in the hypoxic TME, simultaneously producing hydrogen peroxide (H2O2). The presence of H2O2 triggered the expression of catalase in VNP, which, in turn, catalyzed the conversion of H2O2 to oxygen (O2). This cyclic cascade reactor thus provided a continuous and stable oxygen source, promoting sustained lactic acid consumption for metabolic treatment, ultimately leading to tumor growth suppression and an enhanced anticancer effect.
2026, 37(8): 112106
doi: 10.1016/j.cclet.2025.112106
Abstract:
The interfacial electronic interaction between the support and catalyst has been demonstrated to play a significant role in regulating the d-band structure of metal centers. Still, it requires dedicated control over the interaction in a reasonable manner. Herein, we developed a heterostructured support by covalently linking carbon nitride quantum dots (CNQDs) on TiO2, to anchor electroactive CoP clusters (TiO2–CNQD/CoP) for hydrogen evolution reaction (HER). The interfacial electronic interaction between the heterostructured support (TiO2–CNQD) and CoP can be controlled by varying the size of CNQDs, owing to the number of conjugated N-heterocycles in CNQDs induces tunable π-electron delocalization. As a result, a volcano-shaped correlation between the shift of the Co d-band center (Δd) and the HER performance was established, suggesting that TiO2–CNQD/CoP-C2 with a moderate size of CNQD is the optimal HER catalyst. This study highlights the critical role of interfacial interaction in supported catalysts, providing a predictive descriptor focusing on the support design of advanced HER catalysts.
The interfacial electronic interaction between the support and catalyst has been demonstrated to play a significant role in regulating the d-band structure of metal centers. Still, it requires dedicated control over the interaction in a reasonable manner. Herein, we developed a heterostructured support by covalently linking carbon nitride quantum dots (CNQDs) on TiO2, to anchor electroactive CoP clusters (TiO2–CNQD/CoP) for hydrogen evolution reaction (HER). The interfacial electronic interaction between the heterostructured support (TiO2–CNQD) and CoP can be controlled by varying the size of CNQDs, owing to the number of conjugated N-heterocycles in CNQDs induces tunable π-electron delocalization. As a result, a volcano-shaped correlation between the shift of the Co d-band center (Δd) and the HER performance was established, suggesting that TiO2–CNQD/CoP-C2 with a moderate size of CNQD is the optimal HER catalyst. This study highlights the critical role of interfacial interaction in supported catalysts, providing a predictive descriptor focusing on the support design of advanced HER catalysts.
2026, 37(8): 112107
doi: 10.1016/j.cclet.2025.112107
Abstract:
Bifunctional molecules incorporating both germyl and boryl groups represent a significant class of compounds that have attracted considerable attention in organic synthesis due to their unique reactivity and versatility in diverse chemical trans-formations. Here, we present a highly efficient, one-step synthesis of such molecules through the catalytic C–H borylation of parent organogermanes, utilizing germanium as a directing atom. The process employs an iridium catalyst in conjunction with a ligand and acetate base, facilitating the formation of a germylametallacycle intermediate within the catalytic cycle. This methodology demonstrates broad substrate scope, successfully accommodating three distinct classes of organogermanes: benzylhydrogermanes, biaryl-type hydrogermanes, and triarylhydrogermanes, encompassing both sp2 and sp3 C–H activation. The versatile reactivity of the products, derived from both boron and germanium chemistry, highlights their potential utility in various applications.
Bifunctional molecules incorporating both germyl and boryl groups represent a significant class of compounds that have attracted considerable attention in organic synthesis due to their unique reactivity and versatility in diverse chemical trans-formations. Here, we present a highly efficient, one-step synthesis of such molecules through the catalytic C–H borylation of parent organogermanes, utilizing germanium as a directing atom. The process employs an iridium catalyst in conjunction with a ligand and acetate base, facilitating the formation of a germylametallacycle intermediate within the catalytic cycle. This methodology demonstrates broad substrate scope, successfully accommodating three distinct classes of organogermanes: benzylhydrogermanes, biaryl-type hydrogermanes, and triarylhydrogermanes, encompassing both sp2 and sp3 C–H activation. The versatile reactivity of the products, derived from both boron and germanium chemistry, highlights their potential utility in various applications.
2026, 37(8): 112154
doi: 10.1016/j.cclet.2025.112154
Abstract:
Metal-catalyzed alkylarylation of two carbon−carbon (C-C) bonds across vicinal C(sp2) sites in olefins can provide access to diverse combinatorial chemical space. Pre-activated arenes are often used as aryl sources, but the direct utilization of Csp2−H bond instead of pre-activated arenes remains underdeveloped. Herein, ruthenium-catalyzed alkylarylation of alkenes via para-selective C-H functionalization of unprotected aniline has been reported. It bears good functional group tolerance and enables late functionalization of complex natural products. Evaluation of cone angle and minimum percent buried volume help to determine the optimal ligand. The mechanism studies reveal the dissociation of p-cymene during the catalytic cycle which triggers the redox processes for radical generation.
Metal-catalyzed alkylarylation of two carbon−carbon (C-C) bonds across vicinal C(sp2) sites in olefins can provide access to diverse combinatorial chemical space. Pre-activated arenes are often used as aryl sources, but the direct utilization of Csp2−H bond instead of pre-activated arenes remains underdeveloped. Herein, ruthenium-catalyzed alkylarylation of alkenes via para-selective C-H functionalization of unprotected aniline has been reported. It bears good functional group tolerance and enables late functionalization of complex natural products. Evaluation of cone angle and minimum percent buried volume help to determine the optimal ligand. The mechanism studies reveal the dissociation of p-cymene during the catalytic cycle which triggers the redox processes for radical generation.
2026, 37(8): 112156
doi: 10.1016/j.cclet.2025.112156
Abstract:
The radical-mediated 1,2-difunctionalization of alkenes or alkynes has emerged as an efficient strategy for augmenting molecular diversity and complexity. Nevertheless, developing remote 1,4-difunctionalization reactions through radical cascade additions involving two intermolecular unsaturated bonds confronts complex chemo-, regio-, and stereoselectivity challenges. Here, we report a photocatalytic strategy that enables the first radical 1,4-difunctionalization across simple alkenes and arylacetylenes, leveraging the distinct reactivity between alkyl phosphites and different carbon radicals, by employing 1 mol% fac-Ir(ppy)3 as the photocatalyst and quinuclidine as the base. Mechanistic studies reveal that the photoexcited Ir(Ⅲ)* synergistically governs two processes: (1) Single-electron transfer (SET) activation of Rf-X to generate fluoroalkyl radicals, and (2) triplet energy transfer (TEnT)-mediated stereo-control of the constructed alkenyl phosphonates to achieve high Z/E selectivity. This method enables the efficient synthesis of various δ-fluoroalkyl-substituted alkenyl phosphonates with high Z/E selectivity under mild conditions. Furthermore, some products exhibit a synergistic inhibitory effect on porcine epidemic diarrhea virus (PEDV), effectively blocking viral adsorption and replication while preventing PEDV-induced cell apoptosis in vitro.
The radical-mediated 1,2-difunctionalization of alkenes or alkynes has emerged as an efficient strategy for augmenting molecular diversity and complexity. Nevertheless, developing remote 1,4-difunctionalization reactions through radical cascade additions involving two intermolecular unsaturated bonds confronts complex chemo-, regio-, and stereoselectivity challenges. Here, we report a photocatalytic strategy that enables the first radical 1,4-difunctionalization across simple alkenes and arylacetylenes, leveraging the distinct reactivity between alkyl phosphites and different carbon radicals, by employing 1 mol% fac-Ir(ppy)3 as the photocatalyst and quinuclidine as the base. Mechanistic studies reveal that the photoexcited Ir(Ⅲ)* synergistically governs two processes: (1) Single-electron transfer (SET) activation of Rf-X to generate fluoroalkyl radicals, and (2) triplet energy transfer (TEnT)-mediated stereo-control of the constructed alkenyl phosphonates to achieve high Z/E selectivity. This method enables the efficient synthesis of various δ-fluoroalkyl-substituted alkenyl phosphonates with high Z/E selectivity under mild conditions. Furthermore, some products exhibit a synergistic inhibitory effect on porcine epidemic diarrhea virus (PEDV), effectively blocking viral adsorption and replication while preventing PEDV-induced cell apoptosis in vitro.
2026, 37(8): 112162
doi: 10.1016/j.cclet.2025.112162
Abstract:
Here an enantioselective total synthesis of bioactive 3-deoxy-epothilone B is reported. Key features of this synthesis include Nelson’s alkaloid-catalyzed asymmetric ketene-aldehyde [2 + 2] cycloaddition to expeditiously construct the froward cis/trans configuration of C6−C8 position in a stereospecific manner and the subsequent allylic transposition nucleophilic addition to forge the C2−C4 unit. Other key steps involve an iridium-catalyzed asymmetric hydrogenation (AH) to introduce the C15 stereogenic center and a rhodium-catalyzed linear selective hydroformylation to install the C1 unit with our catalytic systems. In addition, the highly electrophilic enantioenriched β-lactone is regarded as a potential synthon for modular syntheses of a series of C1−C4 modified epothilones. Further biological activity evaluation indicated significant cytotoxicity of 3-deoxy-epothilone B against a panel of human tumor cell lines.
Here an enantioselective total synthesis of bioactive 3-deoxy-epothilone B is reported. Key features of this synthesis include Nelson’s alkaloid-catalyzed asymmetric ketene-aldehyde [2 + 2] cycloaddition to expeditiously construct the froward cis/trans configuration of C6−C8 position in a stereospecific manner and the subsequent allylic transposition nucleophilic addition to forge the C2−C4 unit. Other key steps involve an iridium-catalyzed asymmetric hydrogenation (AH) to introduce the C15 stereogenic center and a rhodium-catalyzed linear selective hydroformylation to install the C1 unit with our catalytic systems. In addition, the highly electrophilic enantioenriched β-lactone is regarded as a potential synthon for modular syntheses of a series of C1−C4 modified epothilones. Further biological activity evaluation indicated significant cytotoxicity of 3-deoxy-epothilone B against a panel of human tumor cell lines.
2026, 37(8): 112188
doi: 10.1016/j.cclet.2025.112188
Abstract:
Transition-metal-catalyzed substitution of propargylic electrophiles with secondary phosphine oxides (SPOs) has emerged as a powerful strategy to phosphorus-containing frameworks. However, precise regiocontrol remains elusive due to competing pathways in allenyl-metal intermediates and SPO tautomerism. Herein, we report a dynamic coordination strategy that leverages the tunable binding modes of SPOs to achieve regiodivergent dienylation of propargylic esters, thereby accessing a diverse range of 1,3-dienyl phosphines. Through fine-tuning of ligands and the strategic use of Brønsted or Lewis acid-assisted catalytic systems, we demonstrate switchable C2- versus C3-selective dienylation, governed by dynamic control over the coordination modes and reactivities of SPOs. Mechanistic studies reveal that the dynamic inner- or outer-sphere coordination dictates the regiochemical outcome, which proceeds via relay catalysis or bimetallic cooperative catalysis pathways, thus offering a rationale for the observed regiodivergence. This method provides a robust and modular platform for synthesizing multisubstituted 1,3-dienyl phosphines with broad substrate scope and excellent regio- and stereoselectivity, underscoring the potential of coordination-controlled reactivity in complex bond-forming processes.
Transition-metal-catalyzed substitution of propargylic electrophiles with secondary phosphine oxides (SPOs) has emerged as a powerful strategy to phosphorus-containing frameworks. However, precise regiocontrol remains elusive due to competing pathways in allenyl-metal intermediates and SPO tautomerism. Herein, we report a dynamic coordination strategy that leverages the tunable binding modes of SPOs to achieve regiodivergent dienylation of propargylic esters, thereby accessing a diverse range of 1,3-dienyl phosphines. Through fine-tuning of ligands and the strategic use of Brønsted or Lewis acid-assisted catalytic systems, we demonstrate switchable C2- versus C3-selective dienylation, governed by dynamic control over the coordination modes and reactivities of SPOs. Mechanistic studies reveal that the dynamic inner- or outer-sphere coordination dictates the regiochemical outcome, which proceeds via relay catalysis or bimetallic cooperative catalysis pathways, thus offering a rationale for the observed regiodivergence. This method provides a robust and modular platform for synthesizing multisubstituted 1,3-dienyl phosphines with broad substrate scope and excellent regio- and stereoselectivity, underscoring the potential of coordination-controlled reactivity in complex bond-forming processes.
2026, 37(8): 112246
doi: 10.1016/j.cclet.2025.112246
Abstract:
Aging of Pt in diesel oxidation catalyst (DOC) leads to diminished catalytic activity, presenting a considerable challenge for catalyst regeneration and enhancement. This work investigates on the regeneration of Pt/Al2O3-SiO2 (Pt/AS) catalysts in DOC utilizing the synergistic effect of the indirect non-thermal plasma (INTP) and direct non-thermal plasma (DNTP) to optimize catalytic performance for efficient and stable conversion of gaseous pollutants. The distinctive properties of DNTP-INTP promote the removal of surface particulate matter (PM) and increase the availability of adsorbed oxygen (Oads) on the catalyst surface. Moreover, DNTP effectively reduces the particle size of sintered catalysts by applying a high-energy electric field. This process facilitates the conversion of PtOx to metallic Pt0. Additionally, agglomerated Pt structures can be reverted into regular hexahedral nanoparticles through the synergistic process. The regenerated catalyst demonstrates exceptional catalytic performance and stability, which can rival the performance of newly prepared catalysts. Notably, compared to the aged catalyst, the low-temperature performance improves significantly, with a reduction of 90 ℃ in the temperature at the onset of catalytic activity. These results highlight the considerable potential of plasma-assisted synergistic catalysts regeneration for revitalizing aged DOC within the context of advancing clean energy technologies.
Aging of Pt in diesel oxidation catalyst (DOC) leads to diminished catalytic activity, presenting a considerable challenge for catalyst regeneration and enhancement. This work investigates on the regeneration of Pt/Al2O3-SiO2 (Pt/AS) catalysts in DOC utilizing the synergistic effect of the indirect non-thermal plasma (INTP) and direct non-thermal plasma (DNTP) to optimize catalytic performance for efficient and stable conversion of gaseous pollutants. The distinctive properties of DNTP-INTP promote the removal of surface particulate matter (PM) and increase the availability of adsorbed oxygen (Oads) on the catalyst surface. Moreover, DNTP effectively reduces the particle size of sintered catalysts by applying a high-energy electric field. This process facilitates the conversion of PtOx to metallic Pt0. Additionally, agglomerated Pt structures can be reverted into regular hexahedral nanoparticles through the synergistic process. The regenerated catalyst demonstrates exceptional catalytic performance and stability, which can rival the performance of newly prepared catalysts. Notably, compared to the aged catalyst, the low-temperature performance improves significantly, with a reduction of 90 ℃ in the temperature at the onset of catalytic activity. These results highlight the considerable potential of plasma-assisted synergistic catalysts regeneration for revitalizing aged DOC within the context of advancing clean energy technologies.
2026, 37(8): 112283
doi: 10.1016/j.cclet.2025.112283
Abstract:
Solar-driven hydrogen peroxide (H2O2) production presents a sustainable alternative to energy-intensive industrial methods, yet its efficiency using covalent organic frameworks (COFs) suffer from energy loss caused by strong exciton interactions. Herein, we designed COFs with donor-π-acceptor (D-π-A) architectures, using 2,5-dimethoxy-1,4-benzenedicarboxaldehyde as the D unit and optimizing the N-containing π-bridge units. The resulting TAPT–OCH3 COF, incorporating 4,4′,4′'-(1,3,5-triazine-2,4,6-triyl)trianiline as the A unit, demonstrated the extended electron pathways and the reduced exciton recombination, markedly boosting photocatalytic performance. Experimental results revealed that TAPT–OCH3 achieved a solar-to-chemical efficiency of 0.23% and a quantum yield of 2.21% at 420 nm, outperforming most reported COFs and metal-free catalysts. In situ characterization and theoretical calculations revealed that the TAPT–OCH3 enhances charge separation to drive H2O2 production via a 2e- oxygen reduction pathway, while its tailored electronic structure simultaneously improves the 1e- water oxidation process. Crucially, TAPT–OCH3 maintained high efficacy across diverse water sources and continuous-flow reactors under natural sunlight, enabling scalable H2O2 synthesis for water purification. Life cycle assessment confirmed the application stability of this material, underscoring its potential for sustainable environmental remediation. This work establishes a design paradigm for optimizing exciton dynamics in COF, highlighting the critical role of structural design for artificial H2O2 photosynthesis.
Solar-driven hydrogen peroxide (H2O2) production presents a sustainable alternative to energy-intensive industrial methods, yet its efficiency using covalent organic frameworks (COFs) suffer from energy loss caused by strong exciton interactions. Herein, we designed COFs with donor-π-acceptor (D-π-A) architectures, using 2,5-dimethoxy-1,4-benzenedicarboxaldehyde as the D unit and optimizing the N-containing π-bridge units. The resulting TAPT–OCH3 COF, incorporating 4,4′,4′'-(1,3,5-triazine-2,4,6-triyl)trianiline as the A unit, demonstrated the extended electron pathways and the reduced exciton recombination, markedly boosting photocatalytic performance. Experimental results revealed that TAPT–OCH3 achieved a solar-to-chemical efficiency of 0.23% and a quantum yield of 2.21% at 420 nm, outperforming most reported COFs and metal-free catalysts. In situ characterization and theoretical calculations revealed that the TAPT–OCH3 enhances charge separation to drive H2O2 production via a 2e- oxygen reduction pathway, while its tailored electronic structure simultaneously improves the 1e- water oxidation process. Crucially, TAPT–OCH3 maintained high efficacy across diverse water sources and continuous-flow reactors under natural sunlight, enabling scalable H2O2 synthesis for water purification. Life cycle assessment confirmed the application stability of this material, underscoring its potential for sustainable environmental remediation. This work establishes a design paradigm for optimizing exciton dynamics in COF, highlighting the critical role of structural design for artificial H2O2 photosynthesis.
2026, 37(8): 112284
doi: 10.1016/j.cclet.2025.112284
Abstract:
Achieving biomimetic leaves with high reflectance and polarization spectral similarity to vegetation is highly desirable. However, the polarization, often masked by the complex compositions of coatings, has long been overlooked. Herein, the reflectance and polarization spectral properties are simultaneously realized via electrostatic adsorption between hypoxanthine (HX) and sodium copper chlorophyllin (SCC). The SCC-doped HX coating exhibits high reflectance spectral similarity to vegetation, with a correlation coefficient of 0.9440 and a spectral angle cosine of 0.9685. Additionally, the degree of linear polarization is reduced by 39.3%. This study provides a reference for obtaining high-performance pigments for biomimetic leaves.
Achieving biomimetic leaves with high reflectance and polarization spectral similarity to vegetation is highly desirable. However, the polarization, often masked by the complex compositions of coatings, has long been overlooked. Herein, the reflectance and polarization spectral properties are simultaneously realized via electrostatic adsorption between hypoxanthine (HX) and sodium copper chlorophyllin (SCC). The SCC-doped HX coating exhibits high reflectance spectral similarity to vegetation, with a correlation coefficient of 0.9440 and a spectral angle cosine of 0.9685. Additionally, the degree of linear polarization is reduced by 39.3%. This study provides a reference for obtaining high-performance pigments for biomimetic leaves.
2026, 37(8): 112285
doi: 10.1016/j.cclet.2025.112285
Abstract:
Overcoming the penetration barrier of nanomedicines remains a paramount challenge in antitumor therapy. Apoptotic bodies (ApoBDs), which are naturally generated from apoptotic cells, can mediate a potent neighboring effect by transferring drug to neighboring tumor cells via macropinocytosis. To amplify this process, we developed a tumor microenvironment-responsive nanoplatform (named as AD-NVs@CPP) to selectively enhance chemokine (C-X-C motif) receptor 4 (CXCR4) receptor-stimulated macropinocytosis. This platform was constructed by co-encapsulating doxorubicin (DOX) and the hypoxia-activated prodrug AQ4N into homologous tumor cell membrane-derived nanovesicles (AD-NVs), followed by biomineralization of a calcium phosphate (CaP) shell that incorporated a CXCR4-targeting peptide (RFFE-SHAPAKPVSLSYR). The resultant AD-NVs@CPP exhibited a core-shell structure with a hydrodynamic diameter of ~180 nm and achieved a high peptide encapsulation efficiency of 81.6% ± 8.2%. The CaP shell demonstrated excellent pH-responsive dissolution, releasing ~50% of the peptide within 24 h at pH 6.5 (vs. negligible release at pH 7.4), which consequently promoted cellular uptake and enhanced cytotoxicity under acidic conditions in vitro. Additionally, AD-NVs@CPP-induced ApoBDs served as efficient drug reservoirs, delivering drugs to adjacent cells with an IC50 value of 0.98 µg/mL (in terms of protein concentration). In vivo, AD-NVs@CPP significantly prolonged the blood circulation time (increasing the half-life of DOX compared to the free drug solution) and improved tumor accumulation. Crucially, it enabled programmed drug penetration: AQ4N was selectively delivered into deep hypoxic tumor regions, mediating comprehensive tumor growth inhibition while maintaining a favorable safety profile. This work provides a robust strategy for achieving deep tumor penetration through the synergistic enhancement of macropinocytosis and the ApoBD-mediated neighboring effect.
Overcoming the penetration barrier of nanomedicines remains a paramount challenge in antitumor therapy. Apoptotic bodies (ApoBDs), which are naturally generated from apoptotic cells, can mediate a potent neighboring effect by transferring drug to neighboring tumor cells via macropinocytosis. To amplify this process, we developed a tumor microenvironment-responsive nanoplatform (named as AD-NVs@CPP) to selectively enhance chemokine (C-X-C motif) receptor 4 (CXCR4) receptor-stimulated macropinocytosis. This platform was constructed by co-encapsulating doxorubicin (DOX) and the hypoxia-activated prodrug AQ4N into homologous tumor cell membrane-derived nanovesicles (AD-NVs), followed by biomineralization of a calcium phosphate (CaP) shell that incorporated a CXCR4-targeting peptide (RFFE-SHAPAKPVSLSYR). The resultant AD-NVs@CPP exhibited a core-shell structure with a hydrodynamic diameter of ~180 nm and achieved a high peptide encapsulation efficiency of 81.6% ± 8.2%. The CaP shell demonstrated excellent pH-responsive dissolution, releasing ~50% of the peptide within 24 h at pH 6.5 (vs. negligible release at pH 7.4), which consequently promoted cellular uptake and enhanced cytotoxicity under acidic conditions in vitro. Additionally, AD-NVs@CPP-induced ApoBDs served as efficient drug reservoirs, delivering drugs to adjacent cells with an IC50 value of 0.98 µg/mL (in terms of protein concentration). In vivo, AD-NVs@CPP significantly prolonged the blood circulation time (increasing the half-life of DOX compared to the free drug solution) and improved tumor accumulation. Crucially, it enabled programmed drug penetration: AQ4N was selectively delivered into deep hypoxic tumor regions, mediating comprehensive tumor growth inhibition while maintaining a favorable safety profile. This work provides a robust strategy for achieving deep tumor penetration through the synergistic enhancement of macropinocytosis and the ApoBD-mediated neighboring effect.
2026, 37(8): 112286
doi: 10.1016/j.cclet.2025.112286
Abstract:
In this study, a simple N2 plasma strategy was employed to modify the surface of Co3O4, significantly enhancing its efficiency in activating peroxymonosulfate (PMS) for the degradation of tetracycline hydrochloride (TC). Co3O4 treated with plasma for 30 min (Co3O4–30) achieved a TC degradation efficiency of 93.2% within 30 min (k = 0.078 min−1), which was significantly higher than that of the pristine Co3O4 (k = 0.023 min−1). Studies demonstrated that plasma treatment induced the generation of oxygen vacancies (Ov) on the surface of Co3O4, which serve as key active sites during the catalytic process and facilitate the adsorption of PMS to generate singlet oxygen (1O2). As the dominant reactive oxygen species, the steady-state concentration of 1O2 was positively correlated with the TC degradation rate. Additionally, dominated by the non-radical pathway, the PMS/Co3O4–30 system exhibited high selectivity toward electron-rich pollutants as well as strong anti-interference capability against anions and complex water matrices. This study demonstrates that plasma technology serves as a viable approach for defect engineering in catalysts, enabling the selective generation of 1O2 from PMS.
In this study, a simple N2 plasma strategy was employed to modify the surface of Co3O4, significantly enhancing its efficiency in activating peroxymonosulfate (PMS) for the degradation of tetracycline hydrochloride (TC). Co3O4 treated with plasma for 30 min (Co3O4–30) achieved a TC degradation efficiency of 93.2% within 30 min (k = 0.078 min−1), which was significantly higher than that of the pristine Co3O4 (k = 0.023 min−1). Studies demonstrated that plasma treatment induced the generation of oxygen vacancies (Ov) on the surface of Co3O4, which serve as key active sites during the catalytic process and facilitate the adsorption of PMS to generate singlet oxygen (1O2). As the dominant reactive oxygen species, the steady-state concentration of 1O2 was positively correlated with the TC degradation rate. Additionally, dominated by the non-radical pathway, the PMS/Co3O4–30 system exhibited high selectivity toward electron-rich pollutants as well as strong anti-interference capability against anions and complex water matrices. This study demonstrates that plasma technology serves as a viable approach for defect engineering in catalysts, enabling the selective generation of 1O2 from PMS.
2026, 37(8): 112298
doi: 10.1016/j.cclet.2025.112298
Abstract:
Selenium (Se) speciation analysis is typically performed using complex and costly hyphenated analytical systems. In this study, we developed a novel strategy for Se speciation using gas chromatography combined with a 3D-printed point discharge micro atomic emission detector (GC-PD-μAED), coupled with chemical vapor generation (CVG) and headspace-solid phase microextraction (HS-SPME), for the simultaneous determination of selenite (Se(Ⅳ)), dimethylselenide (DMSe) and dimethyldiselenide (DMDSe) in aqueous matrices. The method involves derivatization of Se(Ⅳ) to volatile diethylselenide (DEtSe) using NaBEt4, followed by HS-SPME preconcentration of all three Se species prior to GC separation and PD-μAED detection at the Se emission line of 196.03 nm. The optimized method achieved limits of detection (LODs) of 2.34, 0.28 and 0.13 μg/L (as Se) for DMSe, DMDSe and Se(Ⅳ), respectively, with precision (RSD) ranging from 4.6% to 4.9%. The accuracy and practicability of the developed method were demonstrated through speciation analysis of Se in seven water samples with excellent recoveries (90.4%−107.9%). Moreover, this novel approach offers simplified instrumentation, significantly lower costs, and minimal use of consumables while maintaining robust analytical performance comparable to conventional methods, making it particularly valuable for resource-limited settings.
Selenium (Se) speciation analysis is typically performed using complex and costly hyphenated analytical systems. In this study, we developed a novel strategy for Se speciation using gas chromatography combined with a 3D-printed point discharge micro atomic emission detector (GC-PD-μAED), coupled with chemical vapor generation (CVG) and headspace-solid phase microextraction (HS-SPME), for the simultaneous determination of selenite (Se(Ⅳ)), dimethylselenide (DMSe) and dimethyldiselenide (DMDSe) in aqueous matrices. The method involves derivatization of Se(Ⅳ) to volatile diethylselenide (DEtSe) using NaBEt4, followed by HS-SPME preconcentration of all three Se species prior to GC separation and PD-μAED detection at the Se emission line of 196.03 nm. The optimized method achieved limits of detection (LODs) of 2.34, 0.28 and 0.13 μg/L (as Se) for DMSe, DMDSe and Se(Ⅳ), respectively, with precision (RSD) ranging from 4.6% to 4.9%. The accuracy and practicability of the developed method were demonstrated through speciation analysis of Se in seven water samples with excellent recoveries (90.4%−107.9%). Moreover, this novel approach offers simplified instrumentation, significantly lower costs, and minimal use of consumables while maintaining robust analytical performance comparable to conventional methods, making it particularly valuable for resource-limited settings.
2026, 37(8): 112299
doi: 10.1016/j.cclet.2025.112299
Abstract:
Widespread arsenic contamination in aquatic environments poses a major threat to human health and ecosystems, underscoring the urgent need for effective and selective remediation strategies. However, conventional technologies often suffer from reduced efficiency due to strong competition from coexisting anions such as phosphate, limiting their real-world applicability. In this study, we present a pH-regulated strategy for selective arsenate removal using ferric oxide (α-Fe2O3), a low-cost, non-toxic, and naturally abundant material. By integrating batch adsorption experiments, in-situ ATR-FTIR spectroscopy, two-dimensional correlation spectroscopy, and density functional theory simulations, we demonstrate that acidic conditions significantly enhance arsenate selectivity by promoting protonation-induced surface complexation. Protonation strengthens hydrogen bonding and facilitates a transition from monodentate to bidentate coordination, improving arsenate binding. We further identify the Fe-Fe interatomic distance as a key structural parameter governing complexation geometry and selectivity: Shorter distances (< 3.27 Å) enable dual coordination, while longer distances (~5.10 Å) restrict it. These mechanistic insights highlight the pivotal role of surface structure and protonation in dictating competitive adsorption outcomes. Overall, these findings provide a mechanistic framework for understanding and optimizing arsenate selectivity in multi-anion systems. By leveraging naturally occurring ferric oxide and simple pH adjustment, this work offers a scalable and practical approach to arsenic remediation in phosphate-rich waters.
Widespread arsenic contamination in aquatic environments poses a major threat to human health and ecosystems, underscoring the urgent need for effective and selective remediation strategies. However, conventional technologies often suffer from reduced efficiency due to strong competition from coexisting anions such as phosphate, limiting their real-world applicability. In this study, we present a pH-regulated strategy for selective arsenate removal using ferric oxide (α-Fe2O3), a low-cost, non-toxic, and naturally abundant material. By integrating batch adsorption experiments, in-situ ATR-FTIR spectroscopy, two-dimensional correlation spectroscopy, and density functional theory simulations, we demonstrate that acidic conditions significantly enhance arsenate selectivity by promoting protonation-induced surface complexation. Protonation strengthens hydrogen bonding and facilitates a transition from monodentate to bidentate coordination, improving arsenate binding. We further identify the Fe-Fe interatomic distance as a key structural parameter governing complexation geometry and selectivity: Shorter distances (< 3.27 Å) enable dual coordination, while longer distances (~5.10 Å) restrict it. These mechanistic insights highlight the pivotal role of surface structure and protonation in dictating competitive adsorption outcomes. Overall, these findings provide a mechanistic framework for understanding and optimizing arsenate selectivity in multi-anion systems. By leveraging naturally occurring ferric oxide and simple pH adjustment, this work offers a scalable and practical approach to arsenic remediation in phosphate-rich waters.
2026, 37(8): 112310
doi: 10.1016/j.cclet.2025.112310
Abstract:
Metal-organic frameworks (MOFs) hold promise as electrochemiluminescence (ECL) emitters but are limited by high operating potentials and low efficiencies, leading to substantial electrochemical interference and reduced sensitivity. Here, we report a defect-rich Fe(Ⅲ)-based MOF (De-Fe(Ⅲ)-MOF) that exhibits highly efficient ECL triggered at an ultralow potential (-0.3 V vs. Ag/AgCl). Prepared using electron-deficient 3,4,9,10-perylenetetracarboxylic acid (PTCA) as ligands and H3PO4 as the acid modulator, De-Fe(Ⅲ)-MOF features abundant open-metal catalytic sites, which achieves an exceptional cathodic ECL efficiency of 553.06%, even using classical Ru(bpy)3Cl2/S2O82− system triggered at -1.2 V as a standard. This outstanding performance is attributed to three key factors: (1) The abundant Fe(Ⅲ) active sites that efficiently catalyze S2O82− to produce SO4•- radicals at ultralow potentials; (2) the electron-deficient PTCA ligand that enables simultaneous reduction at similarly low potentials; and (3) the unified porous frame that facilitates efficient electron transfer through an ultrashort pathway, enhancing ECL efficiency. These features collectively minimize electrochemical side reactions and significantly enhance the sensitivity of the sensing platform. To demonstrate its practical application, we constructed an ECL sensor for carboxylesterase activity, achieving a limit of detection of 6.6 × 10–7 U/L with minimal interference.
Metal-organic frameworks (MOFs) hold promise as electrochemiluminescence (ECL) emitters but are limited by high operating potentials and low efficiencies, leading to substantial electrochemical interference and reduced sensitivity. Here, we report a defect-rich Fe(Ⅲ)-based MOF (De-Fe(Ⅲ)-MOF) that exhibits highly efficient ECL triggered at an ultralow potential (-0.3 V vs. Ag/AgCl). Prepared using electron-deficient 3,4,9,10-perylenetetracarboxylic acid (PTCA) as ligands and H3PO4 as the acid modulator, De-Fe(Ⅲ)-MOF features abundant open-metal catalytic sites, which achieves an exceptional cathodic ECL efficiency of 553.06%, even using classical Ru(bpy)3Cl2/S2O82− system triggered at -1.2 V as a standard. This outstanding performance is attributed to three key factors: (1) The abundant Fe(Ⅲ) active sites that efficiently catalyze S2O82− to produce SO4•- radicals at ultralow potentials; (2) the electron-deficient PTCA ligand that enables simultaneous reduction at similarly low potentials; and (3) the unified porous frame that facilitates efficient electron transfer through an ultrashort pathway, enhancing ECL efficiency. These features collectively minimize electrochemical side reactions and significantly enhance the sensitivity of the sensing platform. To demonstrate its practical application, we constructed an ECL sensor for carboxylesterase activity, achieving a limit of detection of 6.6 × 10–7 U/L with minimal interference.
2026, 37(8): 112321
doi: 10.1016/j.cclet.2025.112321
Abstract:
High-salinity wastewater, especially reverse osmosis (RO) concentrate, is difficult to treat due to severe microbial inhibition and the presence of refractory organics. Herein, a salinity-tolerant bacterium (Chryseobacterium sp.) was isolated and applied in combination with ionizing irradiation to develop an efficient coupled process for RO concentrate treatment. The strain metabolically degraded phenol, p-cresol, indole, and benzoic acid, and transcriptomic analysis revealed that salt tolerance was associated with the synthesis of specific salt-tolerant proteins and enzymes (i.e., branched-chain amino acid). Although elevated chloride and sulfate concentrations reduced the phenol removal rate, complete degradation was achieved. The coupled process achieved up to 78.3% COD removal and completely inactivated Chryseobacterium sp. in the effluent, ensuring biosafety. This study provides a promising strategy integrating halotolerant biodegradation and advanced oxidation for efficient treatment of high-salinity wastewater.
High-salinity wastewater, especially reverse osmosis (RO) concentrate, is difficult to treat due to severe microbial inhibition and the presence of refractory organics. Herein, a salinity-tolerant bacterium (Chryseobacterium sp.) was isolated and applied in combination with ionizing irradiation to develop an efficient coupled process for RO concentrate treatment. The strain metabolically degraded phenol, p-cresol, indole, and benzoic acid, and transcriptomic analysis revealed that salt tolerance was associated with the synthesis of specific salt-tolerant proteins and enzymes (i.e., branched-chain amino acid). Although elevated chloride and sulfate concentrations reduced the phenol removal rate, complete degradation was achieved. The coupled process achieved up to 78.3% COD removal and completely inactivated Chryseobacterium sp. in the effluent, ensuring biosafety. This study provides a promising strategy integrating halotolerant biodegradation and advanced oxidation for efficient treatment of high-salinity wastewater.
2026, 37(8): 112322
doi: 10.1016/j.cclet.2025.112322
Abstract:
Linear mRNA-encoded bispecific T cell engagers (BiTEs) have shown promising efficacy in cancer treatment; however, their clinical translation remains constrained by poor stability and transient protein expression. To overcome these limitations, we engineered a circular RNA (cRNA) encoding PD-L1×CD3 BiTEs using permuted intron-exon splicing and CVB3-IRES elements, and encapsulated it into novel ionizable lipid nanoparticles (D1LNPs) synthesized via a streamlined one-step reaction. This platform, termed D1LNP@cRNABiTEs, achieved robust and sustained in vivo expression of the BiTEs, significantly outperforming conventional linear mRNA formulations. In murine models of colorectal cancer, monotherapy with D1LNP@cRNABiTEs potently inhibited tumor growth, enhanced CD8+ T-cell infiltration into the tumor microenvironment, and elevated levels of proinflammatory cytokines. Furthermore, ELISpot analysis confirmed the enhancement of systemic antigen-specific T cell responses. The D1LNPs delivery system also demonstrated excellent stability and favorable safety profile. In conclusion, our study provides compelling evidence for the D1LNPs@cRNA platform as a potent and scalable strategy for cancer immunotherapy, effectively addressing key challenges of RNA stability and delivery.
Linear mRNA-encoded bispecific T cell engagers (BiTEs) have shown promising efficacy in cancer treatment; however, their clinical translation remains constrained by poor stability and transient protein expression. To overcome these limitations, we engineered a circular RNA (cRNA) encoding PD-L1×CD3 BiTEs using permuted intron-exon splicing and CVB3-IRES elements, and encapsulated it into novel ionizable lipid nanoparticles (D1LNPs) synthesized via a streamlined one-step reaction. This platform, termed D1LNP@cRNABiTEs, achieved robust and sustained in vivo expression of the BiTEs, significantly outperforming conventional linear mRNA formulations. In murine models of colorectal cancer, monotherapy with D1LNP@cRNABiTEs potently inhibited tumor growth, enhanced CD8+ T-cell infiltration into the tumor microenvironment, and elevated levels of proinflammatory cytokines. Furthermore, ELISpot analysis confirmed the enhancement of systemic antigen-specific T cell responses. The D1LNPs delivery system also demonstrated excellent stability and favorable safety profile. In conclusion, our study provides compelling evidence for the D1LNPs@cRNA platform as a potent and scalable strategy for cancer immunotherapy, effectively addressing key challenges of RNA stability and delivery.
2026, 37(8): 112327
doi: 10.1016/j.cclet.2025.112327
Abstract:
Colorectal cancer (CRC) is a common malignant tumor of the digestive tract and has become a serious threat to human health worldwide. As an important part of systems biology, metabolomics is an effective tool to study the pathogenesis of diseases and search for potential biomarkers. Particularly, liquid chromatography-high resolution mass spectrometry (LC-HRMS)-based untargeted metabolomics plays crucial roles in the discovery of CRC biomarkers. However, previous studies still have some limitations, such as small sample cohorts, lack of standardized procedures and independent validation. In this study, LC-HRMS based non-targeted metabolomics analysis was performed to acquire metabolic profiling of 156 urine samples from healthy controls (HC, n = 43), colorectal adenoma patients (CRA, n = 51) and CRC patients (n = 62) to reveal metabolite disturbance, and then differential metabolites were verified in another sample set including 200 urine samples. Compared with CRA patients and HC, the levels of some lipids and lipid-like molecules, organic acids and derivatives, and organic oxygen compounds were increased, whereas the levels of most amino acids and derivatives, benzenoids, lipids and lipid-like molecules, nucleosides, nucleotides, and analogues, organic acids and derivatives, organoheterocyclic compounds as well as phenylpropanoids and polyketides were significantly decreased in CRC patients. Moreover, a potential biomarkers panel consisting of 4 metabolites was defined and validated for CRC diagnosis, and high area under the curve (0.963 for distinguishing CRC from non-CRC subjects) as well as good specificity and sensitivity were obtained. Although further extensive validation with larger sample sizes in different populations is needed before it can be recommended for clinical use, clinical diagnosis of CRC in the future may benefit from the biomarkers panel developed in this study.
Colorectal cancer (CRC) is a common malignant tumor of the digestive tract and has become a serious threat to human health worldwide. As an important part of systems biology, metabolomics is an effective tool to study the pathogenesis of diseases and search for potential biomarkers. Particularly, liquid chromatography-high resolution mass spectrometry (LC-HRMS)-based untargeted metabolomics plays crucial roles in the discovery of CRC biomarkers. However, previous studies still have some limitations, such as small sample cohorts, lack of standardized procedures and independent validation. In this study, LC-HRMS based non-targeted metabolomics analysis was performed to acquire metabolic profiling of 156 urine samples from healthy controls (HC, n = 43), colorectal adenoma patients (CRA, n = 51) and CRC patients (n = 62) to reveal metabolite disturbance, and then differential metabolites were verified in another sample set including 200 urine samples. Compared with CRA patients and HC, the levels of some lipids and lipid-like molecules, organic acids and derivatives, and organic oxygen compounds were increased, whereas the levels of most amino acids and derivatives, benzenoids, lipids and lipid-like molecules, nucleosides, nucleotides, and analogues, organic acids and derivatives, organoheterocyclic compounds as well as phenylpropanoids and polyketides were significantly decreased in CRC patients. Moreover, a potential biomarkers panel consisting of 4 metabolites was defined and validated for CRC diagnosis, and high area under the curve (0.963 for distinguishing CRC from non-CRC subjects) as well as good specificity and sensitivity were obtained. Although further extensive validation with larger sample sizes in different populations is needed before it can be recommended for clinical use, clinical diagnosis of CRC in the future may benefit from the biomarkers panel developed in this study.
2026, 37(8): 112335
doi: 10.1016/j.cclet.2025.112335
Abstract:
The matrix deposition method is one of the critical factors influencing the performance of matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI), as it determines matrix crystal sizes and coating uniformity, thereby impacting ionization efficiency and spatial resolution. Currently, automated sprayers are widely utilized for matrix deposition due to their convenience, speed, and robust reproducibility. However, existing automated spraying techniques typically produce micrometer-sized crystal particles, limiting high-resolution imaging quality and sensitivity. To overcome this, we introduce cluster airflow assisted matrix coating (CAAMC), which employs multiple cluster airflows to achieve a more uniform dispersion and atomization of the matrix droplets, resulting in nano-sized crystal particles—an advance beyond traditional deposition methods. This method represented the first successful automatic spray method for nano-matrix crystallization, surpassing regular-one channel pneumatic spraying and sublimation in producing smaller, more homogeneous crystals. Application to rat brain tissues and single cells demonstrates that CAAMC significantly enhances small molecule and lipid detection efficiency and imaging quality (lateral resolution of 5 μm), exceeding the performance of regular-one channel pneumatic spraying and sublimation. Overall, CAAMC significantly broadens the potential of automated matrix spraying techniques in high-resolution MALDI-MSI.
The matrix deposition method is one of the critical factors influencing the performance of matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI), as it determines matrix crystal sizes and coating uniformity, thereby impacting ionization efficiency and spatial resolution. Currently, automated sprayers are widely utilized for matrix deposition due to their convenience, speed, and robust reproducibility. However, existing automated spraying techniques typically produce micrometer-sized crystal particles, limiting high-resolution imaging quality and sensitivity. To overcome this, we introduce cluster airflow assisted matrix coating (CAAMC), which employs multiple cluster airflows to achieve a more uniform dispersion and atomization of the matrix droplets, resulting in nano-sized crystal particles—an advance beyond traditional deposition methods. This method represented the first successful automatic spray method for nano-matrix crystallization, surpassing regular-one channel pneumatic spraying and sublimation in producing smaller, more homogeneous crystals. Application to rat brain tissues and single cells demonstrates that CAAMC significantly enhances small molecule and lipid detection efficiency and imaging quality (lateral resolution of 5 μm), exceeding the performance of regular-one channel pneumatic spraying and sublimation. Overall, CAAMC significantly broadens the potential of automated matrix spraying techniques in high-resolution MALDI-MSI.
2026, 37(8): 112343
doi: 10.1016/j.cclet.2025.112343
Abstract:
Oxalic acid (OA) promotes the production of reactive oxygen species (ROS) and the degradation of pollutants, while it also enhances the reduction of trivalent iron (Fe(Ⅲ)) in homogeneous Fenton systems. However, due to the coexistence of Fe(Ⅱ) and OA-Fe(Ⅲ)/hydroperoxide complex, the generation pathways of ROS and degradation mechanisms of pollutants have not been clarified. In this work, bisphenol A (BPA) was selected and its degradation mechanisms in the OA/Fe(Ⅲ)/sodium percarbonate (SPC) system were investigated. Results showed that 99% of BPA degradation in OA/Fe(Ⅲ)/SPC system, which was higher than that of single Fe(Ⅲ) and SPC system (degradation ratio < 10%). OA promoted the formation of carbonate radicals (CO3•-) and hydroxyl radicals (•OH). There was no remarkable relationship between the degradation ratio of BPA and the change of Fe(Ⅱ) concentration, suggesting that the reduction properties of OA was not the direct cause of BPA degradation. By further analysis, the chelation of Fe(Ⅲ) and OA resulted in an enormous potential difference between Fe(Ⅱ) and Fe(Ⅲ)-OA complex, which was more favorable for accepting electrons from Fe(Ⅱ) intermediate, and forming more reactive ferrous complexes; moreover, iron oxalate (Fe2(C2O4)3) enhanced BPA degradation in the Fe(Ⅱ)/SPC system, which also evidenced the above findings. Under neutral conditions (pH 7.0), peroxy intermediate (OA-Fe(Ⅲ)-OOH) complex also contributed to CO3•-/•OH production and enhanced BPA degradation. These findings highlight the important role of OA in degradation of pollutants, which provides valuable insights for designing sustainable Fenton-based advanced oxidation processes.
Oxalic acid (OA) promotes the production of reactive oxygen species (ROS) and the degradation of pollutants, while it also enhances the reduction of trivalent iron (Fe(Ⅲ)) in homogeneous Fenton systems. However, due to the coexistence of Fe(Ⅱ) and OA-Fe(Ⅲ)/hydroperoxide complex, the generation pathways of ROS and degradation mechanisms of pollutants have not been clarified. In this work, bisphenol A (BPA) was selected and its degradation mechanisms in the OA/Fe(Ⅲ)/sodium percarbonate (SPC) system were investigated. Results showed that 99% of BPA degradation in OA/Fe(Ⅲ)/SPC system, which was higher than that of single Fe(Ⅲ) and SPC system (degradation ratio < 10%). OA promoted the formation of carbonate radicals (CO3•-) and hydroxyl radicals (•OH). There was no remarkable relationship between the degradation ratio of BPA and the change of Fe(Ⅱ) concentration, suggesting that the reduction properties of OA was not the direct cause of BPA degradation. By further analysis, the chelation of Fe(Ⅲ) and OA resulted in an enormous potential difference between Fe(Ⅱ) and Fe(Ⅲ)-OA complex, which was more favorable for accepting electrons from Fe(Ⅱ) intermediate, and forming more reactive ferrous complexes; moreover, iron oxalate (Fe2(C2O4)3) enhanced BPA degradation in the Fe(Ⅱ)/SPC system, which also evidenced the above findings. Under neutral conditions (pH 7.0), peroxy intermediate (OA-Fe(Ⅲ)-OOH) complex also contributed to CO3•-/•OH production and enhanced BPA degradation. These findings highlight the important role of OA in degradation of pollutants, which provides valuable insights for designing sustainable Fenton-based advanced oxidation processes.
2026, 37(8): 112353
doi: 10.1016/j.cclet.2025.112353
Abstract:
Heavy metals complexed with organic reagents in wastewater jeopardize environmental safety, resist conventional removal methods, but are also valuable metallic resources. Herein, a novel fissured-phosphorylated zero-valent iron (P-ZVIbm&ln) was synthesized via mechanochemical phosphorylation and liquid-nitrogen-quenching, and applied to benzohydroxamic acid-complexed Cu(Ⅱ) (Cu(Ⅱ)-BHA) degradation and synchronous copper recovery. During mechanochemical phosphorylation, a ferrous phosphate shell with abundant surface ferrous (≡Fe2+) was constructed on ZVI, which facilitated the activation of molecular oxygen into reactive oxygen species (ROS) for Cu(Ⅱ)-BHA degradation. Moreover, the subsequent liquid-nitrogen-quenching created surface cracks for more Fe0 cores exposure, which triggered the comproportionation reaction (Fe0 + 2Fe3+ → 3Fe2+), thereby strengthening Fe2+ regeneration and sustainable molecular oxygen activation for efficient oxidative decomplexation and metal recovery. In the P-ZVIbm&ln/Cu(Ⅱ)-BHA decontamination process, nearly 100% of Cu was recovered and BHA was degraded, while P-ZVIbm&ln showed excellent cyclic reaction performance. Through diverse experiments and density functional theory (DFT) calculations, researchers shed light on the mechanism. Meanwhile, the P-ZVIbm&ln could effectively treat other metal-BHA complexes (e.g., Cr(Ⅲ), Mn(Ⅱ), Ni(Ⅱ), Ag(Ⅰ), Cd(Ⅱ), and Pb(Ⅱ)) and actual mine wastewater containing Cu(Ⅱ) complexes with satisfactory metal recovery, showing promising application prospects in treatment of heavy-metal complex wastewater and sustainable development.
Heavy metals complexed with organic reagents in wastewater jeopardize environmental safety, resist conventional removal methods, but are also valuable metallic resources. Herein, a novel fissured-phosphorylated zero-valent iron (P-ZVIbm&ln) was synthesized via mechanochemical phosphorylation and liquid-nitrogen-quenching, and applied to benzohydroxamic acid-complexed Cu(Ⅱ) (Cu(Ⅱ)-BHA) degradation and synchronous copper recovery. During mechanochemical phosphorylation, a ferrous phosphate shell with abundant surface ferrous (≡Fe2+) was constructed on ZVI, which facilitated the activation of molecular oxygen into reactive oxygen species (ROS) for Cu(Ⅱ)-BHA degradation. Moreover, the subsequent liquid-nitrogen-quenching created surface cracks for more Fe0 cores exposure, which triggered the comproportionation reaction (Fe0 + 2Fe3+ → 3Fe2+), thereby strengthening Fe2+ regeneration and sustainable molecular oxygen activation for efficient oxidative decomplexation and metal recovery. In the P-ZVIbm&ln/Cu(Ⅱ)-BHA decontamination process, nearly 100% of Cu was recovered and BHA was degraded, while P-ZVIbm&ln showed excellent cyclic reaction performance. Through diverse experiments and density functional theory (DFT) calculations, researchers shed light on the mechanism. Meanwhile, the P-ZVIbm&ln could effectively treat other metal-BHA complexes (e.g., Cr(Ⅲ), Mn(Ⅱ), Ni(Ⅱ), Ag(Ⅰ), Cd(Ⅱ), and Pb(Ⅱ)) and actual mine wastewater containing Cu(Ⅱ) complexes with satisfactory metal recovery, showing promising application prospects in treatment of heavy-metal complex wastewater and sustainable development.
2026, 37(8): 112363
doi: 10.1016/j.cclet.2026.112363
Abstract:
The development of highly sensitive electrocatalysts for the electrochemical detection of ortho-nitrophenol (ONP) is critical for environmental monitoring due to its high toxicity in water environment. Herein, a novel electronic configuration engineering on CoSeO3/AlO(OH) heterostructure with precisely modulated d-band centers is successfully designed. Crucially, a negative shift in the d-band center enhances the catalysis and adsorption ability of the heterostructure. Benefiting from the electron transfer behavior from AlO(OH) to CoSeO3, the electrocatalyst exhibits exceptional ONP sensing performance, achieving an ultrahigh sensitivity of 0.499 μA L μmol-1 and a record-low detection limit of 5.353 nmol/L. Furthermore, the experimental characterizations and density functional theory (DFT) calculations reveal that the heterostructure-induced d-band center downshifting optimizes the adsorption strength of ONP, further accelerating the electrochemical redox kinetics. The CoSeO3/AlO(OH) also demonstrates good stability, anti-interference capabilities, and successful application in detecting ONP in real water samples. This study offers a promising strategy for designing advanced electrochemical sensors through heterointerface-based electronic structure engineering.
The development of highly sensitive electrocatalysts for the electrochemical detection of ortho-nitrophenol (ONP) is critical for environmental monitoring due to its high toxicity in water environment. Herein, a novel electronic configuration engineering on CoSeO3/AlO(OH) heterostructure with precisely modulated d-band centers is successfully designed. Crucially, a negative shift in the d-band center enhances the catalysis and adsorption ability of the heterostructure. Benefiting from the electron transfer behavior from AlO(OH) to CoSeO3, the electrocatalyst exhibits exceptional ONP sensing performance, achieving an ultrahigh sensitivity of 0.499 μA L μmol-1 and a record-low detection limit of 5.353 nmol/L. Furthermore, the experimental characterizations and density functional theory (DFT) calculations reveal that the heterostructure-induced d-band center downshifting optimizes the adsorption strength of ONP, further accelerating the electrochemical redox kinetics. The CoSeO3/AlO(OH) also demonstrates good stability, anti-interference capabilities, and successful application in detecting ONP in real water samples. This study offers a promising strategy for designing advanced electrochemical sensors through heterointerface-based electronic structure engineering.
2026, 37(8): 112416
doi: 10.1016/j.cclet.2026.112416
Abstract:
The iron-based pyrophosphate Na2FeP2O7 (NFPO) exhibits remarkable advantages including economic viability, exceptional structural stability, and outstanding safety characteristics. Nevertheless, the widespread implementation is fundamentally constrained by its poor inherent electronic conductivity and inadequate Na+ transport kinetics. This work employs a Cu doping strategy to achieve systematic electrochemical optimization through inducing local lattice distortions. The optimized Na2Fe0.97Cu0.03P2O7@C (0.03Cu-NFPO@C) composite delivers an impressive specific capacity of 91.32 mAh/g at 0.05 C and exhibits remarkable rate capability of 39.07 mAh/g at 50 C, whereas pristine NFPO@C merely provides 24.12 mAh/g. Furthermore, 0.03Cu-NFPO@C demonstrates extraordinary cycling stability, retaining 86.40% capacity after 12, 000 cycles at 40 C. Structural characterization through in-situ X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) confirms that Cu doping effectively stabilizes the crystal framework, modifies Fe coordination environments and shortens Fe-O bond lengths. Theory calculations demonstrate that Cu doping reduces the band gap and lowers Na+ diffusion barriers, thereby optimizing intrinsic electronic conductivity and ion transport kinetics. This study introduces an innovative methodology for designing polyanionic cathodes, accelerating the commercialization of sodium-ion batteries for grid-scale energy storage.
The iron-based pyrophosphate Na2FeP2O7 (NFPO) exhibits remarkable advantages including economic viability, exceptional structural stability, and outstanding safety characteristics. Nevertheless, the widespread implementation is fundamentally constrained by its poor inherent electronic conductivity and inadequate Na+ transport kinetics. This work employs a Cu doping strategy to achieve systematic electrochemical optimization through inducing local lattice distortions. The optimized Na2Fe0.97Cu0.03P2O7@C (0.03Cu-NFPO@C) composite delivers an impressive specific capacity of 91.32 mAh/g at 0.05 C and exhibits remarkable rate capability of 39.07 mAh/g at 50 C, whereas pristine NFPO@C merely provides 24.12 mAh/g. Furthermore, 0.03Cu-NFPO@C demonstrates extraordinary cycling stability, retaining 86.40% capacity after 12, 000 cycles at 40 C. Structural characterization through in-situ X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) confirms that Cu doping effectively stabilizes the crystal framework, modifies Fe coordination environments and shortens Fe-O bond lengths. Theory calculations demonstrate that Cu doping reduces the band gap and lowers Na+ diffusion barriers, thereby optimizing intrinsic electronic conductivity and ion transport kinetics. This study introduces an innovative methodology for designing polyanionic cathodes, accelerating the commercialization of sodium-ion batteries for grid-scale energy storage.
2026, 37(8): 112429
doi: 10.1016/j.cclet.2026.112429
Abstract:
We present the synthesis and host-guest complexation of endo-functionalized shape-persistent hexa(ethynylpyridine) macrocycles (Py6MCs). The challenging macrocyclization of linear hexapyridine precursors was achieved by using catalytic amount of PdCl2(PPh3)2 and stoichiometric CuI in the Sonogashira reaction, or with K2CO3 as an additive under copper-free conditions. Single-crystal X-ray diffraction revealed that Py6MCs with different side chains all feature a near-planar framework, with notable flexibility to adopt chair-like or boat-like conformations. The polar and electron-rich cavities of Py6MCs render them attractive hosts for cationic guests. 1H NMR and fluorescence titrations showed that Py6MC1 and Py6MC2 formed 1:1 complexes with N-methyl pyridinium and quaternary ammonium cations, and high affinity (up to 3.1 × 105 L/mol) was achieved for cations of distinct shapes and sizes. Density functional theory (DFT) calculations showed that Py6MC readily deforms to complement the structures of different guests, demonstrating a high level of adaptivity.
We present the synthesis and host-guest complexation of endo-functionalized shape-persistent hexa(ethynylpyridine) macrocycles (Py6MCs). The challenging macrocyclization of linear hexapyridine precursors was achieved by using catalytic amount of PdCl2(PPh3)2 and stoichiometric CuI in the Sonogashira reaction, or with K2CO3 as an additive under copper-free conditions. Single-crystal X-ray diffraction revealed that Py6MCs with different side chains all feature a near-planar framework, with notable flexibility to adopt chair-like or boat-like conformations. The polar and electron-rich cavities of Py6MCs render them attractive hosts for cationic guests. 1H NMR and fluorescence titrations showed that Py6MC1 and Py6MC2 formed 1:1 complexes with N-methyl pyridinium and quaternary ammonium cations, and high affinity (up to 3.1 × 105 L/mol) was achieved for cations of distinct shapes and sizes. Density functional theory (DFT) calculations showed that Py6MC readily deforms to complement the structures of different guests, demonstrating a high level of adaptivity.
2026, 37(8): 112448
doi: 10.1016/j.cclet.2026.112448
Abstract:
In this work, a series of novel non-nucleoside reverse transcriptase inhibitors featuring pyridine-difluoro/dimethylaniline fragment and 4-aminepiperidine moiety were synthesized based on structure-based design strategy. Among these, the dimethyl-substituted analogue 20m, characterized by a larger dihedral angle, emerged as the most potent inhibitor against wild-type (WT) human immunodeficiency virus-1 (HIV-1) as well as multiple resistant strains. Compound 20m exhibited remarkable antiviral activity with median effect concentration (EC50) values of 0.003 µmol/L (WT), 0.011 µmol/L (L100I), 0.001 µmol/L (K103N), 0.006 µmol/L (Y181C), 0.108 µmol/L (Y188L), 0.008 µmol/L (E138K), 0.196 µmol/L (F227L + V106A), and 0.032 µmol/L (Y181C + K103N), consistently outperforming efavirenz (EFV). Notably, 20m also demonstrated dramatically enhanced aqueous solubility, reaching >3954.5 µg/mL in phosphate buffer at pH 4.5 and >7380.6 µg/mL at pH 2.0, far exceeding that of etravirine (ETR). Collectively, these findings lay a robust foundation for the future optimization and development of next-generation non-nucleoside reverse transcriptase inhibitors (NNRTIs).
In this work, a series of novel non-nucleoside reverse transcriptase inhibitors featuring pyridine-difluoro/dimethylaniline fragment and 4-aminepiperidine moiety were synthesized based on structure-based design strategy. Among these, the dimethyl-substituted analogue 20m, characterized by a larger dihedral angle, emerged as the most potent inhibitor against wild-type (WT) human immunodeficiency virus-1 (HIV-1) as well as multiple resistant strains. Compound 20m exhibited remarkable antiviral activity with median effect concentration (EC50) values of 0.003 µmol/L (WT), 0.011 µmol/L (L100I), 0.001 µmol/L (K103N), 0.006 µmol/L (Y181C), 0.108 µmol/L (Y188L), 0.008 µmol/L (E138K), 0.196 µmol/L (F227L + V106A), and 0.032 µmol/L (Y181C + K103N), consistently outperforming efavirenz (EFV). Notably, 20m also demonstrated dramatically enhanced aqueous solubility, reaching >3954.5 µg/mL in phosphate buffer at pH 4.5 and >7380.6 µg/mL at pH 2.0, far exceeding that of etravirine (ETR). Collectively, these findings lay a robust foundation for the future optimization and development of next-generation non-nucleoside reverse transcriptase inhibitors (NNRTIs).
2026, 37(8): 112568
doi: 10.1016/j.cclet.2026.112568
Abstract:
White-light organic molecules (WLOMs) exhibit distinct advantages over multi-component systems, such as good reproducibility and high long-term stability. However, the complex synthesis method and the unsatisfactory CIE coordinates hinder their further application. To meet this challenge, a series of novel white-light-emitting single-molecule compounds (BTP-Phs) based on the benzothiazolopyridinone skeleton were rationally designed and synthesized by modulating the donor-acceptor (D-A) structure of the molecules. The study of the structure-spectra relationship indicated that the strong electron-donating ability of the aromatic substituents and the synergistic effect of the extended π-conjugated system enhanced the intramolecular charge transfer (ICT), which reduces the energy gap of the molecules and favors the long-wavelength emission of BTP-Phs. Notably, ideal white light emission (0.31, 0.34) was achieved through the aldehyde-gemdiol equilibrium in mixed solvents. The emission color could be finely tuned by solvent composition, excitation wavelength and concentration. In addition, a fluorescent ink was developed based on BTP-CHO-OPh as a functional material, which could realize information storage and encryption through QR codes or ASCII binary encoding. This study not only provides valuable design strategies for constructing WLOMs based on aldehyde-geminal diol equilibrium, but also highlights their potential in the field of secure information technology.
White-light organic molecules (WLOMs) exhibit distinct advantages over multi-component systems, such as good reproducibility and high long-term stability. However, the complex synthesis method and the unsatisfactory CIE coordinates hinder their further application. To meet this challenge, a series of novel white-light-emitting single-molecule compounds (BTP-Phs) based on the benzothiazolopyridinone skeleton were rationally designed and synthesized by modulating the donor-acceptor (D-A) structure of the molecules. The study of the structure-spectra relationship indicated that the strong electron-donating ability of the aromatic substituents and the synergistic effect of the extended π-conjugated system enhanced the intramolecular charge transfer (ICT), which reduces the energy gap of the molecules and favors the long-wavelength emission of BTP-Phs. Notably, ideal white light emission (0.31, 0.34) was achieved through the aldehyde-gemdiol equilibrium in mixed solvents. The emission color could be finely tuned by solvent composition, excitation wavelength and concentration. In addition, a fluorescent ink was developed based on BTP-CHO-OPh as a functional material, which could realize information storage and encryption through QR codes or ASCII binary encoding. This study not only provides valuable design strategies for constructing WLOMs based on aldehyde-geminal diol equilibrium, but also highlights their potential in the field of secure information technology.
2026, 37(8): 112623
doi: 10.1016/j.cclet.2026.112623
Abstract:
Equilateral triangular lattices (TLs) with antiferromagnetic interactions are ideal templates for inducing magnetic frustration, offering a platform to explore exotic quantum spin states that are crucial for advancing quantum science and technology. However, few examples meet these structural criteria, and even fewer realize these fascinating physical properties. We report four novel equilateral TL magnets realized through a crystal-symmetry-protected molecular-brick strategy. By deliberately selecting a high-symmetry nonmagnetic structural template and incorporating magnetic molecular building blocks, magnetic ions are geometrically constrained by three-fold rotational symmetry within the a-b plane, enforcing an ideal equilateral TL and turning on magnetism in a nonmagnetic structural template. Magnetic susceptibility and specific heat measurements reveal a long-range magnetic ordering in BaCoBe2(BO3)2F2 around 180 mK, while BaNiBe2(BO3)2F2 remains disordered at 140 mK. Furthermore, crystal orbital Hamilton population analysis shows that different molecular bricks exhibit distinct bonding characteristics, resulting in diverse magnetic properties. Our results demonstrate that the molecular-brick chemical strategy offers valuable insights into the investigation of geometrically frustrated magnets.
Equilateral triangular lattices (TLs) with antiferromagnetic interactions are ideal templates for inducing magnetic frustration, offering a platform to explore exotic quantum spin states that are crucial for advancing quantum science and technology. However, few examples meet these structural criteria, and even fewer realize these fascinating physical properties. We report four novel equilateral TL magnets realized through a crystal-symmetry-protected molecular-brick strategy. By deliberately selecting a high-symmetry nonmagnetic structural template and incorporating magnetic molecular building blocks, magnetic ions are geometrically constrained by three-fold rotational symmetry within the a-b plane, enforcing an ideal equilateral TL and turning on magnetism in a nonmagnetic structural template. Magnetic susceptibility and specific heat measurements reveal a long-range magnetic ordering in BaCoBe2(BO3)2F2 around 180 mK, while BaNiBe2(BO3)2F2 remains disordered at 140 mK. Furthermore, crystal orbital Hamilton population analysis shows that different molecular bricks exhibit distinct bonding characteristics, resulting in diverse magnetic properties. Our results demonstrate that the molecular-brick chemical strategy offers valuable insights into the investigation of geometrically frustrated magnets.
2026, 37(8): 112817
doi: 10.1016/j.cclet.2026.112817
Abstract:
Covalent organic frameworks (COFs) are burgeoning for visible-light photoredox catalysis owing to their modular building blocks and convertible covalent linkages. Herein, the polycondensation of 1,3,6,8-tetra(4-formylphenyl)pyrene (Py) and 4,4′-biphenyldiamine (BD) affords an imine-linked COF, PyBD-COF. Consequently, the conversion of imine into thiazole yields a thiazole-linked COF, PyBTZ-COF. Both pyrene COFs possess well-defined crystallinity and porosity. Compared to PyBD-COF, PyBTZ-COF exhibits superior chemical stability and better electronic structure, attributable to its stable and photoactive thiazole linkages. Both PyBD-COF and PyBTZ-COF drive highly selective sulfoxidation by blue-light photoredox catalysis. Notably, 3 mol% TEMPO (2,2,6,6-tetramethylpiperidine-N-oxyl) as electron transfer mediator enhances the conversions to approximately twofold for both PyBD-COF and PyBTZ-COF compared to TEMPO-free conditions. Due to its better electronic structure, PyBTZ-COF outperforms PyBD-COF for selective aerobic sulfoxidation, irrespective of addition of 3 mol% TEMPO. PyBTZ-COF photoredox catalysis with TEMPO exhibits excellent stability and broad applicability for selective sulfoxidation. The conversion of the linkage of COFs offers a way forward for enhancing performance in photoredox catalysis.
Covalent organic frameworks (COFs) are burgeoning for visible-light photoredox catalysis owing to their modular building blocks and convertible covalent linkages. Herein, the polycondensation of 1,3,6,8-tetra(4-formylphenyl)pyrene (Py) and 4,4′-biphenyldiamine (BD) affords an imine-linked COF, PyBD-COF. Consequently, the conversion of imine into thiazole yields a thiazole-linked COF, PyBTZ-COF. Both pyrene COFs possess well-defined crystallinity and porosity. Compared to PyBD-COF, PyBTZ-COF exhibits superior chemical stability and better electronic structure, attributable to its stable and photoactive thiazole linkages. Both PyBD-COF and PyBTZ-COF drive highly selective sulfoxidation by blue-light photoredox catalysis. Notably, 3 mol% TEMPO (2,2,6,6-tetramethylpiperidine-N-oxyl) as electron transfer mediator enhances the conversions to approximately twofold for both PyBD-COF and PyBTZ-COF compared to TEMPO-free conditions. Due to its better electronic structure, PyBTZ-COF outperforms PyBD-COF for selective aerobic sulfoxidation, irrespective of addition of 3 mol% TEMPO. PyBTZ-COF photoredox catalysis with TEMPO exhibits excellent stability and broad applicability for selective sulfoxidation. The conversion of the linkage of COFs offers a way forward for enhancing performance in photoredox catalysis.
2026, 37(8): 111211
doi: 10.1016/j.cclet.2025.111211
Abstract:
Bone abnormalities induced due to inflammation, trauma, or diabetes have emerged as a serious issue during treatment and post-treatment. Currently, the prevalent treatments for bone abnormalities are surgery and antibiotics. However, they are progressively struggling to meet clinical needs. Metal-organic frameworks (MOFs) are acquiring attention among many bone repair and bone regeneration materials due to their excellent role in this area of research. MOFs -based nanomaterials are characterized by long-term stability, large specific surface area, and can be easily modifiable. Furthermore, their porous structure and increased mechanical capabilities are similar to alternative tissues, making them useful for bone repair and regeneration. This review article outlines the application of MOFs in bone repair and bone regeneration therapy. First, the mechanics of bone repair and regeneration are discussed, followed by a summary of the most frequent synthetic methods of MOFs for treating bone defects. Secondly, the strategies of different types of MOFs in bone repair and bone regeneration therapies are reviewed. Eventually, the challenges and future of MOFs in bone repairs and bone regeneration therapies are described, introducing a novel approach to treating bone abnormalities.
Bone abnormalities induced due to inflammation, trauma, or diabetes have emerged as a serious issue during treatment and post-treatment. Currently, the prevalent treatments for bone abnormalities are surgery and antibiotics. However, they are progressively struggling to meet clinical needs. Metal-organic frameworks (MOFs) are acquiring attention among many bone repair and bone regeneration materials due to their excellent role in this area of research. MOFs -based nanomaterials are characterized by long-term stability, large specific surface area, and can be easily modifiable. Furthermore, their porous structure and increased mechanical capabilities are similar to alternative tissues, making them useful for bone repair and regeneration. This review article outlines the application of MOFs in bone repair and bone regeneration therapy. First, the mechanics of bone repair and regeneration are discussed, followed by a summary of the most frequent synthetic methods of MOFs for treating bone defects. Secondly, the strategies of different types of MOFs in bone repair and bone regeneration therapies are reviewed. Eventually, the challenges and future of MOFs in bone repairs and bone regeneration therapies are described, introducing a novel approach to treating bone abnormalities.
2026, 37(8): 111229
doi: 10.1016/j.cclet.2025.111229
Abstract:
The diverse structure and hierarchical bonding found within Zintl phases play a crucial role in decoupling the electrical and thermal transport properties, thus conferring them with the desired "phonon-glass, electron-crystal" characteristics necessary for high thermoelectric performance. In the last twenty years, a multitude of promising Zintl thermoelectrics have been explored and investigated, with significant systems such as the 1–2–2 phase, 3–1–3 phase, 5–2–6 phase, 9–4–9 phase, 10–1–9 phase, and 14–1–11 phase standing out. More recently, the emergence of 1–1–1 type Zintl phase compounds as potential thermoelectric candidates have sparked considerable interest. In particular, the low lattice thermal conductivity in these compounds offers great possibilities to achieve high thermoelectric figure of merit zT. This review provides a summary of the crystal structures and thermoelectric performance of typical 1–1–1 type Zintl compounds ABSb (A stands for alkali, alkali-earth, or divalent rare-earth metals, B stands for IA, IB or IIB metals). The focus is placed on elucidating the interesting mechanisms of low lattice thermal conductivity in real-space (r-space) and reciprocal-space (k-space), such as huge fluctuation in bonding strengths, larger atomic displacement parameters, rattling-like behavior of atomic vibration, intrinsic vacancy structure, soft optical phonons, phonon softening strategy, avoided crossing effect. This comprehensive review enhances the understanding of structure-property relationships and offers guidance for further improving the thermoelectric performance of 1–1–1 type Zintl compounds.
The diverse structure and hierarchical bonding found within Zintl phases play a crucial role in decoupling the electrical and thermal transport properties, thus conferring them with the desired "phonon-glass, electron-crystal" characteristics necessary for high thermoelectric performance. In the last twenty years, a multitude of promising Zintl thermoelectrics have been explored and investigated, with significant systems such as the 1–2–2 phase, 3–1–3 phase, 5–2–6 phase, 9–4–9 phase, 10–1–9 phase, and 14–1–11 phase standing out. More recently, the emergence of 1–1–1 type Zintl phase compounds as potential thermoelectric candidates have sparked considerable interest. In particular, the low lattice thermal conductivity in these compounds offers great possibilities to achieve high thermoelectric figure of merit zT. This review provides a summary of the crystal structures and thermoelectric performance of typical 1–1–1 type Zintl compounds ABSb (A stands for alkali, alkali-earth, or divalent rare-earth metals, B stands for IA, IB or IIB metals). The focus is placed on elucidating the interesting mechanisms of low lattice thermal conductivity in real-space (r-space) and reciprocal-space (k-space), such as huge fluctuation in bonding strengths, larger atomic displacement parameters, rattling-like behavior of atomic vibration, intrinsic vacancy structure, soft optical phonons, phonon softening strategy, avoided crossing effect. This comprehensive review enhances the understanding of structure-property relationships and offers guidance for further improving the thermoelectric performance of 1–1–1 type Zintl compounds.
2026, 37(8): 111309
doi: 10.1016/j.cclet.2025.111309
Abstract:
Sodium-based batteries (SBBs) are considered as promising next-generation energy storage devices owing to the low cost and natural abundance of raw materials. As the blood of SSBs, electrolytes are required to exhibit specific properties, including broad electrochemical stability windows, high thermal stability, prior ionic conductivity, and so on. Therefore, a diverse array of materials and compositions were developed to form novel electrolytes, thereby satisfying the practical requirements of SSBs. In this review, we comprehensively summarize the latest advances and the corresponding electrochemical properties of different electrolytes for SBBs. First, this review describes the desirable characteristics of electrolytes in detail. Subsequently, the latest progress in the design and regulation of electrolytes is systematically analyzed from four key aspects: organic liquid electrolytes, aqueous electrolytes, solid-state electrolytes, and quasi-solid-state electrolytes. Finally, this review delivers an exhaustive illustration on the challenges and research prospects concerning the further development of electrolytes in SBBs.
Sodium-based batteries (SBBs) are considered as promising next-generation energy storage devices owing to the low cost and natural abundance of raw materials. As the blood of SSBs, electrolytes are required to exhibit specific properties, including broad electrochemical stability windows, high thermal stability, prior ionic conductivity, and so on. Therefore, a diverse array of materials and compositions were developed to form novel electrolytes, thereby satisfying the practical requirements of SSBs. In this review, we comprehensively summarize the latest advances and the corresponding electrochemical properties of different electrolytes for SBBs. First, this review describes the desirable characteristics of electrolytes in detail. Subsequently, the latest progress in the design and regulation of electrolytes is systematically analyzed from four key aspects: organic liquid electrolytes, aqueous electrolytes, solid-state electrolytes, and quasi-solid-state electrolytes. Finally, this review delivers an exhaustive illustration on the challenges and research prospects concerning the further development of electrolytes in SBBs.
2026, 37(8): 111759
doi: 10.1016/j.cclet.2025.111759
Abstract:
As the most common primary intracranial brain tumor, glioma is confronted with critical therapeutic dilemmas characterized by dismal prognosis and restricted treatment modalities. The current standard treatment for glioma includes maximally safe resection combined with radiotherapy and temozolomide (TMZ) chemotherapy. However, the presence of the blood-brain barrier (BBB) significantly impedes drug penetration into the brain, further exacerbating the therapeutic challenges in glioma treatment. Consequently, developing effective strategies to deliver drugs across the BBB remains pivotal for glioma therapy. Hence, this comprehensive review examines innovative drug delivery strategies designed to overcome BBB through two principal approaches: in-situ drug depots and advanced systemic delivery systems. The first section analyzes the fundamental biological and anatomical barriers impeding effective glioma management. Then, we critically evaluate emerging in-situ delivery modalities, including biodegradable wafer implants, intratumoral injectable depots, and convection-enhanced delivery (CED) systems. The last section explores advanced systemic drug delivery systems (DDS) and summarizes cutting-edge strategies using functionalized nanoparticles (NPs), biomimetic delivery vectors, and stimulus-responsive DDS for efficient and safe systemic drug delivery. Challenges and future developments related to the application of drug-delivery strategies for glioma treatment are also discussed. In summary, this review not only maps the current landscape of drug delivery strategies but also illuminates transformative research trajectories that can pave the way for precision medicine in glioma treatment.
As the most common primary intracranial brain tumor, glioma is confronted with critical therapeutic dilemmas characterized by dismal prognosis and restricted treatment modalities. The current standard treatment for glioma includes maximally safe resection combined with radiotherapy and temozolomide (TMZ) chemotherapy. However, the presence of the blood-brain barrier (BBB) significantly impedes drug penetration into the brain, further exacerbating the therapeutic challenges in glioma treatment. Consequently, developing effective strategies to deliver drugs across the BBB remains pivotal for glioma therapy. Hence, this comprehensive review examines innovative drug delivery strategies designed to overcome BBB through two principal approaches: in-situ drug depots and advanced systemic delivery systems. The first section analyzes the fundamental biological and anatomical barriers impeding effective glioma management. Then, we critically evaluate emerging in-situ delivery modalities, including biodegradable wafer implants, intratumoral injectable depots, and convection-enhanced delivery (CED) systems. The last section explores advanced systemic drug delivery systems (DDS) and summarizes cutting-edge strategies using functionalized nanoparticles (NPs), biomimetic delivery vectors, and stimulus-responsive DDS for efficient and safe systemic drug delivery. Challenges and future developments related to the application of drug-delivery strategies for glioma treatment are also discussed. In summary, this review not only maps the current landscape of drug delivery strategies but also illuminates transformative research trajectories that can pave the way for precision medicine in glioma treatment.
2026, 37(8): 111797
doi: 10.1016/j.cclet.2025.111797
Abstract:
Breast cancer is the most prevalent cancer in women worldwide and a major contributor to cancer-related death. It has been established for decades that natural bioactive compounds are a crucial source for developing novel anticancer drugs. However, their poor targeting, limited solubility and bioavailability, and instability hinder the effectiveness of treatment. With advancements in nanotechnology, nanomedicine delivery systems have emerged as viable approaches to enhance drug bioavailability and therapeutic effectiveness, with natural polymer-based drug carriers gaining significant attention for breast cancer treatment. Chitosan's distinct physicochemical characteristics, biocompatibility, and low immunogenicity make it a popular choice for carrier materials in nanomedicine delivery systems. Their desired qualities include the extent of chemical modification, controlled drug release, surface flexibility, non-toxicity, enhanced stability, cellular uptake, anticancer drug solubility, modulation of release kinetics, and biodistribution. This review aims to illustrate current concerns regarding breast cancer treatment, highlighting the untapped potential of natural bioactive compounds while promoting the latest developments of using chitosan-based nanocarriers to deliver natural bioactive compounds. Finally, this review spotlights the limitations of existing research and the futuristic prospects in this emerging field.
Breast cancer is the most prevalent cancer in women worldwide and a major contributor to cancer-related death. It has been established for decades that natural bioactive compounds are a crucial source for developing novel anticancer drugs. However, their poor targeting, limited solubility and bioavailability, and instability hinder the effectiveness of treatment. With advancements in nanotechnology, nanomedicine delivery systems have emerged as viable approaches to enhance drug bioavailability and therapeutic effectiveness, with natural polymer-based drug carriers gaining significant attention for breast cancer treatment. Chitosan's distinct physicochemical characteristics, biocompatibility, and low immunogenicity make it a popular choice for carrier materials in nanomedicine delivery systems. Their desired qualities include the extent of chemical modification, controlled drug release, surface flexibility, non-toxicity, enhanced stability, cellular uptake, anticancer drug solubility, modulation of release kinetics, and biodistribution. This review aims to illustrate current concerns regarding breast cancer treatment, highlighting the untapped potential of natural bioactive compounds while promoting the latest developments of using chitosan-based nanocarriers to deliver natural bioactive compounds. Finally, this review spotlights the limitations of existing research and the futuristic prospects in this emerging field.
2026, 37(8): 111801
doi: 10.1016/j.cclet.2025.111801
Abstract:
Hydrogen evolution reaction (HER) is the critical process of hydrogen production through water electrolysis. However, the dependence on precious metal catalysts limits its large-scale application. Transition metal phosphides (TMPs) are promising alternatives due to their metal-like conductivity, adjustable electronic structure and low cost. Yet they still show some shortcomings such as insufficient intrinsic activity and poor surface stability. This review first systematically summarizes the HER reaction mechanism and its implications for TMPs catalyst design. Subsequently, it details the characteristics, limitations, and performance optimization strategies for monometallic TMPs. Furthermore, it discusses advances in polymetallic TMPs and composite structures for overcoming the activity limitations of monometallic TMPs. Finally, we propose key obstacles limiting TMPs in HER and their research directions and development prospects in the future.
Hydrogen evolution reaction (HER) is the critical process of hydrogen production through water electrolysis. However, the dependence on precious metal catalysts limits its large-scale application. Transition metal phosphides (TMPs) are promising alternatives due to their metal-like conductivity, adjustable electronic structure and low cost. Yet they still show some shortcomings such as insufficient intrinsic activity and poor surface stability. This review first systematically summarizes the HER reaction mechanism and its implications for TMPs catalyst design. Subsequently, it details the characteristics, limitations, and performance optimization strategies for monometallic TMPs. Furthermore, it discusses advances in polymetallic TMPs and composite structures for overcoming the activity limitations of monometallic TMPs. Finally, we propose key obstacles limiting TMPs in HER and their research directions and development prospects in the future.
2026, 37(8): 111817
doi: 10.1016/j.cclet.2025.111817
Abstract:
Metal-based nanomedicine, which involves nanoparticles (NPs) composed of metals such as gold, silver, iron, and platinum, has emerged as a promising approach in drug delivery, cancer therapy, imaging, and diagnostics. This review systematically examines a variety of metal-containing NPs (MNPs), including elemental metal NPs, metal oxides, metal-organic frameworks, nanozymes, and up-conversion NPs, highlighting their unique physicochemical properties and biomedical applications. The biological functions of MNPs, particularly in drug delivery, imaging, and therapeutic contexts, are critically discussed. Key engineering strategies aimed at optimizing targeted delivery, drug loading, responsive release, and biocompatibility are explored, with a focus on enhancing clinical outcomes. Recent advances underscore the potential of MNPs in innovative applications such as liquid biopsy, tumor imaging, chemotherapy, immunotherapy, physical therapy, and nanozyme-mediated treatments. Despite promising developments, clinical translation remains hindered by challenges such as toxicity, scalability, and regulatory hurdles. This review concludes with an outlook on future directions for MNPs, emphasizing their potential to revolutionize disease diagnosis and treatment through innovative biomaterial design and engineering.
Metal-based nanomedicine, which involves nanoparticles (NPs) composed of metals such as gold, silver, iron, and platinum, has emerged as a promising approach in drug delivery, cancer therapy, imaging, and diagnostics. This review systematically examines a variety of metal-containing NPs (MNPs), including elemental metal NPs, metal oxides, metal-organic frameworks, nanozymes, and up-conversion NPs, highlighting their unique physicochemical properties and biomedical applications. The biological functions of MNPs, particularly in drug delivery, imaging, and therapeutic contexts, are critically discussed. Key engineering strategies aimed at optimizing targeted delivery, drug loading, responsive release, and biocompatibility are explored, with a focus on enhancing clinical outcomes. Recent advances underscore the potential of MNPs in innovative applications such as liquid biopsy, tumor imaging, chemotherapy, immunotherapy, physical therapy, and nanozyme-mediated treatments. Despite promising developments, clinical translation remains hindered by challenges such as toxicity, scalability, and regulatory hurdles. This review concludes with an outlook on future directions for MNPs, emphasizing their potential to revolutionize disease diagnosis and treatment through innovative biomaterial design and engineering.
2026, 37(8): 111846
doi: 10.1016/j.cclet.2025.111846
Abstract:
Chronic cutaneous wounds such as diabetic foot and pressure ulcers are increasing worldwide and remain difficult to manage. Conventional approaches are hindered by prolonged healing and antibiotic resistance, highlighting the need for advanced biomaterial strategies. Thus, the production of advanced biomaterials for efficient wound healing has become of special urgency. Mesoporous silica (MS), with its specific features of exceptional biocompatibility, easily tunable pore architectures, and multifunctional surface functionalization, has emerged as a promising choice in such applications. The review systematically overviews the most recent advances in the wound healing application of MS, with its participation in drug delivery, controlled inflammation, modulation of immune response, tissue regeneration, and angiogenesis. Synthesis methods, surface functionalization techniques, and incorporation of advanced technology such as stimulus responsive systems and multifunctional composites are also extensively reviewed. Furthermore, this review critically examines the key barriers to the clinical translation of MS, including long-term biosafety, immune compatibility, and scalable manufacturing. Overcoming these challenges is crucial for harnessing its full potential in next-generation wound healing. By integrating MS with precision medicine and emerging biomedical technologies, this review highlights its transformative role in advancing personalized wound care and regenerative medicine.
Chronic cutaneous wounds such as diabetic foot and pressure ulcers are increasing worldwide and remain difficult to manage. Conventional approaches are hindered by prolonged healing and antibiotic resistance, highlighting the need for advanced biomaterial strategies. Thus, the production of advanced biomaterials for efficient wound healing has become of special urgency. Mesoporous silica (MS), with its specific features of exceptional biocompatibility, easily tunable pore architectures, and multifunctional surface functionalization, has emerged as a promising choice in such applications. The review systematically overviews the most recent advances in the wound healing application of MS, with its participation in drug delivery, controlled inflammation, modulation of immune response, tissue regeneration, and angiogenesis. Synthesis methods, surface functionalization techniques, and incorporation of advanced technology such as stimulus responsive systems and multifunctional composites are also extensively reviewed. Furthermore, this review critically examines the key barriers to the clinical translation of MS, including long-term biosafety, immune compatibility, and scalable manufacturing. Overcoming these challenges is crucial for harnessing its full potential in next-generation wound healing. By integrating MS with precision medicine and emerging biomedical technologies, this review highlights its transformative role in advancing personalized wound care and regenerative medicine.
2026, 37(8): 111887
doi: 10.1016/j.cclet.2025.111887
Abstract:
Respiratory diseases constitute a major global health burden, impacting both public health and socioeconomic conditions. Pulmonary mRNA delivery systems are now emerging as a promising therapeutic strategy to treat respiratory diseases, overcoming challenges of conventional mRNA formulations such as low pulmonary bioavailability and adverse side effects. Notably, lipid and polymer nanoparticles integrated into compatible inhaler devices represent the predominant pulmonary mRNA delivery systems. Despite the promising aspects, pulmonary mRNA delivery systems in respiratory diseases treatments face four key challenges, viz. complex airway tract structure, mucociliary clearance system, immune system, and the "last hurdle" intracellular delivery barrier. All these challenges are critical to the treatment effectiveness and safety. Recent progress made on inhalable mRNA delivery methods based on various vectors is highlighted for addressing the above challenges, boosting prospective development of mRNA-based therapies for the treatment of respiratory diseases. This review examines current challenges, strategies, and advances in inhalable mRNA formulations for respiratory diseases and explores prospects for pulmonary mRNA delivery systems, which hold great promise as a next-generation therapeutic platform.
Respiratory diseases constitute a major global health burden, impacting both public health and socioeconomic conditions. Pulmonary mRNA delivery systems are now emerging as a promising therapeutic strategy to treat respiratory diseases, overcoming challenges of conventional mRNA formulations such as low pulmonary bioavailability and adverse side effects. Notably, lipid and polymer nanoparticles integrated into compatible inhaler devices represent the predominant pulmonary mRNA delivery systems. Despite the promising aspects, pulmonary mRNA delivery systems in respiratory diseases treatments face four key challenges, viz. complex airway tract structure, mucociliary clearance system, immune system, and the "last hurdle" intracellular delivery barrier. All these challenges are critical to the treatment effectiveness and safety. Recent progress made on inhalable mRNA delivery methods based on various vectors is highlighted for addressing the above challenges, boosting prospective development of mRNA-based therapies for the treatment of respiratory diseases. This review examines current challenges, strategies, and advances in inhalable mRNA formulations for respiratory diseases and explores prospects for pulmonary mRNA delivery systems, which hold great promise as a next-generation therapeutic platform.
2026, 37(8): 111910
doi: 10.1016/j.cclet.2025.111910
Abstract:
Sub-nanometer high-entropy materials (HEMs) have opened new pathways in electrocatalysis and biomedicine, leveraging their tunable composition, ultrahigh specific surface area, abundant active sites, and multi-element synergy. In electrocatalysis, their highly disordered multi-element structures significantly enhance the intrinsic activity and stability for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and CO2 reduction reaction (CO2RR), while their unique "cocktail effect" enables precise electronic structure modulation. For biomedical applications, their ultrasmall size facilitates cellular uptake and tissue penetration. Simultaneously, their multi-element composition endows them with multifunctionality, including photothermal/photodynamic/catalytic/magnetic therapy, multimodal imaging, and drug delivery, while also optimizing biocompatibility and reducing toxicity. However, challenges remain in the precise synthesis and mechanistic understanding of sub-nanometer HEMs, hindering their development for next-generation high-performance electrocatalysts and intelligent theranostic platforms. In this review, we comprehensively explore the composition-structure design principles of HEMs, with a focus on the multifunctional properties achieved by small sizes, particularly in the sub-nano range, and their applications in electrocatalysis and biomedicine. Additionally, this paper prospectively discusses emerging strategies that may drive the future development of HEMs, with particular emphasis on the application potential of sub-nanometer HEMs.
Sub-nanometer high-entropy materials (HEMs) have opened new pathways in electrocatalysis and biomedicine, leveraging their tunable composition, ultrahigh specific surface area, abundant active sites, and multi-element synergy. In electrocatalysis, their highly disordered multi-element structures significantly enhance the intrinsic activity and stability for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and CO2 reduction reaction (CO2RR), while their unique "cocktail effect" enables precise electronic structure modulation. For biomedical applications, their ultrasmall size facilitates cellular uptake and tissue penetration. Simultaneously, their multi-element composition endows them with multifunctionality, including photothermal/photodynamic/catalytic/magnetic therapy, multimodal imaging, and drug delivery, while also optimizing biocompatibility and reducing toxicity. However, challenges remain in the precise synthesis and mechanistic understanding of sub-nanometer HEMs, hindering their development for next-generation high-performance electrocatalysts and intelligent theranostic platforms. In this review, we comprehensively explore the composition-structure design principles of HEMs, with a focus on the multifunctional properties achieved by small sizes, particularly in the sub-nano range, and their applications in electrocatalysis and biomedicine. Additionally, this paper prospectively discusses emerging strategies that may drive the future development of HEMs, with particular emphasis on the application potential of sub-nanometer HEMs.
2026, 37(8): 111951
doi: 10.1016/j.cclet.2025.111951
Abstract:
Due to the abundant potassium resources, potassium ion batteries (PIBs) are gradually becoming a promising choice for large-scale energy storage. Among the many anode materials that have been investigated, antimony anode has attracted much attention due to its high theoretical specific capacity, low reaction potential and high electrical conductivity. However, these antimony anodes undergo significant volume changes (≈407%) during the potassium alloying reaction, which negatively affect their cycle stability and rate performance. In this paper, the research progress of antimony anodes in recent years is reviewed. Modification strategies to improve the performance of antimony anodes, including architectural design, alloying with other metals, composite system construction and electrolyte optimization, are discussed in depth. In addition, the possible future development directions for antimony anodes in PIBs with a view to accelerating their practical application are proposed. It is hoped that this review will help researchers design high-performance antimony anode materials more efficiently.
Due to the abundant potassium resources, potassium ion batteries (PIBs) are gradually becoming a promising choice for large-scale energy storage. Among the many anode materials that have been investigated, antimony anode has attracted much attention due to its high theoretical specific capacity, low reaction potential and high electrical conductivity. However, these antimony anodes undergo significant volume changes (≈407%) during the potassium alloying reaction, which negatively affect their cycle stability and rate performance. In this paper, the research progress of antimony anodes in recent years is reviewed. Modification strategies to improve the performance of antimony anodes, including architectural design, alloying with other metals, composite system construction and electrolyte optimization, are discussed in depth. In addition, the possible future development directions for antimony anodes in PIBs with a view to accelerating their practical application are proposed. It is hoped that this review will help researchers design high-performance antimony anode materials more efficiently.
2026, 37(8): 111973
doi: 10.1016/j.cclet.2025.111973
Abstract:
Lithium batteries have an exceptional energy density, efficiency, and long service lives, but their anodes show poor interfacial stability. This review summarizes recent advances in the use of atomic layer deposition (ALD) for interfacial modification of lithium battery anodes. It focuses on challenges, including the poor rate performance of intercalation-type anodes, the volume expansion and low initial Coulombic efficiency (ICE) of alloy-type anodes, and dendrite growth and solid-electrolyte interphase (SEI) instability in lithium-metal anodes. Based on this, the multifunctional roles of ALD-derived nanoscale passivation layers in regulating interfacial reactions, suppressing parasitic processes, and enhancing structural integrity are discussed. By evaluating the ability of ALD to improve the cycling lifespan, rate capability, and capacity retention, its application potential for fabricating high-energy-density storage systems is analyzed. This work provides theoretical principles and engineering pathways for the rational design of advanced anode materials.
Lithium batteries have an exceptional energy density, efficiency, and long service lives, but their anodes show poor interfacial stability. This review summarizes recent advances in the use of atomic layer deposition (ALD) for interfacial modification of lithium battery anodes. It focuses on challenges, including the poor rate performance of intercalation-type anodes, the volume expansion and low initial Coulombic efficiency (ICE) of alloy-type anodes, and dendrite growth and solid-electrolyte interphase (SEI) instability in lithium-metal anodes. Based on this, the multifunctional roles of ALD-derived nanoscale passivation layers in regulating interfacial reactions, suppressing parasitic processes, and enhancing structural integrity are discussed. By evaluating the ability of ALD to improve the cycling lifespan, rate capability, and capacity retention, its application potential for fabricating high-energy-density storage systems is analyzed. This work provides theoretical principles and engineering pathways for the rational design of advanced anode materials.
2026, 37(8): 112325
doi: 10.1016/j.cclet.2025.112325
Abstract:
Ammonia (NH3) is a pivotal industrial chemical extensively utilized in agricultural production, energy storage systems, and chemical manufacturing processes. However, the conventional NH3 synthesis method, the Haber-Bosch process, is not only highly energy-intensive but also produces substantial greenhouse gas emissions. On the other hand, a sustainable alternative is offered by the ambient electrocatalytic nitrate (NO3−) reduction reaction (NO3RR) to NH3, which utilizes renewable electricity. This process not only converts NO3− pollutants into valuable NH3 but also addresses environmental concerns by effectively utilizing NO3− waste. In this review, we focus on the electrocatalytic synthesis of NH3 via NO3RR, systematically outlining the background of NO3RR, the fundamental reaction pathways, and the methods for detecting products and intermediates. We also highlight the advantages of copper (Cu)-based catalysts in this reaction. We explore various strategies to enhance Cu catalysis, including nanoparticle synthesis, facet engineering, alloying, oxidation state tuning, and single-atom dispersion. Additionally, we provide an overview of how electrolyte composition and characteristics affect NO3− reduction efficiency and clarify the processes that underlie these effects. We delve into NO3RR's challenges and the likelihood of NH3 synthesis in the future. The goal of this work is to shed light on how to achieve environmental sustainability and create more effective NH3 synthesis strategies.
Ammonia (NH3) is a pivotal industrial chemical extensively utilized in agricultural production, energy storage systems, and chemical manufacturing processes. However, the conventional NH3 synthesis method, the Haber-Bosch process, is not only highly energy-intensive but also produces substantial greenhouse gas emissions. On the other hand, a sustainable alternative is offered by the ambient electrocatalytic nitrate (NO3−) reduction reaction (NO3RR) to NH3, which utilizes renewable electricity. This process not only converts NO3− pollutants into valuable NH3 but also addresses environmental concerns by effectively utilizing NO3− waste. In this review, we focus on the electrocatalytic synthesis of NH3 via NO3RR, systematically outlining the background of NO3RR, the fundamental reaction pathways, and the methods for detecting products and intermediates. We also highlight the advantages of copper (Cu)-based catalysts in this reaction. We explore various strategies to enhance Cu catalysis, including nanoparticle synthesis, facet engineering, alloying, oxidation state tuning, and single-atom dispersion. Additionally, we provide an overview of how electrolyte composition and characteristics affect NO3− reduction efficiency and clarify the processes that underlie these effects. We delve into NO3RR's challenges and the likelihood of NH3 synthesis in the future. The goal of this work is to shed light on how to achieve environmental sustainability and create more effective NH3 synthesis strategies.
2026, 37(8): 112326
doi: 10.1016/j.cclet.2025.112326
Abstract:
Metal-organic frameworks (MOFs) nanomachines (MNMs) merge high surface area, porosity, and the tunability of MOFs with mobility and intelligence of smart nanomachines. This review provides comprehensive overview of synthesis and post synthetic modifications for MOF tailored for water purification. Further MOF transformation into nanorobots has been elucidated, relating MNM shapes to their functionality. Propulsion modes: Both chemical and physical are also critically evaluated, and research gaps have been explored. For the environmental applications of MNMs, mechanisms of working, ability to remove metal ions, organic pollutants and dyes, sensing and disinfection have been explored. Future potential for the use of MNMs under harsh water conditions has also been discussed. Finally, the review identifies toxicological concerns related to long-term MNMs, research gaps and future challenges, giving a road map for future research, suggesting use of computational chemistry (artificial intelligence (AI) and machine learning (ML)) for effective purposes. By bringing synthesis, PSM, transformation, structural engineering at one place and relating them with propulsion mechanisms as well as with environmental applications of MNMs, this review will act as foundational reference for researchers working to fabricate MNMs for sustainable water treatment.
Metal-organic frameworks (MOFs) nanomachines (MNMs) merge high surface area, porosity, and the tunability of MOFs with mobility and intelligence of smart nanomachines. This review provides comprehensive overview of synthesis and post synthetic modifications for MOF tailored for water purification. Further MOF transformation into nanorobots has been elucidated, relating MNM shapes to their functionality. Propulsion modes: Both chemical and physical are also critically evaluated, and research gaps have been explored. For the environmental applications of MNMs, mechanisms of working, ability to remove metal ions, organic pollutants and dyes, sensing and disinfection have been explored. Future potential for the use of MNMs under harsh water conditions has also been discussed. Finally, the review identifies toxicological concerns related to long-term MNMs, research gaps and future challenges, giving a road map for future research, suggesting use of computational chemistry (artificial intelligence (AI) and machine learning (ML)) for effective purposes. By bringing synthesis, PSM, transformation, structural engineering at one place and relating them with propulsion mechanisms as well as with environmental applications of MNMs, this review will act as foundational reference for researchers working to fabricate MNMs for sustainable water treatment.
2026, 37(8): 112337
doi: 10.1016/j.cclet.2025.112337
Abstract:
Membrane separation technology offers significant advantages in water treatment but faces challenges such as membrane fouling and limited separation capabilities, which often fail to meet the urgent demands of water purification. Integrating versatile piezoelectric materials into conventional membranes is expected to overcome the limitations of existing techniques. This review analyzes recent advancements in piezoelectric membranes for efficient water purification, beginning with the historical evolution and foundational principles of the piezoelectric effect and piezocatalysis. It then presents an overview of conventional and emerging piezoelectric materials used in advanced membrane fabrication. The typical strategies for producing high-performance piezoelectric membranes are outlined, including solution blending, electrospinning, dry pressing, and sintering. The energy sources, applications, and mechanisms of piezoelectric membranes in water purification are examined, covering catalytic degradation, fouling mitigation, and antibacterial effects. Finally, this review assesses the main challenges facing piezoelectric membrane separation technology and considers future development pathways.
Membrane separation technology offers significant advantages in water treatment but faces challenges such as membrane fouling and limited separation capabilities, which often fail to meet the urgent demands of water purification. Integrating versatile piezoelectric materials into conventional membranes is expected to overcome the limitations of existing techniques. This review analyzes recent advancements in piezoelectric membranes for efficient water purification, beginning with the historical evolution and foundational principles of the piezoelectric effect and piezocatalysis. It then presents an overview of conventional and emerging piezoelectric materials used in advanced membrane fabrication. The typical strategies for producing high-performance piezoelectric membranes are outlined, including solution blending, electrospinning, dry pressing, and sintering. The energy sources, applications, and mechanisms of piezoelectric membranes in water purification are examined, covering catalytic degradation, fouling mitigation, and antibacterial effects. Finally, this review assesses the main challenges facing piezoelectric membrane separation technology and considers future development pathways.
2026, 37(8): 112352
doi: 10.1016/j.cclet.2025.112352
Abstract:
Sulfur is a key element in global biogeochemical cycles, participating in the energy exchange among the terrestrial, marine, and atmospheric systems. In the early days, the natural sulfur cycle maintained an input-output balance. However, the rapid expansion of industrial activities has disrupted this equilibrium by altering sulfur species conversion pathways and flux distributions. This has led us to have to explore new sulfur balance states to reduce the impact on the ecological environment. So far, researchers have conducted a series of studies on the modern sulfur cycle, but these findings have not yet been systematically organized. This review systematically examines the sulfur cycle from integrated natural and anthropogenic perspectives. Among them, the natural sulfur cycle encompasses the terrestrial, marine and atmospheric systems of the Earth, focusing on sulfur species, transformation and circulation flux. Furthermore, the investigation of the industrial metabolic process of sulfur has revealed that human activities have disrupted the balance of the Earth’s sulfur cycle, leading to resource depletion and environmental degradation. To mitigate these effects, advancing intra-industrial sulfur recycling strategies is critical for reducing primary resource consumption and waste emissions. This review provided a foundational framework for achieving sustainable sulfur utilization and restoring global sulfur balance.
Sulfur is a key element in global biogeochemical cycles, participating in the energy exchange among the terrestrial, marine, and atmospheric systems. In the early days, the natural sulfur cycle maintained an input-output balance. However, the rapid expansion of industrial activities has disrupted this equilibrium by altering sulfur species conversion pathways and flux distributions. This has led us to have to explore new sulfur balance states to reduce the impact on the ecological environment. So far, researchers have conducted a series of studies on the modern sulfur cycle, but these findings have not yet been systematically organized. This review systematically examines the sulfur cycle from integrated natural and anthropogenic perspectives. Among them, the natural sulfur cycle encompasses the terrestrial, marine and atmospheric systems of the Earth, focusing on sulfur species, transformation and circulation flux. Furthermore, the investigation of the industrial metabolic process of sulfur has revealed that human activities have disrupted the balance of the Earth’s sulfur cycle, leading to resource depletion and environmental degradation. To mitigate these effects, advancing intra-industrial sulfur recycling strategies is critical for reducing primary resource consumption and waste emissions. This review provided a foundational framework for achieving sustainable sulfur utilization and restoring global sulfur balance.
2026, 37(8): 112357
doi: 10.1016/j.cclet.2025.112357
Abstract:
The properties of biomass-derived multifunctional materials have garnered increasing attention in the fields of environmental remediation, energy storage, and heterogeneous catalysis due to their abundant content of N and C, which can effectively modulate electronic structure and facilitate the anchoring of active centers. In this review, we summarized the progress of our team over the past decade on a variety of multifunctional materials with diverse morphologies, electronic structures, and geometric sites, developed through novel synthetic strategies that employ biomass and its derivatives as carbon sources. Those multifunctional materials exhibited excellent catalytic performance for the adsorption and degradation of pollutants in wastewater, absorption of electromagnetic waves (EMW), and photocatalytic reactions. Moreover, the underlying mechanisms of adsorption, degradation, and activation during the reaction process as well as the relationship between activity and structure are also discussed. This review offers comprehensive insights for fabricating biomass-derived materials, with a specific emphasis on their physicochemical properties characterized by controlled morphology, tunable electronic properties, and precise localization of active species, as well as the aspect of the intricate relationship between activity-structure and catalytic mechanisms, providing reference for future advancements in various catalysis fields involving biomass-derived materials.
The properties of biomass-derived multifunctional materials have garnered increasing attention in the fields of environmental remediation, energy storage, and heterogeneous catalysis due to their abundant content of N and C, which can effectively modulate electronic structure and facilitate the anchoring of active centers. In this review, we summarized the progress of our team over the past decade on a variety of multifunctional materials with diverse morphologies, electronic structures, and geometric sites, developed through novel synthetic strategies that employ biomass and its derivatives as carbon sources. Those multifunctional materials exhibited excellent catalytic performance for the adsorption and degradation of pollutants in wastewater, absorption of electromagnetic waves (EMW), and photocatalytic reactions. Moreover, the underlying mechanisms of adsorption, degradation, and activation during the reaction process as well as the relationship between activity and structure are also discussed. This review offers comprehensive insights for fabricating biomass-derived materials, with a specific emphasis on their physicochemical properties characterized by controlled morphology, tunable electronic properties, and precise localization of active species, as well as the aspect of the intricate relationship between activity-structure and catalytic mechanisms, providing reference for future advancements in various catalysis fields involving biomass-derived materials.
2026, 37(8): 112405
doi: 10.1016/j.cclet.2026.112405
Abstract:
Indole-containing polyheterocycles belong to an extremely important class of organic compounds, and the related skeletons are found in many natural products and bioactive molecules. They play an important role in synthetic and medicinal chemistry, agrochemicals, and advanced materials. Moreover, they also serve as versatile building blocks and tools for constructing more complex molecules. Thus, development of efficient methods for assembly of indole-containing polyheterocycles has attracted considerable attention in recent years. The aim of this review is to summarize recent developments in the synthesis of indole-fused or spired polycyclic compounds via cyclization of indole-tethered alkenes. Indole-tethered alkenes with alkenyl species linked to different position of indole moiety is presented.
Indole-containing polyheterocycles belong to an extremely important class of organic compounds, and the related skeletons are found in many natural products and bioactive molecules. They play an important role in synthetic and medicinal chemistry, agrochemicals, and advanced materials. Moreover, they also serve as versatile building blocks and tools for constructing more complex molecules. Thus, development of efficient methods for assembly of indole-containing polyheterocycles has attracted considerable attention in recent years. The aim of this review is to summarize recent developments in the synthesis of indole-fused or spired polycyclic compounds via cyclization of indole-tethered alkenes. Indole-tethered alkenes with alkenyl species linked to different position of indole moiety is presented.
2026, 37(8): 112484
doi: 10.1016/j.cclet.2026.112484
Abstract:
Triketones are fundamental building blocks in discovering many bioactive compounds due to their unique structural features. With three carbonyl groups and the ability to tautomerize into enol forms, triketones can form hydrogen bond donors and acceptors when binding to receptors and serve as metal chelation function groups. This structural diversity enables triketone compounds to be widely applied in herbicides, fungicides, insecticides, anticancer treatments, and tyrosine metabolism disorders, particularly applications as HPPD (4-hydroxyphenylpyruvate dioxygenase) inhibitors, where their herbicidal activity stems from the disruption of plant photosynthesis processes to effectively control weed growth. Moreover, in materials applications, their excellent reactivity allows for the post-polymerization modification of triketone-modified polymers. To facilitate the discovery of triketone pesticides and drugs, in this review, we summarize the current research progress of triketone compounds, highlighting their potential mechanisms of action and environmental fate.
Triketones are fundamental building blocks in discovering many bioactive compounds due to their unique structural features. With three carbonyl groups and the ability to tautomerize into enol forms, triketones can form hydrogen bond donors and acceptors when binding to receptors and serve as metal chelation function groups. This structural diversity enables triketone compounds to be widely applied in herbicides, fungicides, insecticides, anticancer treatments, and tyrosine metabolism disorders, particularly applications as HPPD (4-hydroxyphenylpyruvate dioxygenase) inhibitors, where their herbicidal activity stems from the disruption of plant photosynthesis processes to effectively control weed growth. Moreover, in materials applications, their excellent reactivity allows for the post-polymerization modification of triketone-modified polymers. To facilitate the discovery of triketone pesticides and drugs, in this review, we summarize the current research progress of triketone compounds, highlighting their potential mechanisms of action and environmental fate.
2026, 37(8): 112643
doi: 10.1016/j.cclet.2026.112643
Abstract:
Transarterial chemoembolization (TACE) remains the standard of care for patients with unresectable hepatocellular carcinoma (HCC). However, clinical outcomes are frequently compromised by off-target toxicity, incomplete tumour necrosis, and the induction of a post-procedural immunosuppressive microenvironment. The integration of nanotechnology represents a paradigm shift designed to circumvent these biological and technical barriers. For instance, magnesium-enhanced TACE has demonstrated an objective response rate of ~93.3%, substantially surpassing that of conventional TACE therapies. This review evaluates nanotechnology's impact on TACE through four domains: Smart nanocarriers for stimuli-responsive delivery; theranostic platforms for real-time imaging; immune remodeling to boost immunotherapy; and next-generation embolic materials such as biodegradable polymers and liquid metals. Finally, we address the preclinical-to-clinical translation gap and outline a roadmap for personalized, high-precision interventional oncology.
Transarterial chemoembolization (TACE) remains the standard of care for patients with unresectable hepatocellular carcinoma (HCC). However, clinical outcomes are frequently compromised by off-target toxicity, incomplete tumour necrosis, and the induction of a post-procedural immunosuppressive microenvironment. The integration of nanotechnology represents a paradigm shift designed to circumvent these biological and technical barriers. For instance, magnesium-enhanced TACE has demonstrated an objective response rate of ~93.3%, substantially surpassing that of conventional TACE therapies. This review evaluates nanotechnology's impact on TACE through four domains: Smart nanocarriers for stimuli-responsive delivery; theranostic platforms for real-time imaging; immune remodeling to boost immunotherapy; and next-generation embolic materials such as biodegradable polymers and liquid metals. Finally, we address the preclinical-to-clinical translation gap and outline a roadmap for personalized, high-precision interventional oncology.
2026, 37(8): 112699
doi: 10.1016/j.cclet.2026.112699
Abstract:
The global spread of antibiotic resistance (AR) poses a critical public health threat, urgently requiring effective strategies to control antibiotic-resistant bacteria (ARB) and antibiotic resistance genes (ARGs) in water. Ultraviolet-based advanced oxidation processes (UVC/AOPs) offer a promising solution. By leveraging synergy between UVC light and oxidants (e.g., H2O2, PMS, O3, PAA, Cl2) to generate reactive radicals, they efficiently inactivate ARB, degrade ARGs, and suppress horizontal gene transfer (HGT). This review synthesizes recent advances, emphasizing: (1) Combined mechanisms of direct UVC damage and radical-mediated oxidation; (2) critical efficacy factors like radical kinetics and water matrix effects (DOM, salinity); and (3) key challenges including mechanistic gaps, particulate shielding of ARGs, and variable microbial susceptibility. To address these, we propose a machine learning-augmented approach integrating quantum chemical calculations and real-time spectroscopy to build predictive "radical-biotarget" models for intelligent optimization. While UVC/AOPs show broad efficacy and environmental promise, future research must prioritize elucidating fundamental mechanisms, optimizing parameters for diverse waters, and developing intelligent control systems to enhance specificity and resilience. Through such innovations, UVC/AOPs can become a core technology for precise AR risk management in water systems, providing a sustainable barrier against resistance spread.
The global spread of antibiotic resistance (AR) poses a critical public health threat, urgently requiring effective strategies to control antibiotic-resistant bacteria (ARB) and antibiotic resistance genes (ARGs) in water. Ultraviolet-based advanced oxidation processes (UVC/AOPs) offer a promising solution. By leveraging synergy between UVC light and oxidants (e.g., H2O2, PMS, O3, PAA, Cl2) to generate reactive radicals, they efficiently inactivate ARB, degrade ARGs, and suppress horizontal gene transfer (HGT). This review synthesizes recent advances, emphasizing: (1) Combined mechanisms of direct UVC damage and radical-mediated oxidation; (2) critical efficacy factors like radical kinetics and water matrix effects (DOM, salinity); and (3) key challenges including mechanistic gaps, particulate shielding of ARGs, and variable microbial susceptibility. To address these, we propose a machine learning-augmented approach integrating quantum chemical calculations and real-time spectroscopy to build predictive "radical-biotarget" models for intelligent optimization. While UVC/AOPs show broad efficacy and environmental promise, future research must prioritize elucidating fundamental mechanisms, optimizing parameters for diverse waters, and developing intelligent control systems to enhance specificity and resilience. Through such innovations, UVC/AOPs can become a core technology for precise AR risk management in water systems, providing a sustainable barrier against resistance spread.
2026, 37(8): 112721
doi: 10.1016/j.cclet.2026.112721
Abstract:
The application of MXene-based single-atom catalysts (SACs) in Fenton-like processes has emerged as a rapidly advancing research frontier in recent years. Early studies have demonstrated their superior activity in activating peroxymonosulfate or hydrogen peroxide for pollutant degradation compared to conventional nanoparticle catalysts, while recent efforts have shifted toward precise structural engineering and mechanistic understanding of reaction pathways. However, the transition from laboratory-scale synthesis to industrial implementation remains challenging, due to difficulties in developing green and scalable fabrication methods, long-term instability in complex water matrices, leaching of metal active centers, and the lack of cost-effective integration into continuous-flow systems such as fixed-bed reactors. To date, comprehensive reviews addressing their engineering applications remain limited. This review systematically summarizes advances in synthetic strategies and characterization techniques for achieving atomic dispersion, elucidates the structure–activity relationships and synergistic radical/non-radical mechanisms, and evaluates reactor design and scale-up potential. Particular emphasis is placed on operational adaptability and economic feasibility under real-world conditions. Future perspectives include the rational design of novel MXene supports, machine learning-assisted catalyst optimization, hybrid process integration, and the development of sustainability assessment frameworks, aiming to bridge the gap between fundamental discoveries and practical water purification technologies.
The application of MXene-based single-atom catalysts (SACs) in Fenton-like processes has emerged as a rapidly advancing research frontier in recent years. Early studies have demonstrated their superior activity in activating peroxymonosulfate or hydrogen peroxide for pollutant degradation compared to conventional nanoparticle catalysts, while recent efforts have shifted toward precise structural engineering and mechanistic understanding of reaction pathways. However, the transition from laboratory-scale synthesis to industrial implementation remains challenging, due to difficulties in developing green and scalable fabrication methods, long-term instability in complex water matrices, leaching of metal active centers, and the lack of cost-effective integration into continuous-flow systems such as fixed-bed reactors. To date, comprehensive reviews addressing their engineering applications remain limited. This review systematically summarizes advances in synthetic strategies and characterization techniques for achieving atomic dispersion, elucidates the structure–activity relationships and synergistic radical/non-radical mechanisms, and evaluates reactor design and scale-up potential. Particular emphasis is placed on operational adaptability and economic feasibility under real-world conditions. Future perspectives include the rational design of novel MXene supports, machine learning-assisted catalyst optimization, hybrid process integration, and the development of sustainability assessment frameworks, aiming to bridge the gap between fundamental discoveries and practical water purification technologies.
2026, 37(8): 112642
doi: 10.1016/j.cclet.2026.112642
Abstract:
