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2026 Volume 7 Issue 2
2026, 37(2): 110588
doi: 10.1016/j.cclet.2024.110588
Abstract:
Exploring new material systems and enhancing the birefringence of compounds is a highly valuable endeavor. In this study, we introduce a novel method to enhance the birefringence of inorganic compounds by inducing structural alignment through linear groups and fluoride ions. We report on two new compounds: HgGa2(SeO3)4 and Hg2Ga(SeO3)2F. HgGa2(SeO3)4 crystallizes in a non-centrosymmetric (NCS) space group, exhibiting a second harmonic generation (SHG) efficiency of approximately 60% that of commercial KH2PO4 (KDP), with a birefringence of 0.032@546 nm. Hg2Ga(SeO3)2F, on the other hand, crystallizes in a centrosymmetric space (CS) group and represents the first reported HgⅠ-based selenite birefringent material. Due to the influence of the linear group Hg2O2, its birefringence is significantly enhanced to 0.111@546 nm, which is 3.5 times that of HgGa2(SeO3)4. Moreover, both compounds demonstrate high stability and a broad optical transparency window. These findings indicate that Hg2Ga(SeO3)2F is a promising candidate for birefringent material in the mid-infrared (MIR) range. Our research provides an innovative strategy for improving the birefringence of compounds.
Exploring new material systems and enhancing the birefringence of compounds is a highly valuable endeavor. In this study, we introduce a novel method to enhance the birefringence of inorganic compounds by inducing structural alignment through linear groups and fluoride ions. We report on two new compounds: HgGa2(SeO3)4 and Hg2Ga(SeO3)2F. HgGa2(SeO3)4 crystallizes in a non-centrosymmetric (NCS) space group, exhibiting a second harmonic generation (SHG) efficiency of approximately 60% that of commercial KH2PO4 (KDP), with a birefringence of 0.032@546 nm. Hg2Ga(SeO3)2F, on the other hand, crystallizes in a centrosymmetric space (CS) group and represents the first reported HgⅠ-based selenite birefringent material. Due to the influence of the linear group Hg2O2, its birefringence is significantly enhanced to 0.111@546 nm, which is 3.5 times that of HgGa2(SeO3)4. Moreover, both compounds demonstrate high stability and a broad optical transparency window. These findings indicate that Hg2Ga(SeO3)2F is a promising candidate for birefringent material in the mid-infrared (MIR) range. Our research provides an innovative strategy for improving the birefringence of compounds.
2026, 37(2): 110590
doi: 10.1016/j.cclet.2024.110590
Abstract:
In comparison with their 2D and 3D counterparts, 1D covalent organic frameworks (COFs) have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed. Herein, two novel imide-linked 1D COFs with phthalocyanine building blocks, namely NiPc-CZDM-COF and NiPc-CZDL-COF, were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(Ⅱ) (NiPc(COOH)8) with 9H-carbazole-3,6-diamine (CZDM) and 4,4′-(9H-carbazole-3,6-diyl)dianiline (CZDL), respectively. Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy. Due to their high ratio of exposed active centers on the edge sites of porous ribbons, both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0% and 7.5% according to the electrochemical measurement, resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH3 Faradaic efficiency of nearly 100%. In particular, NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH3 partial current density of −246 mA/cm2, ammonia yield rate of 19.5 mg cm−2 h−1, and turnover frequency of 5.8 s−1 at −1.2 V in an H-type cell associated with its higher conductivity. This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.
In comparison with their 2D and 3D counterparts, 1D covalent organic frameworks (COFs) have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed. Herein, two novel imide-linked 1D COFs with phthalocyanine building blocks, namely NiPc-CZDM-COF and NiPc-CZDL-COF, were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(Ⅱ) (NiPc(COOH)8) with 9H-carbazole-3,6-diamine (CZDM) and 4,4′-(9H-carbazole-3,6-diyl)dianiline (CZDL), respectively. Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy. Due to their high ratio of exposed active centers on the edge sites of porous ribbons, both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0% and 7.5% according to the electrochemical measurement, resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH3 Faradaic efficiency of nearly 100%. In particular, NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH3 partial current density of −246 mA/cm2, ammonia yield rate of 19.5 mg cm−2 h−1, and turnover frequency of 5.8 s−1 at −1.2 V in an H-type cell associated with its higher conductivity. This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.
2026, 37(2): 110591
doi: 10.1016/j.cclet.2024.110591
Abstract:
Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures, bringing challenges to the application of lithium-ion batteries (LIBs) at low temperatures. Herein, the ester solvent of methyl propionate (MP) with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes. Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions. The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied. As a result, methyl pentafluoropropionate (M5F) with five fluorine atoms was selected for its optimal interactions with both Li+ and MP solvent in the primary solvation structure, contributing to desired solvation structure for fast interfacial transport. The LiFePO4 (LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8% after 120 cycles and retained 81.2% of room-temperature capacity when charged and discharged at −30 ℃. 1 Ah LFP||graphite pouch cell with high cathode loading (20 mg/cm2) in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at −20 ℃. This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application.
Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures, bringing challenges to the application of lithium-ion batteries (LIBs) at low temperatures. Herein, the ester solvent of methyl propionate (MP) with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes. Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions. The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied. As a result, methyl pentafluoropropionate (M5F) with five fluorine atoms was selected for its optimal interactions with both Li+ and MP solvent in the primary solvation structure, contributing to desired solvation structure for fast interfacial transport. The LiFePO4 (LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8% after 120 cycles and retained 81.2% of room-temperature capacity when charged and discharged at −30 ℃. 1 Ah LFP||graphite pouch cell with high cathode loading (20 mg/cm2) in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at −20 ℃. This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application.
2026, 37(2): 110592
doi: 10.1016/j.cclet.2024.110592
Abstract:
There are limitations to using hard carbon (HC) in K+ storage due to its insufficient high-current reversible capacity and plateau potential, which result from the lack of effective active sites and low intercalation capabilities. The construction of HC cathodes with more available functional groups and ordered carbon nanocrystal structures is essential for improving K+ storage efficiency. Herein, a new perspective is proposed for synthesizing hard carbon nanosheets (HCNS) with abundant hydroxyl groups (O-H)/carboxylic groups (O-C = O) and rational carbon nanocrystals by interfacial assembly and carbonization. Systematic in ex-situ observations, dynamic analysis and theory calculations elucidate that the superior electrochemical capability of HCNS is ascribed to the synergistic effect of abundant available functional groups and ordered graphitic microcrystalline. Consequently, the HCNS exhibits outstanding K+ storage capabilities in terms of superb energy density (146.2 Wh/kg), high power density (1,7800 Wh/kg), and ultralong lifespan (102.9% capacity retention after 10,000 cycles). It was also found that the HC structure correlates with the discharge/charge plateau, confirming the 'adsorption-insertion' charge storage mechanism. Furthermore, the proposed work provides a theoretical basis for making high-performance HC anodes by understanding the effect of their microstructure on K+ storage.
There are limitations to using hard carbon (HC) in K+ storage due to its insufficient high-current reversible capacity and plateau potential, which result from the lack of effective active sites and low intercalation capabilities. The construction of HC cathodes with more available functional groups and ordered carbon nanocrystal structures is essential for improving K+ storage efficiency. Herein, a new perspective is proposed for synthesizing hard carbon nanosheets (HCNS) with abundant hydroxyl groups (O-H)/carboxylic groups (O-C = O) and rational carbon nanocrystals by interfacial assembly and carbonization. Systematic in ex-situ observations, dynamic analysis and theory calculations elucidate that the superior electrochemical capability of HCNS is ascribed to the synergistic effect of abundant available functional groups and ordered graphitic microcrystalline. Consequently, the HCNS exhibits outstanding K+ storage capabilities in terms of superb energy density (146.2 Wh/kg), high power density (1,7800 Wh/kg), and ultralong lifespan (102.9% capacity retention after 10,000 cycles). It was also found that the HC structure correlates with the discharge/charge plateau, confirming the 'adsorption-insertion' charge storage mechanism. Furthermore, the proposed work provides a theoretical basis for making high-performance HC anodes by understanding the effect of their microstructure on K+ storage.
2026, 37(2): 110605
doi: 10.1016/j.cclet.2024.110605
Abstract:
The intrinsic insulation and drastic volume change of the red phosphorus during the 3-electron alloying process greatly limits its widespread applications in sodium-ion batteries. Here, we report a monomicelle-directed assembly approach for controllable synthesis of monodispersed mesoporous polypyrrole (PPy) nanospheres, which allows for the shape-preserving conversion into N-doped carbon with regular mesoscopic pore and high surface area, thus affording a high dispersion of red phosphorus during melt impregnation process due to the available diffusion apertures and strong molecular chemical anchoring. Moreover, the theoretical calculations further revealed that positively polarized pyridine N atoms in N-doped mesoporous carbon nanospheres can empower comprehensive regulation of red phosphorus adsorption by strong chemical binding. Benefitting from the above advantages, the resultant red phosphorus host for sodium-ion batteries delivered an outstanding reversible capacity of 856 mAh/g with a capacity fading rate of only 0.025% per cycle during 1000 cycles at 1.0 A/g. This work provides an effective approach based on monomicelle-directed assembly engineering of carbon-based phosphorus hosts for advanced energy conversion and storage systems.
The intrinsic insulation and drastic volume change of the red phosphorus during the 3-electron alloying process greatly limits its widespread applications in sodium-ion batteries. Here, we report a monomicelle-directed assembly approach for controllable synthesis of monodispersed mesoporous polypyrrole (PPy) nanospheres, which allows for the shape-preserving conversion into N-doped carbon with regular mesoscopic pore and high surface area, thus affording a high dispersion of red phosphorus during melt impregnation process due to the available diffusion apertures and strong molecular chemical anchoring. Moreover, the theoretical calculations further revealed that positively polarized pyridine N atoms in N-doped mesoporous carbon nanospheres can empower comprehensive regulation of red phosphorus adsorption by strong chemical binding. Benefitting from the above advantages, the resultant red phosphorus host for sodium-ion batteries delivered an outstanding reversible capacity of 856 mAh/g with a capacity fading rate of only 0.025% per cycle during 1000 cycles at 1.0 A/g. This work provides an effective approach based on monomicelle-directed assembly engineering of carbon-based phosphorus hosts for advanced energy conversion and storage systems.
2026, 37(2): 110622
doi: 10.1016/j.cclet.2024.110622
Abstract:
The high voltage of Li||LiCoO2 battery can increase the energy density. However, the cycling performance associated with cathode structural stability remains challenging. To address this question, we proposed an electrolyte strategy for improving the performance of 4.6 V Li||LiCoO2 battery by using trimethylsilyl isocyanate (TMIS) as electrolyte additive. The trimethylsilyl group of TMIS can trap HF while the isocyanate group brings polyamide components to the CEI and the SEI. By the synergistic action, the Co3+ dissolution problem of the LiCoO2 cathode was effectively curbed. Furthermore, TMIS regulates the construction of anion-dominated LiF-rich SEI by influencing the solvation structure of Li+. As expected, the 4.6 V Li||LiCoO2 battery with TMIS retains 77.9% initial capacity after 200 cycles at 0.5 C.
The high voltage of Li||LiCoO2 battery can increase the energy density. However, the cycling performance associated with cathode structural stability remains challenging. To address this question, we proposed an electrolyte strategy for improving the performance of 4.6 V Li||LiCoO2 battery by using trimethylsilyl isocyanate (TMIS) as electrolyte additive. The trimethylsilyl group of TMIS can trap HF while the isocyanate group brings polyamide components to the CEI and the SEI. By the synergistic action, the Co3+ dissolution problem of the LiCoO2 cathode was effectively curbed. Furthermore, TMIS regulates the construction of anion-dominated LiF-rich SEI by influencing the solvation structure of Li+. As expected, the 4.6 V Li||LiCoO2 battery with TMIS retains 77.9% initial capacity after 200 cycles at 0.5 C.
2026, 37(2): 110828
doi: 10.1016/j.cclet.2025.110828
Abstract:
The insufficient performance of Pt and Pd benchmark catalysts remains a significant obstacle to the practical application of direct liquid fuel cells. In this study, we report a synthesis of amorphous PdSe/crystalline Pt nanoparticles (AC-PdPtSe NPs) by chemical leaching of PdPtSe NPs. AC-PdPtSe NPs display significantly enhanced activity and stability for the electrooxidation of ethylene glycol and glycerol, far surpassing that of amorphous-dominant PdPtSe NPs, commercial Pd/C, and Pt/C catalysts. Notably, the integration of crystalline and amorphous domains leverages the advantages of high electrical conductivity and a wealth of active sites, which can substantially accelerate reaction kinetics. Furthermore, detailed investigations reveal that the boundary between the Pt crystalline and PdSe amorphous phases induces a 3% surface tensile strain. The formation of amorphous-crystalline heterointerfaces optimizes the d-band states, thereby strengthening the adsorption and activation of ethylene glycol and glycerol. This study highlights the advance in phase engineering toward the development of highly active noble-metal nanostructures.
The insufficient performance of Pt and Pd benchmark catalysts remains a significant obstacle to the practical application of direct liquid fuel cells. In this study, we report a synthesis of amorphous PdSe/crystalline Pt nanoparticles (AC-PdPtSe NPs) by chemical leaching of PdPtSe NPs. AC-PdPtSe NPs display significantly enhanced activity and stability for the electrooxidation of ethylene glycol and glycerol, far surpassing that of amorphous-dominant PdPtSe NPs, commercial Pd/C, and Pt/C catalysts. Notably, the integration of crystalline and amorphous domains leverages the advantages of high electrical conductivity and a wealth of active sites, which can substantially accelerate reaction kinetics. Furthermore, detailed investigations reveal that the boundary between the Pt crystalline and PdSe amorphous phases induces a 3% surface tensile strain. The formation of amorphous-crystalline heterointerfaces optimizes the d-band states, thereby strengthening the adsorption and activation of ethylene glycol and glycerol. This study highlights the advance in phase engineering toward the development of highly active noble-metal nanostructures.
2026, 37(2): 110830
doi: 10.1016/j.cclet.2025.110830
Abstract:
Designing a highly active and stable bifunctional catalyst is essential for achieving superior overall water splitting (OWS). In this study, a three-dimensional (3D) core-shell structure Co3S4/CuS@NiFe LDH nanocoral spheres electrocatalyst was constructed on nickel foam (NF) via an interfacial engineering strategy. This 3D core-shell heterostructure maximizes the exposure of active sites, optimizes the charge transport pathway and accelerates gas release rates. The protective shell strategy of NiFe LDH provides favorable stability, which contributes to inhibiting the electrochemical corrosion of the electrocatalyst and mitigating the toxic effects of Cl− and other microorganisms during the seawater splitting process. Moreover, the introduction of NiFe LDH induces a change in the OER mechanism from an adsorption evolution mechanism (AEM) to a lattice oxygen mechanism (LOM), which improves the intrinsic activity of the catalyst. Consequently, Co3S4/CuS@NiFe LDH demonstrates exceptional performance in the oxygen evolution reaction (OER) (η100 = 251 mV) and in the hydrogen evolution reaction (HER) (η100 = 254 mV), alongside remarkable stability over 100 h. For OWS, it exhibits a voltage of 1.46 V at 10 mA/cm2 and maintain stability for 100 h. Impressively, Co3S4/CuS@NiFe LDH still possesses outstanding activity and stability in natural alkaline seawater. This work proposes interfacial engineering to construct bifunctional catalysts with core-shell heterostructures, providing instructive guidelines for the design of highly efficient electrocatalysts toward seawater electrolysis.
Designing a highly active and stable bifunctional catalyst is essential for achieving superior overall water splitting (OWS). In this study, a three-dimensional (3D) core-shell structure Co3S4/CuS@NiFe LDH nanocoral spheres electrocatalyst was constructed on nickel foam (NF) via an interfacial engineering strategy. This 3D core-shell heterostructure maximizes the exposure of active sites, optimizes the charge transport pathway and accelerates gas release rates. The protective shell strategy of NiFe LDH provides favorable stability, which contributes to inhibiting the electrochemical corrosion of the electrocatalyst and mitigating the toxic effects of Cl− and other microorganisms during the seawater splitting process. Moreover, the introduction of NiFe LDH induces a change in the OER mechanism from an adsorption evolution mechanism (AEM) to a lattice oxygen mechanism (LOM), which improves the intrinsic activity of the catalyst. Consequently, Co3S4/CuS@NiFe LDH demonstrates exceptional performance in the oxygen evolution reaction (OER) (η100 = 251 mV) and in the hydrogen evolution reaction (HER) (η100 = 254 mV), alongside remarkable stability over 100 h. For OWS, it exhibits a voltage of 1.46 V at 10 mA/cm2 and maintain stability for 100 h. Impressively, Co3S4/CuS@NiFe LDH still possesses outstanding activity and stability in natural alkaline seawater. This work proposes interfacial engineering to construct bifunctional catalysts with core-shell heterostructures, providing instructive guidelines for the design of highly efficient electrocatalysts toward seawater electrolysis.
2026, 37(2): 110951
doi: 10.1016/j.cclet.2025.110951
Abstract:
New-skeleton terpenoids have prompted considerable interest owing to their chemical and biological significance. A chemical study on the bark of Croton laui led to the isolation and identification of a new norsesterterpenoid, crolatinoid A (1), and two new neoclerodane diterpenoids, crolatinoids B and C (2 and 3). Structurally, compound 1 exhibits an unprecedented 12,17-cyclo20-nor phenyllabdane skeleton. Compound 2 features a novel 19(5→4)-abeo-3,5-cycloneoclerodane skeleton, which is hypothetically derived from precursor 3 through an oxa-di-π-methane rearrangement process. Furthermore, compound 1 demonstrated a significant capacity to reverse multidrug resistance in paclitaxel-resistant HCT-15 cells with a reversal fold value of 16. All three compounds displayed adipogenesis inhibition in 3T3-L1 adipocytes.
New-skeleton terpenoids have prompted considerable interest owing to their chemical and biological significance. A chemical study on the bark of Croton laui led to the isolation and identification of a new norsesterterpenoid, crolatinoid A (1), and two new neoclerodane diterpenoids, crolatinoids B and C (2 and 3). Structurally, compound 1 exhibits an unprecedented 12,17-cyclo20-nor phenyllabdane skeleton. Compound 2 features a novel 19(5→4)-abeo-3,5-cycloneoclerodane skeleton, which is hypothetically derived from precursor 3 through an oxa-di-π-methane rearrangement process. Furthermore, compound 1 demonstrated a significant capacity to reverse multidrug resistance in paclitaxel-resistant HCT-15 cells with a reversal fold value of 16. All three compounds displayed adipogenesis inhibition in 3T3-L1 adipocytes.
2026, 37(2): 110961
doi: 10.1016/j.cclet.2025.110961
Abstract:
Triple-negative breast cancer (TNBC) presents significant diagnostic and therapeutic challenges due to the lack of targeted treatments, rapid progression, high recurrence and metastasis rates, and overall poorer prognosis. Herein, the targeted theranostic platform of cysteine-modified gold nanodots-sulfhydrated luteinizing hormone releasing hormone (CGN-SLR) nanosystem was designed for target recognition and precise dual-mode imaging-guided photothermal therapy (PTT) against TNBC. On the one hand, the CGN-SLR nanosystem can serve as an ideal targeting fluorescent probe and computed tomography (CT) enhancer to facilitate the accurate diagnosis and surgical guidance of TNBC. On the other hand, the CGN-SLR nanosystem with great targeting and PTT ability can significantly inhibit the growth of TNBC, without causing harm to normal tissues and healthy organs. It provides an effective strategy for the diagnosis and treatment of TNBC through the rational design of multifunctional nanoplatform with target recognition, multiple imaging guidance/monitoring, and high-efficiency PTT.
Triple-negative breast cancer (TNBC) presents significant diagnostic and therapeutic challenges due to the lack of targeted treatments, rapid progression, high recurrence and metastasis rates, and overall poorer prognosis. Herein, the targeted theranostic platform of cysteine-modified gold nanodots-sulfhydrated luteinizing hormone releasing hormone (CGN-SLR) nanosystem was designed for target recognition and precise dual-mode imaging-guided photothermal therapy (PTT) against TNBC. On the one hand, the CGN-SLR nanosystem can serve as an ideal targeting fluorescent probe and computed tomography (CT) enhancer to facilitate the accurate diagnosis and surgical guidance of TNBC. On the other hand, the CGN-SLR nanosystem with great targeting and PTT ability can significantly inhibit the growth of TNBC, without causing harm to normal tissues and healthy organs. It provides an effective strategy for the diagnosis and treatment of TNBC through the rational design of multifunctional nanoplatform with target recognition, multiple imaging guidance/monitoring, and high-efficiency PTT.
2026, 37(2): 110965
doi: 10.1016/j.cclet.2025.110965
Abstract:
Triterpenoids are valuable medicinal scaffolds, characterized by excellent pharmacological properties and the presence of hydroxyl and carboxyl groups that allow for further structural modifications. Expanding the scope of oxidative modifications on these molecules is crucial for increasing their synthetic structural diversity and unlocking new potential pharmacological activities. However, the progress has been limited by the scarcity of suitable tailoring enzymes. Here, we reported a break-through in achieving targeted and remote dual-site oxidation of licorice triterpenoids using a single P450 mutant. This approach successfully enabled the selective synthesis of the rare triterpenoid, liquiritic acid and 24-OH-liquiritic acid. Our findings demonstrate that microenvironmental accessibility engineering of triterpenoid substrates within the P450 enzyme is essential for continuous and regioselective oxidation. This study not only sheds light on the mechanistic aspects of P450 catalysis but also expands the enzymatic toolkit for selective oxidative modifications in triterpenoid biosynthesis.
Triterpenoids are valuable medicinal scaffolds, characterized by excellent pharmacological properties and the presence of hydroxyl and carboxyl groups that allow for further structural modifications. Expanding the scope of oxidative modifications on these molecules is crucial for increasing their synthetic structural diversity and unlocking new potential pharmacological activities. However, the progress has been limited by the scarcity of suitable tailoring enzymes. Here, we reported a break-through in achieving targeted and remote dual-site oxidation of licorice triterpenoids using a single P450 mutant. This approach successfully enabled the selective synthesis of the rare triterpenoid, liquiritic acid and 24-OH-liquiritic acid. Our findings demonstrate that microenvironmental accessibility engineering of triterpenoid substrates within the P450 enzyme is essential for continuous and regioselective oxidation. This study not only sheds light on the mechanistic aspects of P450 catalysis but also expands the enzymatic toolkit for selective oxidative modifications in triterpenoid biosynthesis.
2026, 37(2): 110977
doi: 10.1016/j.cclet.2025.110977
Abstract:
The level of glutathione (GSH) is significantly associated with numerous pathological processes, thus, real-time detection of the GSH level is of significance for early diagnosis of GSH-related diseases. Herein, we developed in vivo second near-infrared (NIR-Ⅱ) window fluorescence (FL) and ratiometric photoacoustic (RPA) dual-modality imaging of GSH using a GSH-activatable probe (LET-14). LET-14 was synthesized based on a rhodamine hybrid xanthene skeleton with a FL shielding 2,4-dinitrobenzene sulfonyl group that can be specifically cleaved by GSH, thus resulting in a markedly bathochromic-shift absorption, a 6.5-fold increase in NIR-Ⅱ FL intensity (FL920) and a 13-fold increase in RPA signal (PA880/PA705) in vitro. Intriguingly, LET-14 exhibits good selectivity and sensitivity for NIR-Ⅱ FL and RPA dual-modality imaging of GSH in 4T1 tumor-bearing mouse model. Our findings develop an in vivo detection tool of GSH, which has great potential in the field of cancer diagnosis.
The level of glutathione (GSH) is significantly associated with numerous pathological processes, thus, real-time detection of the GSH level is of significance for early diagnosis of GSH-related diseases. Herein, we developed in vivo second near-infrared (NIR-Ⅱ) window fluorescence (FL) and ratiometric photoacoustic (RPA) dual-modality imaging of GSH using a GSH-activatable probe (LET-14). LET-14 was synthesized based on a rhodamine hybrid xanthene skeleton with a FL shielding 2,4-dinitrobenzene sulfonyl group that can be specifically cleaved by GSH, thus resulting in a markedly bathochromic-shift absorption, a 6.5-fold increase in NIR-Ⅱ FL intensity (FL920) and a 13-fold increase in RPA signal (PA880/PA705) in vitro. Intriguingly, LET-14 exhibits good selectivity and sensitivity for NIR-Ⅱ FL and RPA dual-modality imaging of GSH in 4T1 tumor-bearing mouse model. Our findings develop an in vivo detection tool of GSH, which has great potential in the field of cancer diagnosis.
2026, 37(2): 110992
doi: 10.1016/j.cclet.2025.110992
Abstract:
The von Hippel-Lindau tumor suppressor (VHL) has been extensively used to develop degraders targeting numerous proteins of interest. However, studies on the rational design of VHL-proteolysis-targeting chimeras (PROTACs) remain scarce. This study aimed to develop strategies to investigate VHL-recruiting PROTACs connecting with varying attachment sites on VHL ligands, which could be utilized for KRASG12C degraders development and expanded to additional targets. We developed a molecular dynamics (MD)-based strategy to explore the stability of ternary complexes induced by KRASG12C PROTACs with four distinct attachment sites of VH032. We found a potent degrader namely YN14-H, linked to hydroxyl group on VH032 benzene ring, exhibited the most superior ability of inducing ternary complexes, reflected by the lowest dissociation constant (Kd) for ternary complex induction and the highest AlphaScreen (AS)-based interaction. YN14-H inhibited cell growth with low nanomolar half maximal inhibitory concentration (IC50) and half maximal degradation concentration (DC50) values as well as >98% of maximum degradation (Dmax) in NCI-H358 and MIA PaCa-2 cells harboring KRASG12C-mutation. Mechanistically, YN14-H significantly induced apoptosis and inhibited the migratory capacity. Notably, YN14-H demonstrated favorable pharmacokinetic properties and excellent antitumor activity in vivo. Furthermore, bromodomain-containing protein 7 (BRD7) and Bruton tyrosine kinase (BTK) degraders attached to distinct sites on VH032 further verified the rationality and universality of our MD-based strategies. Our findings demonstrated that YN14-H could serve as a promising candidate for the treatment of tumors with KRASG12C-mutation and present a strategy for the rational design of VHL-recruiting PROTACs that target additional proteins at distinct attachment sites.
The von Hippel-Lindau tumor suppressor (VHL) has been extensively used to develop degraders targeting numerous proteins of interest. However, studies on the rational design of VHL-proteolysis-targeting chimeras (PROTACs) remain scarce. This study aimed to develop strategies to investigate VHL-recruiting PROTACs connecting with varying attachment sites on VHL ligands, which could be utilized for KRASG12C degraders development and expanded to additional targets. We developed a molecular dynamics (MD)-based strategy to explore the stability of ternary complexes induced by KRASG12C PROTACs with four distinct attachment sites of VH032. We found a potent degrader namely YN14-H, linked to hydroxyl group on VH032 benzene ring, exhibited the most superior ability of inducing ternary complexes, reflected by the lowest dissociation constant (Kd) for ternary complex induction and the highest AlphaScreen (AS)-based interaction. YN14-H inhibited cell growth with low nanomolar half maximal inhibitory concentration (IC50) and half maximal degradation concentration (DC50) values as well as >98% of maximum degradation (Dmax) in NCI-H358 and MIA PaCa-2 cells harboring KRASG12C-mutation. Mechanistically, YN14-H significantly induced apoptosis and inhibited the migratory capacity. Notably, YN14-H demonstrated favorable pharmacokinetic properties and excellent antitumor activity in vivo. Furthermore, bromodomain-containing protein 7 (BRD7) and Bruton tyrosine kinase (BTK) degraders attached to distinct sites on VH032 further verified the rationality and universality of our MD-based strategies. Our findings demonstrated that YN14-H could serve as a promising candidate for the treatment of tumors with KRASG12C-mutation and present a strategy for the rational design of VHL-recruiting PROTACs that target additional proteins at distinct attachment sites.
2026, 37(2): 111014
doi: 10.1016/j.cclet.2025.111014
Abstract:
The protein corona formation has been reported to influence the liposomes’ behavioral performance in vivo. Accordingly, the effect of physiologically relevant inorganic ion pairs (sodium chloride, sodium sulfate, magnesium chloride, and magnesium sulfate) was investigated. Bovine serum albumin (BSA) was selected as the model protein. Parameters including particle size and zeta potential were assessed, while various spectroscopic techniques were utilized to elucidate the changes in BSA during its interaction with liposomes. The particle size and light intensity distribution changes indicated that the introduction of inorganic pairs, especially the metal cations, could significantly influence both the adsorption of BSA and the aggregation of particles. Furthermore, spectral characterization elucidated that BSA exhibited more extended peptide chains with enhanced exposure to hydrophobic acid amino residues upon adding ion pairs. Electrostatic adsorption and chelation insertion were proposed as metal ion binding modes and the corresponding BSA corona formation. In the electrostatic adsorption mode, sodium ions can enhance the electrostatic interactions, facilitating the “connection” between BSA and liposomes. Magnesium ions can induce stronger hydrophobic interactions through chelation, effectively “drag” BSA segments into the lipid bilayer. This work highlighted important physiological factors for protein-liposome interaction and provided rational model constructions to lay the foundation for further relevant studies.
The protein corona formation has been reported to influence the liposomes’ behavioral performance in vivo. Accordingly, the effect of physiologically relevant inorganic ion pairs (sodium chloride, sodium sulfate, magnesium chloride, and magnesium sulfate) was investigated. Bovine serum albumin (BSA) was selected as the model protein. Parameters including particle size and zeta potential were assessed, while various spectroscopic techniques were utilized to elucidate the changes in BSA during its interaction with liposomes. The particle size and light intensity distribution changes indicated that the introduction of inorganic pairs, especially the metal cations, could significantly influence both the adsorption of BSA and the aggregation of particles. Furthermore, spectral characterization elucidated that BSA exhibited more extended peptide chains with enhanced exposure to hydrophobic acid amino residues upon adding ion pairs. Electrostatic adsorption and chelation insertion were proposed as metal ion binding modes and the corresponding BSA corona formation. In the electrostatic adsorption mode, sodium ions can enhance the electrostatic interactions, facilitating the “connection” between BSA and liposomes. Magnesium ions can induce stronger hydrophobic interactions through chelation, effectively “drag” BSA segments into the lipid bilayer. This work highlighted important physiological factors for protein-liposome interaction and provided rational model constructions to lay the foundation for further relevant studies.
2026, 37(2): 111017
doi: 10.1016/j.cclet.2025.111017
Abstract:
Hemorrhagic shock (HS) is a leading cause of death worldwide, particularly within the first 24 h post-injury. Current treatments are limited, especially in low-resource settings. Therapeutic hypothermia (TH) offers potential benefits by reducing metabolic demands and protecting organs, but its application in HS is challenged by cooling difficulties and side effects. This study introduces a novel nasal gel formulation of N6-cyclohexyladenosine (CHA), an adenosine A1 receptor agonist, designed to enhance brain delivery while minimizing peripheral side effects. In a mouse model of HS, administration of CHA nasal gel significantly improved survival rates, reduced metabolic rates, and protected major organs without worsening coagulopathy. Metabolomics analysis revealed a shift towards fatty acid oxidation and increased antioxidant capacity. These findings demonstrate that CHA nasal gel effectively induces TH, offering a safe and innovative treatment strategy for HS, particularly in resource-limited environments.
Hemorrhagic shock (HS) is a leading cause of death worldwide, particularly within the first 24 h post-injury. Current treatments are limited, especially in low-resource settings. Therapeutic hypothermia (TH) offers potential benefits by reducing metabolic demands and protecting organs, but its application in HS is challenged by cooling difficulties and side effects. This study introduces a novel nasal gel formulation of N6-cyclohexyladenosine (CHA), an adenosine A1 receptor agonist, designed to enhance brain delivery while minimizing peripheral side effects. In a mouse model of HS, administration of CHA nasal gel significantly improved survival rates, reduced metabolic rates, and protected major organs without worsening coagulopathy. Metabolomics analysis revealed a shift towards fatty acid oxidation and increased antioxidant capacity. These findings demonstrate that CHA nasal gel effectively induces TH, offering a safe and innovative treatment strategy for HS, particularly in resource-limited environments.
2026, 37(2): 111020
doi: 10.1016/j.cclet.2025.111020
Abstract:
Thermoplastic polyurethane (TPU) consists of a hard segment and a soft segment, where the former affords mechanical strength and thermal stability, while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt. Thus, TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries. However, the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains, which greatly reduces the dissociation of lithium salts. Herein, a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate) (PEGDA) in fully dispersed TPU. Hence a stretchable solid-state electrolyte (denoted as TELL and the contrast sample was denoted as TLL) with high ionic conductivity of 7.18 × 10−4 S/cm was obtained at room temperature. The Li+ transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm2, while the contrast sample is short-circuited after 634 h of cycling. The LiFePO4|TELL|Li cell achieves a capacity retention of 78.93% after 200 cycles at 2 C. The LiFePO4|TLL|Li cell only gains the capacity retention of 51.9% after 50 cycles at the same current density. So, the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.
Thermoplastic polyurethane (TPU) consists of a hard segment and a soft segment, where the former affords mechanical strength and thermal stability, while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt. Thus, TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries. However, the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains, which greatly reduces the dissociation of lithium salts. Herein, a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate) (PEGDA) in fully dispersed TPU. Hence a stretchable solid-state electrolyte (denoted as TELL and the contrast sample was denoted as TLL) with high ionic conductivity of 7.18 × 10−4 S/cm was obtained at room temperature. The Li+ transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm2, while the contrast sample is short-circuited after 634 h of cycling. The LiFePO4|TELL|Li cell achieves a capacity retention of 78.93% after 200 cycles at 2 C. The LiFePO4|TLL|Li cell only gains the capacity retention of 51.9% after 50 cycles at the same current density. So, the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.
2026, 37(2): 111031
doi: 10.1016/j.cclet.2025.111031
Abstract:
In situ tumor vaccines, which leverage the antigenic profile of individual tumors, have demonstrated significant potential in tumor immunotherapy. However, their efficacy is often limited by the immunosuppressive tumor microenvironment (TME) and insufficient tumor targeting. To address these challenges, we engineered in situ nanovaccines through the self-assembly of the photosensitizer indocyanine green, immune adjuvant aluminum (Al3+), and hydrophilic drug zoledronic acid (ZOL). Intravenous injection of these nanovaccines led to efficient tumor accumulation, enhancing drug bioavailability and enabling the release of tumor-associated antigens via photothermal therapy. Additionally, the built-in ZOL induces polarization of tumor-associated macrophages, reversing the immunosuppressive TME. The potent antitumor immune response triggered by these nanovaccines effectively suppresses tumor growth. This study, which integrates a straightforward assembly method, substantial drug loading capacity, and promising therapeutic outcomes, introduces a novel and effective paradigm for carrier-free in situ nanovaccines in cancer treatment.
In situ tumor vaccines, which leverage the antigenic profile of individual tumors, have demonstrated significant potential in tumor immunotherapy. However, their efficacy is often limited by the immunosuppressive tumor microenvironment (TME) and insufficient tumor targeting. To address these challenges, we engineered in situ nanovaccines through the self-assembly of the photosensitizer indocyanine green, immune adjuvant aluminum (Al3+), and hydrophilic drug zoledronic acid (ZOL). Intravenous injection of these nanovaccines led to efficient tumor accumulation, enhancing drug bioavailability and enabling the release of tumor-associated antigens via photothermal therapy. Additionally, the built-in ZOL induces polarization of tumor-associated macrophages, reversing the immunosuppressive TME. The potent antitumor immune response triggered by these nanovaccines effectively suppresses tumor growth. This study, which integrates a straightforward assembly method, substantial drug loading capacity, and promising therapeutic outcomes, introduces a novel and effective paradigm for carrier-free in situ nanovaccines in cancer treatment.
2026, 37(2): 111048
doi: 10.1016/j.cclet.2025.111048
Abstract:
Hyperactivation of DNA repairing pathway is highly associated with the chemosensitivity and chemoresistance of cancer cells. In this manuscript, guided by cascaded one strain many compounds-global natural products social molecular networking (OSMAC-GNPS) strategy, a pair of epimeric environmental-induced metabolites were isolated from Aspergillus sp. EGF 15-0-3. Structurally, sterpiperazines A (1) and B (2) represent the first steroid-based indole alkaloids with unprecedented backbones. Biologically, compound 1 could be identified as a novel tyrosyl-DNA phosphodiesterase 1 (Tdp1) inhibitor with a unique mechanism distinct from the reported modulators, and was able to significantly enhance the sensitivity of NCI-H460 cells to the clinic chemotherapeutic drug through inhibiting the DNA repairment and enhanced the DNA damage of cancer cells.
Hyperactivation of DNA repairing pathway is highly associated with the chemosensitivity and chemoresistance of cancer cells. In this manuscript, guided by cascaded one strain many compounds-global natural products social molecular networking (OSMAC-GNPS) strategy, a pair of epimeric environmental-induced metabolites were isolated from Aspergillus sp. EGF 15-0-3. Structurally, sterpiperazines A (1) and B (2) represent the first steroid-based indole alkaloids with unprecedented backbones. Biologically, compound 1 could be identified as a novel tyrosyl-DNA phosphodiesterase 1 (Tdp1) inhibitor with a unique mechanism distinct from the reported modulators, and was able to significantly enhance the sensitivity of NCI-H460 cells to the clinic chemotherapeutic drug through inhibiting the DNA repairment and enhanced the DNA damage of cancer cells.
2026, 37(2): 111055
doi: 10.1016/j.cclet.2025.111055
Abstract:
Novel antibacterial strategies such as antibacterial photodynamic therapy (aPDT) and photothermal therapy (PTT) have gained significant attention, however, relying on a single-treatment approach still faces challenges of insufficient therapeutic efficiency and the potential for drug resistance. In this study, a multimodal synergistic antibacterial nanoplatform by coupling a carbon monoxide (CO) donor (4-(3-hydroxy-4-oxo-4H-chromen-2-yl)benzoic acid (4-BA)) with carbon dots (CDs) is developed, referred to as CDs-CO, which integrates multiple antibacterial modes of aPDT, PTT, and gas therapy. This nanoplatform is designed for highly efficient antibacterial action with a low risk of inducing drug resistance. CDs are engineered to possess tailored functions, including deep-red light-triggered heat and singlet oxygen (1O2) production. After modification with 4-BA and exposure to 660 nm laser irradiation, CDs-CO exhibits favorable photothermal conversion efficiency (η = 52.7%), robust 1O2 generation, and 1O2-activated CO release. Antibacterial experiments demonstrated the excellent sterilization effects of CDs-CO against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), underscoring the enhanced antibacterial efficiency of this multimodal nanoplatform. This study offers a rational approach for designing multimodal synergistic antibacterial platforms, highlighting their potential for effectively treating bacterial infections.
Novel antibacterial strategies such as antibacterial photodynamic therapy (aPDT) and photothermal therapy (PTT) have gained significant attention, however, relying on a single-treatment approach still faces challenges of insufficient therapeutic efficiency and the potential for drug resistance. In this study, a multimodal synergistic antibacterial nanoplatform by coupling a carbon monoxide (CO) donor (4-(3-hydroxy-4-oxo-4H-chromen-2-yl)benzoic acid (4-BA)) with carbon dots (CDs) is developed, referred to as CDs-CO, which integrates multiple antibacterial modes of aPDT, PTT, and gas therapy. This nanoplatform is designed for highly efficient antibacterial action with a low risk of inducing drug resistance. CDs are engineered to possess tailored functions, including deep-red light-triggered heat and singlet oxygen (1O2) production. After modification with 4-BA and exposure to 660 nm laser irradiation, CDs-CO exhibits favorable photothermal conversion efficiency (η = 52.7%), robust 1O2 generation, and 1O2-activated CO release. Antibacterial experiments demonstrated the excellent sterilization effects of CDs-CO against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), underscoring the enhanced antibacterial efficiency of this multimodal nanoplatform. This study offers a rational approach for designing multimodal synergistic antibacterial platforms, highlighting their potential for effectively treating bacterial infections.
Mechanical force-induced switchable multiple-color and white-light circularly polarized luminescence
2026, 37(2): 111060
doi: 10.1016/j.cclet.2025.111060
Abstract:
Achieving rational control over polarization states and color of circularly polarized luminescence (CPL) through simple modulation poses a challenging yet highly practical problem. To address this issue, we developed a mechano-responsive chiral supramolecular system based on a cyclohexanediamide-derived gelator CCPy. This molecule exhibited a strong blue fluorescence accompanied by a distinct CPL signal upon forming a supramolecular gel in toluene. However, upon the application of mechanical force, the gel rapidly transformed into a faintly emissive suspension with a silent CPL signal, along with a notable morphological alteration. Furthermore, by implementing the circularly polarized Förster resonance energy transfer (CP-FRET) strategy, the mechano-responsiveness was effectively imparted to binary systems through the incorporation of dyes Nile red (NR) and coumarin 7 (C7), thus realizing mechanical force-switchable green and red CPL systems. It was particularly noteworthy that by adjusting the ratio of CCPy, C7 and NR, a ternary mechanical force-induced CPL ON-OFF switch that emitted a standard white emission was achieved through sequential CP-FRET. Following this, an information encryption experiment was performed. This work provided a paradigm for fabricating smart multi-color and white-light CPL materials.
Achieving rational control over polarization states and color of circularly polarized luminescence (CPL) through simple modulation poses a challenging yet highly practical problem. To address this issue, we developed a mechano-responsive chiral supramolecular system based on a cyclohexanediamide-derived gelator CCPy. This molecule exhibited a strong blue fluorescence accompanied by a distinct CPL signal upon forming a supramolecular gel in toluene. However, upon the application of mechanical force, the gel rapidly transformed into a faintly emissive suspension with a silent CPL signal, along with a notable morphological alteration. Furthermore, by implementing the circularly polarized Förster resonance energy transfer (CP-FRET) strategy, the mechano-responsiveness was effectively imparted to binary systems through the incorporation of dyes Nile red (NR) and coumarin 7 (C7), thus realizing mechanical force-switchable green and red CPL systems. It was particularly noteworthy that by adjusting the ratio of CCPy, C7 and NR, a ternary mechanical force-induced CPL ON-OFF switch that emitted a standard white emission was achieved through sequential CP-FRET. Following this, an information encryption experiment was performed. This work provided a paradigm for fabricating smart multi-color and white-light CPL materials.
2026, 37(2): 111097
doi: 10.1016/j.cclet.2025.111097
Abstract:
Photoreforming poly(lactic acid) (PLA) plastics into pyruvic acid (PA) coupled with hydrogen evolution is of great significance for sustainable development. However, a significant challenge lies in α-OH bond cleaving of lactic acid (LA). Herein, CdS/Bi4Ti3O12 composite is fabricated, bridged by Bi−S bonds, through in-situ growth of CdS nanoparticles on Bi4Ti3O12 nanoflowers for the successive removal of hydrogen from α-C in LA. In-situ X-ray photoelectron spectroscopy confirms the S-scheme carriers transfer route and interfacial Bi−S bond in CdS/Bi4Ti3O12. Consequently, the photo-electrons and holes with extended lifetimes and strong redox potential accumulate in the CdS conduction band and Bi4Ti3O12 valence band, respectively, as evidenced by in-situ electron spin resonance and time-resolved photoluminescence. This facilitates the generation of •OH radicals, which further participate in the successive dehydrogenation reaction of LA. Consequently, the photoreforming efficiencies of converting PLA into PA and H2 by CdS/Bi4Ti3O12 are 1.7 and 3.16 mmol g–1 h–1, which are respectively 2.8 and 22 times higher than that by pristine Bi4Ti3O12. The present work provides a new approach for designing S-scheme to achieve hydrogen production and value-added conversion of plastics.
Photoreforming poly(lactic acid) (PLA) plastics into pyruvic acid (PA) coupled with hydrogen evolution is of great significance for sustainable development. However, a significant challenge lies in α-OH bond cleaving of lactic acid (LA). Herein, CdS/Bi4Ti3O12 composite is fabricated, bridged by Bi−S bonds, through in-situ growth of CdS nanoparticles on Bi4Ti3O12 nanoflowers for the successive removal of hydrogen from α-C in LA. In-situ X-ray photoelectron spectroscopy confirms the S-scheme carriers transfer route and interfacial Bi−S bond in CdS/Bi4Ti3O12. Consequently, the photo-electrons and holes with extended lifetimes and strong redox potential accumulate in the CdS conduction band and Bi4Ti3O12 valence band, respectively, as evidenced by in-situ electron spin resonance and time-resolved photoluminescence. This facilitates the generation of •OH radicals, which further participate in the successive dehydrogenation reaction of LA. Consequently, the photoreforming efficiencies of converting PLA into PA and H2 by CdS/Bi4Ti3O12 are 1.7 and 3.16 mmol g–1 h–1, which are respectively 2.8 and 22 times higher than that by pristine Bi4Ti3O12. The present work provides a new approach for designing S-scheme to achieve hydrogen production and value-added conversion of plastics.
2026, 37(2): 111109
doi: 10.1016/j.cclet.2025.111109
Abstract:
The implementation of multiple pathogen testing is essential for a rapid response to future outbreaks and for reducing disease transmission. This study introduces a 96-channel microfluidic chip, fabricated through a molding process, which enables the batch detection of pathogens. It explores the rapid lysis and elution processes of pathogens within the microfluidic chips to ensure that nucleic acid extraction, elution, and amplification are completed entirely within the chip. This chip can extract nucleic acids from samples in just 10 min, achieving an extraction efficiency comparable to that of traditional in-tube methods. An oil phase is pre-loaded into the chip to effectively prevent aerosol contamination. This approach allows for the simultaneous detection of 21 common respiratory pathogens, with a detection limit of 10 copies per reaction. Furthermore, applications involving clinical samples demonstrate significant practicality. Compared to many traditional in-tube pathogen detection methods and molecular biology technologies that utilize microfluidic chips, this detection chip not only enables simultaneous detection of multiple pathogens but also demonstrates high sensitivity.
The implementation of multiple pathogen testing is essential for a rapid response to future outbreaks and for reducing disease transmission. This study introduces a 96-channel microfluidic chip, fabricated through a molding process, which enables the batch detection of pathogens. It explores the rapid lysis and elution processes of pathogens within the microfluidic chips to ensure that nucleic acid extraction, elution, and amplification are completed entirely within the chip. This chip can extract nucleic acids from samples in just 10 min, achieving an extraction efficiency comparable to that of traditional in-tube methods. An oil phase is pre-loaded into the chip to effectively prevent aerosol contamination. This approach allows for the simultaneous detection of 21 common respiratory pathogens, with a detection limit of 10 copies per reaction. Furthermore, applications involving clinical samples demonstrate significant practicality. Compared to many traditional in-tube pathogen detection methods and molecular biology technologies that utilize microfluidic chips, this detection chip not only enables simultaneous detection of multiple pathogens but also demonstrates high sensitivity.
2026, 37(2): 111117
doi: 10.1016/j.cclet.2025.111117
Abstract:
Constructing nanofibers with specific therapeutic effects against cancer is a challenge. Here, we present the synthesis approach and application prospects of supramolecular nanofibers, which are based on cucurbit[8]uril (CB[8]) as the host and terpyridine lanthanum ions metal complex as the guest, constructed by layer-by-layer self-assembly through supramolecular interaction. Moreover, nanofibers with lanthanide luminescence properties exhibit surprising pH-responsive deformation properties and antibacterial behavior. In the tumor micro-environment, the dramatic reduction in the size of the nanofibers enables specific and hierarchical release of anticancer drugs in tumor cells to exert an advanced therapeutic effect. In addition, the synergistic therapeutic efficacy was achieved by reducing the excess of Gram-positive and Gram-negative bacteria surrounding tumor cells. The novel supramolecular nanofibers with sequential drug release and combined therapeutic mode provide new guidance for the synthesis of drug carrier materials and direction for the promotion of nanomaterial-mediated cancer therapy.
Constructing nanofibers with specific therapeutic effects against cancer is a challenge. Here, we present the synthesis approach and application prospects of supramolecular nanofibers, which are based on cucurbit[8]uril (CB[8]) as the host and terpyridine lanthanum ions metal complex as the guest, constructed by layer-by-layer self-assembly through supramolecular interaction. Moreover, nanofibers with lanthanide luminescence properties exhibit surprising pH-responsive deformation properties and antibacterial behavior. In the tumor micro-environment, the dramatic reduction in the size of the nanofibers enables specific and hierarchical release of anticancer drugs in tumor cells to exert an advanced therapeutic effect. In addition, the synergistic therapeutic efficacy was achieved by reducing the excess of Gram-positive and Gram-negative bacteria surrounding tumor cells. The novel supramolecular nanofibers with sequential drug release and combined therapeutic mode provide new guidance for the synthesis of drug carrier materials and direction for the promotion of nanomaterial-mediated cancer therapy.
2026, 37(2): 111121
doi: 10.1016/j.cclet.2025.111121
Abstract:
Asplactones A–E (1–5), five unique diphenyl ether hybrids, along with two rare spiro-diphenyl ethers, aspviolaceols A (6) and B (7), were isolated and characterized from Aspergillus sp. F1–8A, an endophytic fungus associated with the parotoid glands of Bufo gargarizans Cantor. Compounds 1–5 represent the first examples of diphenyl ether hybrids fused with unusual moieties, including conjugated γ-butyrolactone and cyclopentenone. Compounds 6 and 7 are the first known natural spiro-diphenyl ethers, with 6 featuring an uncommon 6/6/6/6-membered carbon skeleton, and 7 possessing a distinct 6/6/6/6/6/6-membered diphenyl ether spiro-heterodimer carbon framework. Structural elucidation was performed using a combination of spectroscopic techniques, X-ray crystallography, and quantum-chemical calculations, and plausible biosynthetic pathways were proposed. Biologically, compounds 1, 2, 4, 6, and 7 exhibited antioxidant activity comparable to or surpassing that of vitamin C in 1,1-diphenyl-2-picrylhydrazyl (DPPH) and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS), and ferric reducing power assays. They also significantly improved cell viability in H2O2-induced oxidative injury assays using A549 cells.
Asplactones A–E (1–5), five unique diphenyl ether hybrids, along with two rare spiro-diphenyl ethers, aspviolaceols A (6) and B (7), were isolated and characterized from Aspergillus sp. F1–8A, an endophytic fungus associated with the parotoid glands of Bufo gargarizans Cantor. Compounds 1–5 represent the first examples of diphenyl ether hybrids fused with unusual moieties, including conjugated γ-butyrolactone and cyclopentenone. Compounds 6 and 7 are the first known natural spiro-diphenyl ethers, with 6 featuring an uncommon 6/6/6/6-membered carbon skeleton, and 7 possessing a distinct 6/6/6/6/6/6-membered diphenyl ether spiro-heterodimer carbon framework. Structural elucidation was performed using a combination of spectroscopic techniques, X-ray crystallography, and quantum-chemical calculations, and plausible biosynthetic pathways were proposed. Biologically, compounds 1, 2, 4, 6, and 7 exhibited antioxidant activity comparable to or surpassing that of vitamin C in 1,1-diphenyl-2-picrylhydrazyl (DPPH) and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS), and ferric reducing power assays. They also significantly improved cell viability in H2O2-induced oxidative injury assays using A549 cells.
2026, 37(2): 111136
doi: 10.1016/j.cclet.2025.111136
Abstract:
Successfully generating reactive oxygen species (ROS) in a targeted and efficient manner for the detoxification of chlorinated organic pollutants (CPs) is a significant and demanding challenge. Herein, we present an in-situ photoreduction strategy to fabricate a composite of palladium (Pd) nanoparticles anchored few-layer carbon nitride nanosheets (Pd-CN). This innovative Pd-CN is then leveraged to activate peroxymonosulfate (PMS) in pursuit of our objective. The incorporation of Pd nanoparticles enhances PMS absorption and targets its terminal oxygen, thereby aiding in the cleavage of the O-O bond. This process generates crucial intermediates, including adsorbed hydroxyl radicals (*OH) and adsorbed atomic oxygen (O*), which are essential for the production of 1O2. Consequently, the Pd-CN catalyst demonstrates strong preference for 1O2 generation during the PMS activation process, successfully degrading over 95% of pollutants such as 4-chlorophenol (4-CP), 2,4-dichlorophenol (2,4-DCP), and 2,4,6-trichlorophenol (2,4,6-TCP) within just 20 min. Additionally, the catalyst exhibits total organic carbon (TOC) removal rates ranging from 49.4% to 31.4%, while the rates for de-chlorination fall between 68.6% and 72.7%. A subsequent continuous-flow treatment experiment has confirmed the application potential of this system, demonstrating consistent catalytic activity for up to 8 h. This promising technique presents an efficient strategy for addressing the high toxicity of chlorinated organic pollutants in contaminated water.
Successfully generating reactive oxygen species (ROS) in a targeted and efficient manner for the detoxification of chlorinated organic pollutants (CPs) is a significant and demanding challenge. Herein, we present an in-situ photoreduction strategy to fabricate a composite of palladium (Pd) nanoparticles anchored few-layer carbon nitride nanosheets (Pd-CN). This innovative Pd-CN is then leveraged to activate peroxymonosulfate (PMS) in pursuit of our objective. The incorporation of Pd nanoparticles enhances PMS absorption and targets its terminal oxygen, thereby aiding in the cleavage of the O-O bond. This process generates crucial intermediates, including adsorbed hydroxyl radicals (*OH) and adsorbed atomic oxygen (O*), which are essential for the production of 1O2. Consequently, the Pd-CN catalyst demonstrates strong preference for 1O2 generation during the PMS activation process, successfully degrading over 95% of pollutants such as 4-chlorophenol (4-CP), 2,4-dichlorophenol (2,4-DCP), and 2,4,6-trichlorophenol (2,4,6-TCP) within just 20 min. Additionally, the catalyst exhibits total organic carbon (TOC) removal rates ranging from 49.4% to 31.4%, while the rates for de-chlorination fall between 68.6% and 72.7%. A subsequent continuous-flow treatment experiment has confirmed the application potential of this system, demonstrating consistent catalytic activity for up to 8 h. This promising technique presents an efficient strategy for addressing the high toxicity of chlorinated organic pollutants in contaminated water.
2026, 37(2): 111148
doi: 10.1016/j.cclet.2025.111148
Abstract:
Chiral benzylic amines are important motifs in medicines. A dicationic nickel complex of chiral diphosphine (R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source. The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of (S)-rivastigmine. Building on this success, we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal, nickel.
Chiral benzylic amines are important motifs in medicines. A dicationic nickel complex of chiral diphosphine (R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source. The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of (S)-rivastigmine. Building on this success, we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal, nickel.
2026, 37(2): 111155
doi: 10.1016/j.cclet.2025.111155
Abstract:
Understanding the photoluminescence (PL) mechanism of metal nanoclusters from both molecular and supramolecular perspectives is crucial for developing highly emissive cluster-based nanomaterials. In this study, we synthesized two structurally similar Ag14 nanoclusters with different phosphine stabilizers, which demonstrated opposite PL behaviors in solution and crystalline states. The Ag14 nanocluster stabilized by P(Ph-OMe)3 ligands exhibited a higher PL intensity compared to the one stabilized by P(Ph-F)3 ligands, which was attributed to the stronger electron-donating ability of the P(Ph-OMe)3 ligand that improved ligand-to-metal charge transfer efficiency. In contrast, the P(Ph-F)3 stabilized Ag14 crystals displayed greater PL intensity than the Ag14 cluster crystal with a -OMe surface, which was due to stronger intermolecular interactions within the cluster lattice of the former that limited non-radiative energy loss and thus enhanced PL. Overall, this work aims to promote a comprehensive understanding of the fluorescence in cluster-based nanomaterials, which will be beneficial for their downstream applications.
Understanding the photoluminescence (PL) mechanism of metal nanoclusters from both molecular and supramolecular perspectives is crucial for developing highly emissive cluster-based nanomaterials. In this study, we synthesized two structurally similar Ag14 nanoclusters with different phosphine stabilizers, which demonstrated opposite PL behaviors in solution and crystalline states. The Ag14 nanocluster stabilized by P(Ph-OMe)3 ligands exhibited a higher PL intensity compared to the one stabilized by P(Ph-F)3 ligands, which was attributed to the stronger electron-donating ability of the P(Ph-OMe)3 ligand that improved ligand-to-metal charge transfer efficiency. In contrast, the P(Ph-F)3 stabilized Ag14 crystals displayed greater PL intensity than the Ag14 cluster crystal with a -OMe surface, which was due to stronger intermolecular interactions within the cluster lattice of the former that limited non-radiative energy loss and thus enhanced PL. Overall, this work aims to promote a comprehensive understanding of the fluorescence in cluster-based nanomaterials, which will be beneficial for their downstream applications.
2026, 37(2): 111196
doi: 10.1016/j.cclet.2025.111196
Abstract:
Sulfoxides and sulfide compounds have broad-spectrum biological properties and have received considerable attention in the past few decades. Herein we reported two metal and oxidant-free, practical and efficient methods for the synthesis of highly synthetically useful and structurally diverse ortho-aminoaryl sulfoxides and 3,4,5-trisubstituted oxazolones from readily accessible N-arylhydroxylamines and N-thiophthalimides. This rapid transformation occurred smoothly to achieve chemo- and regioselective cascade rearrangements due to the differences of the protecting-groups of the nitrogen atom of N-arylhydroxyamines. DFT studies suggested that the competing S-O and S-C bond formations via SN2 nucleophilic substitution are crucial for the observed protecting-group-dependent chemoselectivity. Subsequent applications have shown that these two protocols might be powerful tools for the construction of sulfur-containing complex molecules under simple conditions.
Sulfoxides and sulfide compounds have broad-spectrum biological properties and have received considerable attention in the past few decades. Herein we reported two metal and oxidant-free, practical and efficient methods for the synthesis of highly synthetically useful and structurally diverse ortho-aminoaryl sulfoxides and 3,4,5-trisubstituted oxazolones from readily accessible N-arylhydroxylamines and N-thiophthalimides. This rapid transformation occurred smoothly to achieve chemo- and regioselective cascade rearrangements due to the differences of the protecting-groups of the nitrogen atom of N-arylhydroxyamines. DFT studies suggested that the competing S-O and S-C bond formations via SN2 nucleophilic substitution are crucial for the observed protecting-group-dependent chemoselectivity. Subsequent applications have shown that these two protocols might be powerful tools for the construction of sulfur-containing complex molecules under simple conditions.
2026, 37(2): 111203
doi: 10.1016/j.cclet.2025.111203
Abstract:
Freshwater scarcity is exacerbated by uneven distribution of limited freshwater resources and high energy costs of desalination technologies. Atmospheric water vapor, a vast and geographically unrestricted reservoir, could become a sustainable alternative. Sorption-based atmospheric water harvesting (SAWH) has emerged as an available solution, yet conventional desorption methods relying on energy-intensive electrical heating hinder its scalability. Herein, a photothermal hygroscopic sponge has been developed for solar-driven atmospheric water harvesting. The composites combine a malleable melamine sponge skeleton, lithium chloride as a hygroscopic agent, and hydrangea-like molybdenum disulfide as a photothermal component, forming a multiscale "pore-film" cross-linked structure by an eco-friendly immersion-freeze-drying method. The optimized sample achieves exceptional hygroscopic capacity (3.92 g/g at 90% RH) and freshwater production efficiency (87.77%), which is attributed to synergistic effects of porous skeleton based crosslinked structures and "pore-film" structures, and outstanding photothermal conversion efficiency of MoS2. The unique structure could stabilize LiCl to prevent leakage, increase mass transfer effectiveness of whole SWAH process, and enable flexibility for diverse applications. We carried out outdoor experiments to demonstrate a solar-driven water production rate of 4.22 L m-2 d-1 without external energy input. This work provides insights into sustainable freshwater generation and promotes green energy utilization in addressing global water scarcity.
Freshwater scarcity is exacerbated by uneven distribution of limited freshwater resources and high energy costs of desalination technologies. Atmospheric water vapor, a vast and geographically unrestricted reservoir, could become a sustainable alternative. Sorption-based atmospheric water harvesting (SAWH) has emerged as an available solution, yet conventional desorption methods relying on energy-intensive electrical heating hinder its scalability. Herein, a photothermal hygroscopic sponge has been developed for solar-driven atmospheric water harvesting. The composites combine a malleable melamine sponge skeleton, lithium chloride as a hygroscopic agent, and hydrangea-like molybdenum disulfide as a photothermal component, forming a multiscale "pore-film" cross-linked structure by an eco-friendly immersion-freeze-drying method. The optimized sample achieves exceptional hygroscopic capacity (3.92 g/g at 90% RH) and freshwater production efficiency (87.77%), which is attributed to synergistic effects of porous skeleton based crosslinked structures and "pore-film" structures, and outstanding photothermal conversion efficiency of MoS2. The unique structure could stabilize LiCl to prevent leakage, increase mass transfer effectiveness of whole SWAH process, and enable flexibility for diverse applications. We carried out outdoor experiments to demonstrate a solar-driven water production rate of 4.22 L m-2 d-1 without external energy input. This work provides insights into sustainable freshwater generation and promotes green energy utilization in addressing global water scarcity.
2026, 37(2): 111209
doi: 10.1016/j.cclet.2025.111209
Abstract:
The coexistence of emerging containments, such as antibiotic resistant bacteria (ARB), antibiotic-resistant genes (ARGs) and antibiotics, potentially influence elimination efficiencies in UV light-emitting diode (UV-LED) alone and UV-LED/H2O2 system as their complex interactions. Tetracycline (TC) degradation efficiency (kF) correlated closely with its UV molar absorbance (R2 = 0.831) in UV-LED alone system and with •OH yield (R2 = 0.999) in UV-LED/H2O2 system across studied wavelengths (265, 280 and 310 nm). The kF values for intracellular DNA (i-ARGs) also exhibited a high correlation with UV-LED wavelengths in both systems (R2 = 0.997–0.999). The coexistence of TC and ARB/ARGs resulted in a mutual inhibition of their degradation efficiencies due to competition for photons and •OH, along with the consequent reduction in intracellular ROS within ARB, with their degradation efficiencies exhibiting marked dependence on wavelength in both systems. Notably, the UV-LED/H2O2 system at 265 nm effectively achieved the simultaneous removal of TC, ARB and ARGs with minimal energy consumption, and successfully fragmented ARGs. The degradation pathway of TC was analyzed, and the biotoxicity of its degradation intermediates demonstrated the environmental friendliness and safety of UV-LED/H2O2 technology. This study elucidated the competitive interactions between antibiotics and ARB/ARGs within UV-LED/H2O2 system, providing a promising approach for their simultaneous removal while ensuring energy efficiency.
The coexistence of emerging containments, such as antibiotic resistant bacteria (ARB), antibiotic-resistant genes (ARGs) and antibiotics, potentially influence elimination efficiencies in UV light-emitting diode (UV-LED) alone and UV-LED/H2O2 system as their complex interactions. Tetracycline (TC) degradation efficiency (kF) correlated closely with its UV molar absorbance (R2 = 0.831) in UV-LED alone system and with •OH yield (R2 = 0.999) in UV-LED/H2O2 system across studied wavelengths (265, 280 and 310 nm). The kF values for intracellular DNA (i-ARGs) also exhibited a high correlation with UV-LED wavelengths in both systems (R2 = 0.997–0.999). The coexistence of TC and ARB/ARGs resulted in a mutual inhibition of their degradation efficiencies due to competition for photons and •OH, along with the consequent reduction in intracellular ROS within ARB, with their degradation efficiencies exhibiting marked dependence on wavelength in both systems. Notably, the UV-LED/H2O2 system at 265 nm effectively achieved the simultaneous removal of TC, ARB and ARGs with minimal energy consumption, and successfully fragmented ARGs. The degradation pathway of TC was analyzed, and the biotoxicity of its degradation intermediates demonstrated the environmental friendliness and safety of UV-LED/H2O2 technology. This study elucidated the competitive interactions between antibiotics and ARB/ARGs within UV-LED/H2O2 system, providing a promising approach for their simultaneous removal while ensuring energy efficiency.
2026, 37(2): 111210
doi: 10.1016/j.cclet.2025.111210
Abstract:
Hard carbon (HC) in sodium-ion batteries is searched by numerous investigations, which can offer the excellent performance of reversible Na+ insertion and extraction. The covalent heteroatom doping in HC is recently worth concentrating, which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes. However, the reported doping strategies of the modified HC have only resulted in limited improvement, especially unobvious effects on tuning porous structure. In this study, tannin extract and K2SO4 are respectively utilized as carbon source and sulfur source for the fabrication of HC, in which K2SO4 can contribute to the heteroatom doping, and the pore forming as well. The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability, achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g. Even after 500 cycles at a current density of 3 A/g, a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6% can be reserved. Compared with the initial carbon, the adsorption energy of Na+ is multifold times higher, whereas Na+ diffusion energy barriers manyfold decrease. Moreover, the full battery assembled with Na3V2(PO4)3/tannin-based HC demonstrates a stable cycling performance. This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries (SIBs), which could especially offer an explanation of Na+ storage and solid-electrolyte interface (SEI) stability to the electrochemical performance.
Hard carbon (HC) in sodium-ion batteries is searched by numerous investigations, which can offer the excellent performance of reversible Na+ insertion and extraction. The covalent heteroatom doping in HC is recently worth concentrating, which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes. However, the reported doping strategies of the modified HC have only resulted in limited improvement, especially unobvious effects on tuning porous structure. In this study, tannin extract and K2SO4 are respectively utilized as carbon source and sulfur source for the fabrication of HC, in which K2SO4 can contribute to the heteroatom doping, and the pore forming as well. The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability, achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g. Even after 500 cycles at a current density of 3 A/g, a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6% can be reserved. Compared with the initial carbon, the adsorption energy of Na+ is multifold times higher, whereas Na+ diffusion energy barriers manyfold decrease. Moreover, the full battery assembled with Na3V2(PO4)3/tannin-based HC demonstrates a stable cycling performance. This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries (SIBs), which could especially offer an explanation of Na+ storage and solid-electrolyte interface (SEI) stability to the electrochemical performance.
2026, 37(2): 111218
doi: 10.1016/j.cclet.2025.111218
Abstract:
High-sensitive quantitative determination of alpha-fetoprotein (AFP) is of crucial importance for early clinical diagnosis of cancers. Herein, an AuNPs-free electrochemical immunosensor (Ab1-Fc-COF) was prepared from a carboxylic group enriched COF by post-functionalization with detecting antibody (Ab1) and ferrocene (Fc), and used for electrochemical detection of AFP. Due to the small, homogeneous pore size of the COF, Ab1 with a big size was immobilized on the surface of the COF, while Fc with a small size was covalently modified both on the surface and in the pores of COF. The covalently immobilized Ab1 was quite stable and beneficial to specifically detect AFP biomarkers. Meanwhile, the enriched Fc molecules not only improved the conductivity of the COF, but also effectively transferred and amplified the electrochemical signal. This proposed immunosensor exhibited high sensitivity in detecting AFP with a detection limit of 0.39 pg/mL (S/N of 3:1) and a wide linear response range spanning from 1 pg/mL to 100 ng/mL when plotted against logarithmic concentrations. Furthermore, this immunosensor showed excellent selectivity, stability and reproducibility in the testing of real samples. This study presents an innovative prototype for construction of a precious metal-free, antibody-directly-immobilized, simple and stable electrochemical immunoprobe.
High-sensitive quantitative determination of alpha-fetoprotein (AFP) is of crucial importance for early clinical diagnosis of cancers. Herein, an AuNPs-free electrochemical immunosensor (Ab1-Fc-COF) was prepared from a carboxylic group enriched COF by post-functionalization with detecting antibody (Ab1) and ferrocene (Fc), and used for electrochemical detection of AFP. Due to the small, homogeneous pore size of the COF, Ab1 with a big size was immobilized on the surface of the COF, while Fc with a small size was covalently modified both on the surface and in the pores of COF. The covalently immobilized Ab1 was quite stable and beneficial to specifically detect AFP biomarkers. Meanwhile, the enriched Fc molecules not only improved the conductivity of the COF, but also effectively transferred and amplified the electrochemical signal. This proposed immunosensor exhibited high sensitivity in detecting AFP with a detection limit of 0.39 pg/mL (S/N of 3:1) and a wide linear response range spanning from 1 pg/mL to 100 ng/mL when plotted against logarithmic concentrations. Furthermore, this immunosensor showed excellent selectivity, stability and reproducibility in the testing of real samples. This study presents an innovative prototype for construction of a precious metal-free, antibody-directly-immobilized, simple and stable electrochemical immunoprobe.
2026, 37(2): 111281
doi: 10.1016/j.cclet.2025.111281
Abstract:
Plant-related organic compound (PROC) may interact with redox-active metals like iron while they are present in soil or aquatic environment, but their effects on the photoreduction of Fe(Ⅲ) remain largely unexplored. This study investigates the photochemical behavior of Fe(Ⅲ)-PROC complexes using alkaline lignin (AL), betaine hydrochloride (BH), and phytic acid (PA) as representative proxies for PROC. The reductive agent AL demonstrated the ability to directly reduce Fe(Ⅲ) to Fe(Ⅱ). In contrast, BH, being unable to form strong complexes with Fe(Ⅲ), was able to quench •OH, thereby resulting in a shift of the redox equilibrium towards Fe(Ⅱ). PA exhibited a strong binding affinity for Fe(Ⅲ), effectively inhibiting its photoreduction. Electron paramagnetic resonance (EPR) analysis, utilizing 5,5-dimethyl-1-pyrroline-N-oxide (DMPO) as a spin trap, revealed that the DMPO-OH signal detected in photolyzed Fe(Ⅲ)-PROC solutions originated from various pathways. Specifically, uncomplexed Fe(Ⅲ) in AL or BH solutions was shown to oxidize DMPO directly, leading to the formation of a false DMPO-OH adduct. The addition of ethanol to the photolyzed Fe(Ⅲ)-AL and Fe(Ⅲ)-BH systems resulted in the generation of the DMPO-CH(CH3)OH adduct, thereby confirming the presence of authentic •OH in these systems. The photolysis of the Fe(Ⅲ)-PA complex may proceed via a photodissociation mechanism, where the resulting loosely bound Fe(Ⅲ) can oxidize DMPO, followed by a nucleophilic attack from water. This research highlights the multifaceted roles of PROC in facilitating the redox cycling of iron within soil and aquatic ecosystems.
Plant-related organic compound (PROC) may interact with redox-active metals like iron while they are present in soil or aquatic environment, but their effects on the photoreduction of Fe(Ⅲ) remain largely unexplored. This study investigates the photochemical behavior of Fe(Ⅲ)-PROC complexes using alkaline lignin (AL), betaine hydrochloride (BH), and phytic acid (PA) as representative proxies for PROC. The reductive agent AL demonstrated the ability to directly reduce Fe(Ⅲ) to Fe(Ⅱ). In contrast, BH, being unable to form strong complexes with Fe(Ⅲ), was able to quench •OH, thereby resulting in a shift of the redox equilibrium towards Fe(Ⅱ). PA exhibited a strong binding affinity for Fe(Ⅲ), effectively inhibiting its photoreduction. Electron paramagnetic resonance (EPR) analysis, utilizing 5,5-dimethyl-1-pyrroline-N-oxide (DMPO) as a spin trap, revealed that the DMPO-OH signal detected in photolyzed Fe(Ⅲ)-PROC solutions originated from various pathways. Specifically, uncomplexed Fe(Ⅲ) in AL or BH solutions was shown to oxidize DMPO directly, leading to the formation of a false DMPO-OH adduct. The addition of ethanol to the photolyzed Fe(Ⅲ)-AL and Fe(Ⅲ)-BH systems resulted in the generation of the DMPO-CH(CH3)OH adduct, thereby confirming the presence of authentic •OH in these systems. The photolysis of the Fe(Ⅲ)-PA complex may proceed via a photodissociation mechanism, where the resulting loosely bound Fe(Ⅲ) can oxidize DMPO, followed by a nucleophilic attack from water. This research highlights the multifaceted roles of PROC in facilitating the redox cycling of iron within soil and aquatic ecosystems.
2026, 37(2): 111289
doi: 10.1016/j.cclet.2025.111289
Abstract:
In the pharmaceutical field, machine learning can play an important role in drug development, production and treatment. Co-crystallization techniques have shown promising potential to enhance the properties of active pharmaceutical ingredients (APIs) such as solubility, permeability, and bioavailability, all without altering their chemical structure. This approach opens new avenues for developing natural products into effective drugs, especially those previously challenging in formulation. Emodin, an anthraquinone-based natural product, is a notable example due to its diverse biological activities; however, its physicochemical limitations, such as poor solubility and easy sublimation, restricted its clinical application. While various methods have improved emodin's physicochemical properties, research on its bioavailability remains limited. In our study, we summarize cocrystals and salts produced through co-crystallization technology and identify piperazine as a favorable coformer. Conflicting conclusions from computational chemistry and molecular modeling method and machine learning method regarding the formation of an emodin-piperazine cocrystal or salt led us to experimentally validate these possibilities. Ultimately, we successfully obtained the emodin-piperazine cocrystal, which were characterized and evaluated by several in vitro methods and pharmacokinetic studies. In addition, experiments have shown that emodin has a certain therapeutic effect on sepsis, so we also evaluated emodin-piperazine biological activity in a sepsis model. The results demonstrate that co-crystallization significantly enhances emodin's solubility, permeability, and bioavailability. Pharmacodynamic studies indicate that the emodin-piperazine cocrystal improves sepsis symptoms and provides protective effects against liver and kidney damage associated with sepsis. This study offers renewed hope for natural products with broad biological activities yet hindered by physicochemical limitations by advancing co-crystallization as a viable development approach.
In the pharmaceutical field, machine learning can play an important role in drug development, production and treatment. Co-crystallization techniques have shown promising potential to enhance the properties of active pharmaceutical ingredients (APIs) such as solubility, permeability, and bioavailability, all without altering their chemical structure. This approach opens new avenues for developing natural products into effective drugs, especially those previously challenging in formulation. Emodin, an anthraquinone-based natural product, is a notable example due to its diverse biological activities; however, its physicochemical limitations, such as poor solubility and easy sublimation, restricted its clinical application. While various methods have improved emodin's physicochemical properties, research on its bioavailability remains limited. In our study, we summarize cocrystals and salts produced through co-crystallization technology and identify piperazine as a favorable coformer. Conflicting conclusions from computational chemistry and molecular modeling method and machine learning method regarding the formation of an emodin-piperazine cocrystal or salt led us to experimentally validate these possibilities. Ultimately, we successfully obtained the emodin-piperazine cocrystal, which were characterized and evaluated by several in vitro methods and pharmacokinetic studies. In addition, experiments have shown that emodin has a certain therapeutic effect on sepsis, so we also evaluated emodin-piperazine biological activity in a sepsis model. The results demonstrate that co-crystallization significantly enhances emodin's solubility, permeability, and bioavailability. Pharmacodynamic studies indicate that the emodin-piperazine cocrystal improves sepsis symptoms and provides protective effects against liver and kidney damage associated with sepsis. This study offers renewed hope for natural products with broad biological activities yet hindered by physicochemical limitations by advancing co-crystallization as a viable development approach.
2026, 37(2): 111301
doi: 10.1016/j.cclet.2025.111301
Abstract:
Nowadays, higher requirements are put forward to the storage and utilization of energy, and supercapacitor is a kind of energy storage electronic devices. The resulting CA-N, with a specific surface area of 320.6 m2/g and a pore volume of 0.28 cm3/g, demonstrated a remarkable supercapacitance of 283.3 F/g. As a mesoporous material, CA-N offers numerous channels for the diffusion and absorption of electrolyte ions. Furthermore, it exhibited an impressive capacity retention rate of 98.48% after 5000 charge-discharge cycles. These outstanding electrochemical properties highlight the potential of CA-N for applications in energy storage.
Nowadays, higher requirements are put forward to the storage and utilization of energy, and supercapacitor is a kind of energy storage electronic devices. The resulting CA-N, with a specific surface area of 320.6 m2/g and a pore volume of 0.28 cm3/g, demonstrated a remarkable supercapacitance of 283.3 F/g. As a mesoporous material, CA-N offers numerous channels for the diffusion and absorption of electrolyte ions. Furthermore, it exhibited an impressive capacity retention rate of 98.48% after 5000 charge-discharge cycles. These outstanding electrochemical properties highlight the potential of CA-N for applications in energy storage.
2026, 37(2): 111306
doi: 10.1016/j.cclet.2025.111306
Abstract:
Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar. In this paper, a K2FeO4-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar (MHC) for Fenton-like degradation of tetracycline in aqueous solution. Diverse shapes of Fe3O4 and nano zero-valent iron (nZVI) were doped with abundant oxygen containing groups and persistent free radicals (PFRs). Multiple catalysis sites including iron species, PFRs, oxygen containing groups, and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect. Notably, MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L, with a total organic carbon (TOC) removal rate of 35%. Furthermore, after four cycles of reuse, the degradation efficiency slightly decreased to 93%. This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.
Oxidative magnetization has attracted great attention as an efficient strategy for modulating physiochemical properties of magnetic biochar. In this paper, a K2FeO4-involving hydrothermal oxidative magnetization was explored to regulate multiple micro-structures for manufacture magnetic hydrochar (MHC) for Fenton-like degradation of tetracycline in aqueous solution. Diverse shapes of Fe3O4 and nano zero-valent iron (nZVI) were doped with abundant oxygen containing groups and persistent free radicals (PFRs). Multiple catalysis sites including iron species, PFRs, oxygen containing groups, and graphite defects contributed to accelerate the Fenton-like degradation with synergistic effect. Notably, MHC achieved a tetracycline removal rate of 99% within 60 min at 50 mg/L, with a total organic carbon (TOC) removal rate of 35%. Furthermore, after four cycles of reuse, the degradation efficiency slightly decreased to 93%. This study highlights the potential of magnetic hydrochar with multiple catalytic sites in the effective and sustainable degradation of pollutants.
2026, 37(2): 111323
doi: 10.1016/j.cclet.2025.111323
Abstract:
Simultaneous identification and quantitative detection of phenylenediamine (PDA) isomers, including o-phenylenediamine (OPD), m-phenylenediamine (MPD), and p-phenylenediamine (PPD), are essential for environmental risk assessment and human health protection. However, current visual detection methods can only distinguish individual PDA isomers and failed to identify binary or ternary mixtures. Herein, a highly active and ultrastable peroxidase (POD)–like CoPt graphitic nanozyme was used for naked-eye identification and colorimetric/fluorescent (FL) dual-mode quantitative detection of PDA isomers. The CoPt@G nanozyme effectively catalyzed the oxidation of OPD, MPD, PPD, OPD + PPD, OPD + MPD, MPD + PPD and OPD + MPD + PPD into yellow, colorless, lilac, yellow, yellow, wine red and reddish-brown products, respectively, in the presence of H2O2. Thus, the MPD, PPD, MPD + PPD and OPD + MPD + PPD were easily identified based on the distinct color of their oxidation products, and the OPD, OPD + PPD, OPD + MPD could be further identified by the additional addition of MPD or PPD. Subsequently, CoPt@G/H2O2-, a 3,3′,5,5′-tetramethylbenzidine (TMB)/CoPt@G/H2O2-, and MPD/CoPt@G/H2O2-enabled colorimetric/FL dual-mode platforms for the quantitative detection of OPD, MPD and PPD were proposed. The experimental results illustrated that the constructed sensing platforms exhibit satisfactory sensitivity, comparable to that reported in previous studies. Finally, the evaluation of PDAs in water samples was realized, yielding satisfactory recoveries. This work expanded the application prospects of nanozymes in assessing environmental risks and protection of human security.
Simultaneous identification and quantitative detection of phenylenediamine (PDA) isomers, including o-phenylenediamine (OPD), m-phenylenediamine (MPD), and p-phenylenediamine (PPD), are essential for environmental risk assessment and human health protection. However, current visual detection methods can only distinguish individual PDA isomers and failed to identify binary or ternary mixtures. Herein, a highly active and ultrastable peroxidase (POD)–like CoPt graphitic nanozyme was used for naked-eye identification and colorimetric/fluorescent (FL) dual-mode quantitative detection of PDA isomers. The CoPt@G nanozyme effectively catalyzed the oxidation of OPD, MPD, PPD, OPD + PPD, OPD + MPD, MPD + PPD and OPD + MPD + PPD into yellow, colorless, lilac, yellow, yellow, wine red and reddish-brown products, respectively, in the presence of H2O2. Thus, the MPD, PPD, MPD + PPD and OPD + MPD + PPD were easily identified based on the distinct color of their oxidation products, and the OPD, OPD + PPD, OPD + MPD could be further identified by the additional addition of MPD or PPD. Subsequently, CoPt@G/H2O2-, a 3,3′,5,5′-tetramethylbenzidine (TMB)/CoPt@G/H2O2-, and MPD/CoPt@G/H2O2-enabled colorimetric/FL dual-mode platforms for the quantitative detection of OPD, MPD and PPD were proposed. The experimental results illustrated that the constructed sensing platforms exhibit satisfactory sensitivity, comparable to that reported in previous studies. Finally, the evaluation of PDAs in water samples was realized, yielding satisfactory recoveries. This work expanded the application prospects of nanozymes in assessing environmental risks and protection of human security.
2026, 37(2): 111333
doi: 10.1016/j.cclet.2025.111333
Abstract:
Small extracellular vesicles (sEVs) membrane protein profile (sEVpp) is a novel biomarker for cancer, and it can reveal the in-depth phenotype information. The point-of-care testing (POCT) of sEVpp holds great significance for mass screening of cancer, so the cost-effective and simple detection methods of sEVpp are urgently demanded. Herein, we constructed a paper-based multichannel sEVpp POCT device (sEVpp-PAD) enabled by functional DNA probes and metal-organic framework (MOF). The core components are aptamer/MOF-modified paper chips. The modified aptamers can immunocapture the sEV expressing corresponding proteins, while the modified MOF can provide abundant sites for aptamer-modification, reduce the nonspecific protein absorption, and act as reference for ratiometric detection. Simply powered by two syringes, the sEVpp-PAD can efficiently capture sEVs expressing corresponding protein from cell culture media and sera. Furthermore, a detection probe (DP) consisted of CD63 aptamer and G-quadruplex was developed for the colorimetric detection of captured sEVs. Utilizing this device, the sEVpp in various hepatocellular carcinoma cell culture medium and, more importantly, in human sera can be accurately determined, only with ＄2 device, ＄0.2 detection reagents and 1.8 h procedure. This simple strategy for sEVpp detection can innovatively promote the POCT and subtyping of cancer based on sEV-related liquid biopsy.
Small extracellular vesicles (sEVs) membrane protein profile (sEVpp) is a novel biomarker for cancer, and it can reveal the in-depth phenotype information. The point-of-care testing (POCT) of sEVpp holds great significance for mass screening of cancer, so the cost-effective and simple detection methods of sEVpp are urgently demanded. Herein, we constructed a paper-based multichannel sEVpp POCT device (sEVpp-PAD) enabled by functional DNA probes and metal-organic framework (MOF). The core components are aptamer/MOF-modified paper chips. The modified aptamers can immunocapture the sEV expressing corresponding proteins, while the modified MOF can provide abundant sites for aptamer-modification, reduce the nonspecific protein absorption, and act as reference for ratiometric detection. Simply powered by two syringes, the sEVpp-PAD can efficiently capture sEVs expressing corresponding protein from cell culture media and sera. Furthermore, a detection probe (DP) consisted of CD63 aptamer and G-quadruplex was developed for the colorimetric detection of captured sEVs. Utilizing this device, the sEVpp in various hepatocellular carcinoma cell culture medium and, more importantly, in human sera can be accurately determined, only with ＄2 device, ＄0.2 detection reagents and 1.8 h procedure. This simple strategy for sEVpp detection can innovatively promote the POCT and subtyping of cancer based on sEV-related liquid biopsy.
2026, 37(2): 111335
doi: 10.1016/j.cclet.2025.111335
Abstract:
Doxorubicin (DOX) is known to elicit potent antitumor immune responses through the induction of immunogenic cell death (ICD). However, its therapeutic efficacy is undermined by the adaptive upregulation of programmed cell death ligand 1 (PD-L1), which hijacked the antitumor immunity. In this study, we developed a reactive oxygen species (ROS)-responsive dihydroartemisinin (DHA) prodrug to facilitate the delivery of DOX via hydrophobic and electrostatic interactions. Upon internalization by tumor cells, the nanoparticles (NPs) preferentially accumulated in endoplasmic reticulum (ER), exacerbating ER stress and amplifying ICD to enhance tumor immunogenicity. Simultaneously, the oxidative intracellular environment trigged the degradation of NPs, releasing DHA, which downregulated PD-L1 by disrupting signal transducer and activator of transcription 3 (STAT3) phosphorylation and inactivating the nuclear factor kappa-B (NF-κB) pathway. Consequently, the effective PD-L1 blockade and robust ICD response, synergistically inhibited breast cancer progression, significantly enhancing the chemo-immunotherapy efficacy of doxorubicin.
Doxorubicin (DOX) is known to elicit potent antitumor immune responses through the induction of immunogenic cell death (ICD). However, its therapeutic efficacy is undermined by the adaptive upregulation of programmed cell death ligand 1 (PD-L1), which hijacked the antitumor immunity. In this study, we developed a reactive oxygen species (ROS)-responsive dihydroartemisinin (DHA) prodrug to facilitate the delivery of DOX via hydrophobic and electrostatic interactions. Upon internalization by tumor cells, the nanoparticles (NPs) preferentially accumulated in endoplasmic reticulum (ER), exacerbating ER stress and amplifying ICD to enhance tumor immunogenicity. Simultaneously, the oxidative intracellular environment trigged the degradation of NPs, releasing DHA, which downregulated PD-L1 by disrupting signal transducer and activator of transcription 3 (STAT3) phosphorylation and inactivating the nuclear factor kappa-B (NF-κB) pathway. Consequently, the effective PD-L1 blockade and robust ICD response, synergistically inhibited breast cancer progression, significantly enhancing the chemo-immunotherapy efficacy of doxorubicin.
2026, 37(2): 111342
doi: 10.1016/j.cclet.2025.111342
Abstract:
Raw water temperature can fluctuate significantly throughout the year, with peaks above 30 ℃ in summer and below 15 ℃ in winter. Traditional desalination systems (e.g., reverse osmosis, RO) face challenges under these varying temperature conditions. Specifically, while the RO system performs well under high temperatures, its efficiency decreases sharply at lower temperatures. Membrane capacitive deionization (MCDI) is considered as an emergent and promising technology for brackish water desalination. While plenty of studies have been devoted to investigating the impacts of raw water properties (e.g., salinity, coexisting ions, and natural organic matter) on MCDI performance, the role of water temperatures during the desalination remains under-explored. In this study, we first tested and determined the optimized MCDI operation parameters, such as the cell voltage and feedwater flow rate. Key findings showed that MCDI's salt removal efficiency remains unaffected by feedwater temperature fluctuations. However, as feedwater temperature increases from 15 ℃ to 40 ℃, the specific energy consumption for desalination slightly rises by 16.3%, and current efficiency drops by 14.1%. Compared to RO systems, the resilience of MCDI to temperature fluctuations makes it a preferable choice for brackish water treatment in areas with a large temperature difference.
Raw water temperature can fluctuate significantly throughout the year, with peaks above 30 ℃ in summer and below 15 ℃ in winter. Traditional desalination systems (e.g., reverse osmosis, RO) face challenges under these varying temperature conditions. Specifically, while the RO system performs well under high temperatures, its efficiency decreases sharply at lower temperatures. Membrane capacitive deionization (MCDI) is considered as an emergent and promising technology for brackish water desalination. While plenty of studies have been devoted to investigating the impacts of raw water properties (e.g., salinity, coexisting ions, and natural organic matter) on MCDI performance, the role of water temperatures during the desalination remains under-explored. In this study, we first tested and determined the optimized MCDI operation parameters, such as the cell voltage and feedwater flow rate. Key findings showed that MCDI's salt removal efficiency remains unaffected by feedwater temperature fluctuations. However, as feedwater temperature increases from 15 ℃ to 40 ℃, the specific energy consumption for desalination slightly rises by 16.3%, and current efficiency drops by 14.1%. Compared to RO systems, the resilience of MCDI to temperature fluctuations makes it a preferable choice for brackish water treatment in areas with a large temperature difference.
2026, 37(2): 111355
doi: 10.1016/j.cclet.2025.111355
Abstract:
Peroxymonosulfate (PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies. Advanced catalyst design is essential to this technology. Herein, a vanadium-doped LaFeO3 perovskite (LFO-V) featuring asymmetric Fe-O-V sites was rationally designed. Thanks to orbital electron interaction between Fe and V atoms, the modified electronic structure elevated electron density near the Fermi energy level while reducing the energy barrier toward effective PMS activation. This facilitated concurrent PMS reduction at the Fe sites to generate SO4•- and •OH (57.7%), and PMS oxidation at V sites to produce 1O2 (42.3%). The LFO-V/PMS system demonstrated excellent tetracycline (TC) degradation performance with a 2-fold enhancement in rate constant compared to that of pristine LFO. Further, the LFO-V maintained long-term stability, and the toxicity of degradation intermediates was evaluated through microbial metabolomics. This work establishes an effective route to regulate the PMS activation pathways through precise electronic structure modulation, advancing the rational design of advanced Fenton-like catalysts.
Peroxymonosulfate (PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies. Advanced catalyst design is essential to this technology. Herein, a vanadium-doped LaFeO3 perovskite (LFO-V) featuring asymmetric Fe-O-V sites was rationally designed. Thanks to orbital electron interaction between Fe and V atoms, the modified electronic structure elevated electron density near the Fermi energy level while reducing the energy barrier toward effective PMS activation. This facilitated concurrent PMS reduction at the Fe sites to generate SO4•- and •OH (57.7%), and PMS oxidation at V sites to produce 1O2 (42.3%). The LFO-V/PMS system demonstrated excellent tetracycline (TC) degradation performance with a 2-fold enhancement in rate constant compared to that of pristine LFO. Further, the LFO-V maintained long-term stability, and the toxicity of degradation intermediates was evaluated through microbial metabolomics. This work establishes an effective route to regulate the PMS activation pathways through precise electronic structure modulation, advancing the rational design of advanced Fenton-like catalysts.
2026, 37(2): 111357
doi: 10.1016/j.cclet.2025.111357
Abstract:
The limited redox capability of photocatalysts often leads to harmful NO2 byproduct formation during photocatalytic NO oxidation. Herein, Bi4Ti3O12 nanosheets modified with plasmonic metallic bismuth and abundant oxygen vacancies were synthesized via an in-situ reduction method. The optimized catalyst (BTOR2, with a molar ratio of 40% NaBH4 to Bi4Ti3O12) achieved a maximum NO removal efficiency of 62.3%, significantly higher than pristine Bi4Ti3O12 (40.5%) while minimizing NO2 production. The results reveal that the synergistic effects of Bi's plasmonic resonance and oxygen vacancies enhanced visible light absorption and charge separation. The density functional theory (DFT) analysis showed electrons can transfer from Bi4Ti3O12 to Bi, promoting O2 activation to •O2- radicals. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirmed that light-induced H2O adsorption was strengthened, improving •OH radical generation. These radicals promoted the selective conversion of activated NO- to NO3-, rather than NO2. This work provides valuable insights for advancing research into efficient photocatalysts for air pollution control.
The limited redox capability of photocatalysts often leads to harmful NO2 byproduct formation during photocatalytic NO oxidation. Herein, Bi4Ti3O12 nanosheets modified with plasmonic metallic bismuth and abundant oxygen vacancies were synthesized via an in-situ reduction method. The optimized catalyst (BTOR2, with a molar ratio of 40% NaBH4 to Bi4Ti3O12) achieved a maximum NO removal efficiency of 62.3%, significantly higher than pristine Bi4Ti3O12 (40.5%) while minimizing NO2 production. The results reveal that the synergistic effects of Bi's plasmonic resonance and oxygen vacancies enhanced visible light absorption and charge separation. The density functional theory (DFT) analysis showed electrons can transfer from Bi4Ti3O12 to Bi, promoting O2 activation to •O2- radicals. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirmed that light-induced H2O adsorption was strengthened, improving •OH radical generation. These radicals promoted the selective conversion of activated NO- to NO3-, rather than NO2. This work provides valuable insights for advancing research into efficient photocatalysts for air pollution control.
2026, 37(2): 111372
doi: 10.1016/j.cclet.2025.111372
Abstract:
Machine learning (ML) is recognized as a potent tool for the inverse design of environmental functional material, particularly for complex entities like biochar-based catalysts (BCs). Thus, the tailored BCs can have a distinct ability to trigger the nonradical pathway in advance oxidation processes (AOPs), promising a stable, rapid and selective degradation of persistent contaminants. However, due to the inherent "black box" nature and limitations of input features, results and conclusions derived from ML may not always be intuitively understood or comprehensively validated. To tackle this challenge, we linked the front-point interpretable analysis approaches with back-point density functional theory (DFT) calculations to form a chained learning strategy for deeper sight into the intrinsic activation mechanism of BCs in AOPs. At the front point, we conducted an easy-to-interpret meta-analysis to validate two strategies for enhancing nonradical pathways by increasing oxygen content and specific surface area (SSA), and prepared oxidized biochar (OBC500) and SSA-increased biochar (SBC900) by controlling pyrolysis conditions and modification methods. Subsequently, experimental results showed that OBC500 and SBC900 had distinct dominant degradation pathways for 1O2 generation and electron transfer, respectively. Finally, at the end point, DFT calculations revealed their active sites and degradation mechanisms. This chained learning strategy elucidates fundamental principles for BC inverse design and showcases the exceptional capacity to integrate computational techniques to accelerate catalyst inverse design.
Machine learning (ML) is recognized as a potent tool for the inverse design of environmental functional material, particularly for complex entities like biochar-based catalysts (BCs). Thus, the tailored BCs can have a distinct ability to trigger the nonradical pathway in advance oxidation processes (AOPs), promising a stable, rapid and selective degradation of persistent contaminants. However, due to the inherent "black box" nature and limitations of input features, results and conclusions derived from ML may not always be intuitively understood or comprehensively validated. To tackle this challenge, we linked the front-point interpretable analysis approaches with back-point density functional theory (DFT) calculations to form a chained learning strategy for deeper sight into the intrinsic activation mechanism of BCs in AOPs. At the front point, we conducted an easy-to-interpret meta-analysis to validate two strategies for enhancing nonradical pathways by increasing oxygen content and specific surface area (SSA), and prepared oxidized biochar (OBC500) and SSA-increased biochar (SBC900) by controlling pyrolysis conditions and modification methods. Subsequently, experimental results showed that OBC500 and SBC900 had distinct dominant degradation pathways for 1O2 generation and electron transfer, respectively. Finally, at the end point, DFT calculations revealed their active sites and degradation mechanisms. This chained learning strategy elucidates fundamental principles for BC inverse design and showcases the exceptional capacity to integrate computational techniques to accelerate catalyst inverse design.
2026, 37(2): 111373
doi: 10.1016/j.cclet.2025.111373
Abstract:
Chlorinated antibiotics pose great challenges in efficient removal, while for the first time, this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co3O4/g-C3N4 heterojunctions to improve process cost-effectiveness. The Co3O4/g-C3N4 heterojunction demonstrated an effective removal of 93.6% thiamphenicol (TAP) within 45 min, with the rate constant (0.0584 min-1) that was 2.4 and 2.8 times that of Co3O4 and g-C3N4 alone, respectively. The formation of heterojunctions facilitated electron transfer, enriched the electron density on Co3O4, and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates. The enhanced production of atomic hydrogen (H*) of Co3O4/g-C3N4, which increased by 13.6–28.2 times, contributed more to pollutant removal (64.0%), much higher than that of Co3O4 (37.3%) and g-C3N4 (6.1%). The energy barrier for H2 formation on Co3O4/g-C3N4 (0.75 eV) was higher than that on Co3O4 (-1.84 eV), supporting that it could stabilize H* and inhibit the formation of H2. The Co3O4/g-C3N4 heterojunction exhibited stable performance with less impact by pH and co-existing ions, and posed effectiveness for the dechlorination of typical chlorinated antibiotics. This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
Chlorinated antibiotics pose great challenges in efficient removal, while for the first time, this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co3O4/g-C3N4 heterojunctions to improve process cost-effectiveness. The Co3O4/g-C3N4 heterojunction demonstrated an effective removal of 93.6% thiamphenicol (TAP) within 45 min, with the rate constant (0.0584 min-1) that was 2.4 and 2.8 times that of Co3O4 and g-C3N4 alone, respectively. The formation of heterojunctions facilitated electron transfer, enriched the electron density on Co3O4, and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates. The enhanced production of atomic hydrogen (H*) of Co3O4/g-C3N4, which increased by 13.6–28.2 times, contributed more to pollutant removal (64.0%), much higher than that of Co3O4 (37.3%) and g-C3N4 (6.1%). The energy barrier for H2 formation on Co3O4/g-C3N4 (0.75 eV) was higher than that on Co3O4 (-1.84 eV), supporting that it could stabilize H* and inhibit the formation of H2. The Co3O4/g-C3N4 heterojunction exhibited stable performance with less impact by pH and co-existing ions, and posed effectiveness for the dechlorination of typical chlorinated antibiotics. This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
2026, 37(2): 111379
doi: 10.1016/j.cclet.2025.111379
Abstract:
A visible-light induced cascade sulfonation/cyclization reaction of 3-allyl-2-arylquinazolinones employing water as an environmentally friendly solvent was revealed. This transition metal-free protocol, using 9-mesityl-10-methylacridinium perchlorate as the photocatalyst, represents a masterly tactic for the synthesis of sulfonated dihydroisoquinolino[1,2-b]quinazolinones featuring mild conditions, facile operation, and broad substrate scope.
A visible-light induced cascade sulfonation/cyclization reaction of 3-allyl-2-arylquinazolinones employing water as an environmentally friendly solvent was revealed. This transition metal-free protocol, using 9-mesityl-10-methylacridinium perchlorate as the photocatalyst, represents a masterly tactic for the synthesis of sulfonated dihydroisoquinolino[1,2-b]quinazolinones featuring mild conditions, facile operation, and broad substrate scope.
2026, 37(2): 111380
doi: 10.1016/j.cclet.2025.111380
Abstract:
ADPr-ATP is a natural nucleotide with three sugar rings and five pentavalent phosphorus, and can be produced through TIR-catalyzed ADP-ribosylation reactions for plant immunity. Here, we report the first total synthesis of ADPr-ATP (1) with a total yield of 6.4% through 14 steps, featuring late-stage P(V)−N activation reaction of pyrophosphate (4) and 5′-phosphoromorpholidate (25). The protected adenosine 5′-phosphoromorpholidate (24) was prepared on the basis of a scalable to adenosine 5′′-monophosphate (2). The construction of P(V)−N bond in phosphoramidate is esteemed as a critical step as they are sufficiently stable in deprotection reactions. The chemical synthesis of ADPr-ATP can offer an appealing alternative to traditional enzymatic synthesis and fractionation methods. Furthermore, the pRib-AMP and its prodrug are also synthesized to evaluate cytotoxicity and anti-influenza activity in vitro.
ADPr-ATP is a natural nucleotide with three sugar rings and five pentavalent phosphorus, and can be produced through TIR-catalyzed ADP-ribosylation reactions for plant immunity. Here, we report the first total synthesis of ADPr-ATP (1) with a total yield of 6.4% through 14 steps, featuring late-stage P(V)−N activation reaction of pyrophosphate (4) and 5′-phosphoromorpholidate (25). The protected adenosine 5′-phosphoromorpholidate (24) was prepared on the basis of a scalable to adenosine 5′′-monophosphate (2). The construction of P(V)−N bond in phosphoramidate is esteemed as a critical step as they are sufficiently stable in deprotection reactions. The chemical synthesis of ADPr-ATP can offer an appealing alternative to traditional enzymatic synthesis and fractionation methods. Furthermore, the pRib-AMP and its prodrug are also synthesized to evaluate cytotoxicity and anti-influenza activity in vitro.
2026, 37(2): 111423
doi: 10.1016/j.cclet.2025.111423
Abstract:
Lysine-targeting reversible covalent inhibitors, particularly salicylaldehyde-based compounds such as the Food and Drug Administration (FDA)-approved drug Voxelotor, exhibit significant therapeutic potential but are limited by challenges including instability and off-target effects. To overcome these limitations in kinase inhibitor A5, we devised a pH-responsive prodrug strategy by masking its reactive aldehyde group with an acid-labile hydrazone linkage and enhancing intracellular delivery through conjugation with FK506. The optimized prodrug demonstrated robust antitumor efficacy in K562 tumor-bearing mice. Furthermore, the incorporation of the photosensitizer chlorin e6 (Ce6) led to the formation of self-assembled nanoparticles (AKNP), which not only improved physiological stability and prolonged tumor retention but also enabled light-triggered release of A5 in conjunction with photodynamic therapy (PDT). Our study thus presents a promising prodrug self-assembly strategy that combines the on-demand release of a novel lysine-targeting, reversible covalent kinase inhibitor with PDT in clinical cancer therapy.
Lysine-targeting reversible covalent inhibitors, particularly salicylaldehyde-based compounds such as the Food and Drug Administration (FDA)-approved drug Voxelotor, exhibit significant therapeutic potential but are limited by challenges including instability and off-target effects. To overcome these limitations in kinase inhibitor A5, we devised a pH-responsive prodrug strategy by masking its reactive aldehyde group with an acid-labile hydrazone linkage and enhancing intracellular delivery through conjugation with FK506. The optimized prodrug demonstrated robust antitumor efficacy in K562 tumor-bearing mice. Furthermore, the incorporation of the photosensitizer chlorin e6 (Ce6) led to the formation of self-assembled nanoparticles (AKNP), which not only improved physiological stability and prolonged tumor retention but also enabled light-triggered release of A5 in conjunction with photodynamic therapy (PDT). Our study thus presents a promising prodrug self-assembly strategy that combines the on-demand release of a novel lysine-targeting, reversible covalent kinase inhibitor with PDT in clinical cancer therapy.
2026, 37(2): 111424
doi: 10.1016/j.cclet.2025.111424
Abstract:
Light-energy-driven semiconductor catalysis offers attractive ways to address environmental and energy crises. TiO2 is the most promising catalyst for photocatalysis, but the lack of charge-carrier separation efficiency severely limits its catalytic performance. In this study, we carried out crystal phase engineering to prepare in situ Z-scheme hetero-phase homojunction of anatase-rutile and clarified the structure-performance relationship. The efficiency of sulfamerazine removal by hetero-phase homojunction TiO2 nanotube arrays in a single-compartment photocatalytic fuel cell system was improved by 1.93 times compared to conventional anatase TiO2 nanotube arrays and the degradation pathways were revealed by the Fukui function combined with HP-LCMS. The successful construction of Z-scheme hetero-phase homojunction was confirmed by Raman, X-ray diffraction (XRD), and electron spin resonance (ESR), which combined with density functional theory (DFT) calculations revealed the key role of crystal phase engineering in the construction of hetero-phase homojunction. This work provides a novel strategy for the scientific design of titanium dioxide photocatalysts.
Light-energy-driven semiconductor catalysis offers attractive ways to address environmental and energy crises. TiO2 is the most promising catalyst for photocatalysis, but the lack of charge-carrier separation efficiency severely limits its catalytic performance. In this study, we carried out crystal phase engineering to prepare in situ Z-scheme hetero-phase homojunction of anatase-rutile and clarified the structure-performance relationship. The efficiency of sulfamerazine removal by hetero-phase homojunction TiO2 nanotube arrays in a single-compartment photocatalytic fuel cell system was improved by 1.93 times compared to conventional anatase TiO2 nanotube arrays and the degradation pathways were revealed by the Fukui function combined with HP-LCMS. The successful construction of Z-scheme hetero-phase homojunction was confirmed by Raman, X-ray diffraction (XRD), and electron spin resonance (ESR), which combined with density functional theory (DFT) calculations revealed the key role of crystal phase engineering in the construction of hetero-phase homojunction. This work provides a novel strategy for the scientific design of titanium dioxide photocatalysts.
2026, 37(2): 111428
doi: 10.1016/j.cclet.2025.111428
Abstract:
The preparation of a novel nanoscale imazalil (IMZ)-based coordination polymer [Zn(HBTC)(IMZ)2]n (PDCP1) (H3BTC = 1,3,5-benzenetricarboxylic acid), and its antifungal application within a sustainable delivery system was reported. The intermolecular interactions presented in the structure, and their contributions to crystal packing were studied by Hirshfeld, Fingerprint plot and Mayer bond order. The obtained PDCP1 had a relatively high loading rate of IMZ (68.5%). PDCP1 exhibited notable antifungal activities against Colletotrichum gloeosporioides, Magnaporthe Oryzae, and Alternaria Nees strains, with EC50 values of 0.72, 0.92, and 0.56 µg/mL, respectively. The key benefits of the application of PDCP1 as a control release pesticide include high fungicide loading and offer nearly complete release, pH-responsive release, enhanced UV stability, exhibits favorable biosafety profiles. The remarkable inhibition of C. gloeosporioides growth by PDCP1 underscores a promising strategy for agrochemical material development, high loading of active ingredients and readily delivery fosters more efficient pesticides utilization in agricultural processes.
The preparation of a novel nanoscale imazalil (IMZ)-based coordination polymer [Zn(HBTC)(IMZ)2]n (PDCP1) (H3BTC = 1,3,5-benzenetricarboxylic acid), and its antifungal application within a sustainable delivery system was reported. The intermolecular interactions presented in the structure, and their contributions to crystal packing were studied by Hirshfeld, Fingerprint plot and Mayer bond order. The obtained PDCP1 had a relatively high loading rate of IMZ (68.5%). PDCP1 exhibited notable antifungal activities against Colletotrichum gloeosporioides, Magnaporthe Oryzae, and Alternaria Nees strains, with EC50 values of 0.72, 0.92, and 0.56 µg/mL, respectively. The key benefits of the application of PDCP1 as a control release pesticide include high fungicide loading and offer nearly complete release, pH-responsive release, enhanced UV stability, exhibits favorable biosafety profiles. The remarkable inhibition of C. gloeosporioides growth by PDCP1 underscores a promising strategy for agrochemical material development, high loading of active ingredients and readily delivery fosters more efficient pesticides utilization in agricultural processes.
2026, 37(2): 111434
doi: 10.1016/j.cclet.2025.111434
Abstract:
Polyethylene oxide (PEO)-based solid polymer electrolytes (SPEs) have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes. Here, we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions, which self-assemble into flower-like spherulites with radially aligned lamellar crystals. This unique structure creates continuous Li+ transport highways through densely packed crystalline domains, achieving a record-high ionic conductivity of 1.70 × 10–4 S/cm at 25 ℃ for pristine PEO-based systems. Strategic incorporation of lithium montmorillonite (MMTli, 10 wt%) further optimizes the composite electrolyte, balancing high ionic conductivity (1.47 × 10–4 S/cm) with enhanced electrochemical stability (4.99 V vs. Li+/Li), elevated Li+ transference number (0.62), and mechanical robustness. The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO4||Li solid-state batteries with 82% capacity retention after 200 cycles at 0.2 C under ambient conditions. This work pioneers a scalable processing paradigm for crystalline polymer electrolytes, offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.
Polyethylene oxide (PEO)-based solid polymer electrolytes (SPEs) have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes. Here, we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions, which self-assemble into flower-like spherulites with radially aligned lamellar crystals. This unique structure creates continuous Li+ transport highways through densely packed crystalline domains, achieving a record-high ionic conductivity of 1.70 × 10–4 S/cm at 25 ℃ for pristine PEO-based systems. Strategic incorporation of lithium montmorillonite (MMTli, 10 wt%) further optimizes the composite electrolyte, balancing high ionic conductivity (1.47 × 10–4 S/cm) with enhanced electrochemical stability (4.99 V vs. Li+/Li), elevated Li+ transference number (0.62), and mechanical robustness. The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO4||Li solid-state batteries with 82% capacity retention after 200 cycles at 0.2 C under ambient conditions. This work pioneers a scalable processing paradigm for crystalline polymer electrolytes, offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.
2026, 37(2): 111452
doi: 10.1016/j.cclet.2025.111452
Abstract:
Albumin, owing to its high abundance and excellent biocompatibility, is widely used as a drug carrier to enhance delivery efficiency and reduce systemic toxicity. The Michael addition between albumin thiols and maleimide-functionalized prodrugs is a common in situ macromolecular prodrug strategy. However, the resulting reversible adducts are susceptible to retro-Michael reactions in vivo, leading to premature drug release and off-target effects. To address this limitation, a gemcitabine prodrug (GAB) bearing a chloroacetamide group was designed to form irreversible covalent bonds with albumin via nucleophilic substitution. A maleimide-based prodrug (GAM) was synthesized as a control. Compared to GAM, GAB showed faster and stronger albumin binding in plasma, enhanced blood circulation time, improved tumor accumulation, and superior in vivo antitumor efficacy. Moreover, GAB exhibited a better safety profile, with reduced cytotoxicity in normal tissues and no observable systemic toxicity. These advantages are attributed to the stable albumin-drug conjugate formed by GAB, which improves drug retention and targeted delivery. This study presents an effective and generalizable albumin-hitchhiking strategy for constructing irreversible prodrugs, offering a promising approach to enhance the therapeutic index of chemotherapeutic agents.
Albumin, owing to its high abundance and excellent biocompatibility, is widely used as a drug carrier to enhance delivery efficiency and reduce systemic toxicity. The Michael addition between albumin thiols and maleimide-functionalized prodrugs is a common in situ macromolecular prodrug strategy. However, the resulting reversible adducts are susceptible to retro-Michael reactions in vivo, leading to premature drug release and off-target effects. To address this limitation, a gemcitabine prodrug (GAB) bearing a chloroacetamide group was designed to form irreversible covalent bonds with albumin via nucleophilic substitution. A maleimide-based prodrug (GAM) was synthesized as a control. Compared to GAM, GAB showed faster and stronger albumin binding in plasma, enhanced blood circulation time, improved tumor accumulation, and superior in vivo antitumor efficacy. Moreover, GAB exhibited a better safety profile, with reduced cytotoxicity in normal tissues and no observable systemic toxicity. These advantages are attributed to the stable albumin-drug conjugate formed by GAB, which improves drug retention and targeted delivery. This study presents an effective and generalizable albumin-hitchhiking strategy for constructing irreversible prodrugs, offering a promising approach to enhance the therapeutic index of chemotherapeutic agents.
2026, 37(2): 111487
doi: 10.1016/j.cclet.2025.111487
Abstract:
Fluorinated motifs are prevalent in both pharmaceuticals and agrochemicals. The incorporation of fluorine-containing moieties to drug candidates has emerged as a potent strategy for lead optimization in pharmaceutical research and development. While extensive research has been devoted to constructing molecules that incorporate a trifluoromethylthio (SCF3−) group on a stereogenic carbon, the synthesis of trifluoromethylthiolated alkanes featuring a SCF3-substituted stereogenic carbon at non-activated site remains understudied. Herein, we report a Cu-catalyzed regio- and enantioselective hydroallylation of 1-trifluoromethylthiolated alkenes. Important to the process is the regio- and enantioselective Cu-H insertion to SCF3-substituted alkene to form chiral α-SCF3 alkyl copper intermediates, outcompeting unproductive insertion to the coupling partner, and eventually proceed to afford optically active homoallylic trifluoromethylthiolated products.
Fluorinated motifs are prevalent in both pharmaceuticals and agrochemicals. The incorporation of fluorine-containing moieties to drug candidates has emerged as a potent strategy for lead optimization in pharmaceutical research and development. While extensive research has been devoted to constructing molecules that incorporate a trifluoromethylthio (SCF3−) group on a stereogenic carbon, the synthesis of trifluoromethylthiolated alkanes featuring a SCF3-substituted stereogenic carbon at non-activated site remains understudied. Herein, we report a Cu-catalyzed regio- and enantioselective hydroallylation of 1-trifluoromethylthiolated alkenes. Important to the process is the regio- and enantioselective Cu-H insertion to SCF3-substituted alkene to form chiral α-SCF3 alkyl copper intermediates, outcompeting unproductive insertion to the coupling partner, and eventually proceed to afford optically active homoallylic trifluoromethylthiolated products.
2026, 37(2): 111491
doi: 10.1016/j.cclet.2025.111491
Abstract:
The formation of Zn dendrites and the occurrence of the hydrogen evolution reaction (HER) at Zn anodes represent two major obstacles that significantly impede the widespread commercialization of aqueous Zn-ion batteries. In this work, we propose sorbitan oleate (Span 80) as a novel amphiphilic electrolyte additive for 2 mol/L ZnSO4, demonstrating multifunctional performance. The unique ultra-long hydrophobic carbon chains of Span 80 effectively reduce free water molecules at the Zn anode-electrolyte interface, forming a robust hydrophobic interfacial layer that significantly suppresses HER and corrosion reactions. Simultaneously, carbon chains can enhance the desolvation effect of [Zn(H2O)6]2+, leading to improve rate performance. Additionally, the hydrophilic sorbitan groups in Span 80 selectively adsorb onto active sites of the Zn anode, promoting uniform Zn2+ deposition and suppressing dendrite growth. The optimized Zn||Zn symmetric cell exhibits outstanding cycling stability, sustaining reversible plating/stripping for 570 h at 50 mA/cm2 and the Zn||V2O5 full cell retains exceptional stability over 2000 cycles at 1 A/g. Our work presents a promising strategy for suppressing interfacial side reactions by constructing a hydrophobic protective layer through the use of ultra-long carbon chain surfactants. This approach offers new insights into enhancing the performance of aqueous Zn-ion batteries.
The formation of Zn dendrites and the occurrence of the hydrogen evolution reaction (HER) at Zn anodes represent two major obstacles that significantly impede the widespread commercialization of aqueous Zn-ion batteries. In this work, we propose sorbitan oleate (Span 80) as a novel amphiphilic electrolyte additive for 2 mol/L ZnSO4, demonstrating multifunctional performance. The unique ultra-long hydrophobic carbon chains of Span 80 effectively reduce free water molecules at the Zn anode-electrolyte interface, forming a robust hydrophobic interfacial layer that significantly suppresses HER and corrosion reactions. Simultaneously, carbon chains can enhance the desolvation effect of [Zn(H2O)6]2+, leading to improve rate performance. Additionally, the hydrophilic sorbitan groups in Span 80 selectively adsorb onto active sites of the Zn anode, promoting uniform Zn2+ deposition and suppressing dendrite growth. The optimized Zn||Zn symmetric cell exhibits outstanding cycling stability, sustaining reversible plating/stripping for 570 h at 50 mA/cm2 and the Zn||V2O5 full cell retains exceptional stability over 2000 cycles at 1 A/g. Our work presents a promising strategy for suppressing interfacial side reactions by constructing a hydrophobic protective layer through the use of ultra-long carbon chain surfactants. This approach offers new insights into enhancing the performance of aqueous Zn-ion batteries.
2026, 37(2): 111503
doi: 10.1016/j.cclet.2025.111503
Abstract:
The demand for 238Pu (nuclear battery heat source) drives the separation of its precursor, 237Np, from spent nuclear fuel (SNF). However, the co-existence of multi-valence states (Ⅳ/Ⅴ/Ⅵ) of Np and similar redox behavior with Pu(Ⅳ) hinder the effective separation of Np. N-Butyraldehyde (n-C3H7CHO) selectively reduces Np(Ⅵ) to Np(Ⅴ) without reducing Pu(Ⅳ). Herein, we examined the reduction mechanisms of Np(Ⅵ) and Pu(Ⅳ) by n-C3H7CHO using relativistic density functional theory. Based on the results of the potential energy profiles, the reductions of both Np(Ⅵ) and Pu(Ⅳ) by n-C3H7CHO are thermodynamically feasible, whereas only the former is kinetically achievable. It uncovers that n-C3H7CHO can only reduce Np(Ⅵ) to Np(Ⅴ) owing to kinetically controlled selective reduction. The analyses of spin density and bond distance indicate that the reduction nature for the first Np(Ⅵ)/Pu(Ⅳ) belongs to hydrogen atom transfer, whereas that for the second one involves outer-sphere electron transfer. Localized molecular orbitals (LMOs) analysis discloses the bonding evolution during the reduction process of Np(Ⅵ)/Pu(Ⅳ). This study elucidates the reason behind the kinetically controlled selective reduction of Np(Ⅵ)/Pu(Ⅳ) by n-C3H7CHO at the molecular level and offers in-depth perspectives on the isolation of specific metal ions from the view of kinetic control.
The demand for 238Pu (nuclear battery heat source) drives the separation of its precursor, 237Np, from spent nuclear fuel (SNF). However, the co-existence of multi-valence states (Ⅳ/Ⅴ/Ⅵ) of Np and similar redox behavior with Pu(Ⅳ) hinder the effective separation of Np. N-Butyraldehyde (n-C3H7CHO) selectively reduces Np(Ⅵ) to Np(Ⅴ) without reducing Pu(Ⅳ). Herein, we examined the reduction mechanisms of Np(Ⅵ) and Pu(Ⅳ) by n-C3H7CHO using relativistic density functional theory. Based on the results of the potential energy profiles, the reductions of both Np(Ⅵ) and Pu(Ⅳ) by n-C3H7CHO are thermodynamically feasible, whereas only the former is kinetically achievable. It uncovers that n-C3H7CHO can only reduce Np(Ⅵ) to Np(Ⅴ) owing to kinetically controlled selective reduction. The analyses of spin density and bond distance indicate that the reduction nature for the first Np(Ⅵ)/Pu(Ⅳ) belongs to hydrogen atom transfer, whereas that for the second one involves outer-sphere electron transfer. Localized molecular orbitals (LMOs) analysis discloses the bonding evolution during the reduction process of Np(Ⅵ)/Pu(Ⅳ). This study elucidates the reason behind the kinetically controlled selective reduction of Np(Ⅵ)/Pu(Ⅳ) by n-C3H7CHO at the molecular level and offers in-depth perspectives on the isolation of specific metal ions from the view of kinetic control.
2026, 37(2): 111506
doi: 10.1016/j.cclet.2025.111506
Abstract:
Hard carbon is a vital anode material for sodium-ion batteries; however, the nonuniform growth of solid electrolyte interphase (SEI) film substantially diminishes its initial coulombic efficiency (ICE) and cycle life. The chemical and morphological properties of surface highly influence the electrode/electrolyte interfacial reactions. In this study, we have tuned orbital hybridization states forming an interface enriched with sp2 hybridized carbon (sp2–C), which decreases the binding energy to solvent molecules and inhibits excessive solvent decomposition during SEI formation. Benefiting from successfully constructed inorganic-rich SEI, the ICE increased to 91% and sodium storage capacity reached 346 mAh/g. Besides, the capacity retention rate was 90.7% after 700 cycles at 1 A/g higher than pristine electrode (83.8%).
Hard carbon is a vital anode material for sodium-ion batteries; however, the nonuniform growth of solid electrolyte interphase (SEI) film substantially diminishes its initial coulombic efficiency (ICE) and cycle life. The chemical and morphological properties of surface highly influence the electrode/electrolyte interfacial reactions. In this study, we have tuned orbital hybridization states forming an interface enriched with sp2 hybridized carbon (sp2–C), which decreases the binding energy to solvent molecules and inhibits excessive solvent decomposition during SEI formation. Benefiting from successfully constructed inorganic-rich SEI, the ICE increased to 91% and sodium storage capacity reached 346 mAh/g. Besides, the capacity retention rate was 90.7% after 700 cycles at 1 A/g higher than pristine electrode (83.8%).
2026, 37(2): 111507
doi: 10.1016/j.cclet.2025.111507
Abstract:
One-dimensional (1D) organic-inorganic halide perovskites have produced significant research interest due to their unique structure and superior tunable luminescence properties. Here, we successfully achieved a unique color-tunable phenomenon of Mn-doped 1D post-perovskite (TDMP)PbBr4 (TDMP = trans-2,5-dimethylpiperazine) (TPBM-14) under high pressure. Which exhibited tunable photoluminescence (PL) emission from red to yellow orange. Meanwhile, the band gap continued to decrease below 20.0 GPa, accompanied by piezochromism, which was associated the shrinkage and distortion of inorganic, which enhances the crystal field splitting energy and reduces the energy gap of the 4T1 to 6A1 transition. The unique octahedral corner- and edge-sharing structure of (TDMP)PbBr4, the synergistic effect of Mn doping and pressure induces local lattice distortion in TPBM-14, leading to a significant enhancement of the STE emission at 8.1 GPa. Our research explores the intrinsic connection between the band structure and optical properties of TPBM-14 under high pressure and offers valuable insights for performance optimization.
One-dimensional (1D) organic-inorganic halide perovskites have produced significant research interest due to their unique structure and superior tunable luminescence properties. Here, we successfully achieved a unique color-tunable phenomenon of Mn-doped 1D post-perovskite (TDMP)PbBr4 (TDMP = trans-2,5-dimethylpiperazine) (TPBM-14) under high pressure. Which exhibited tunable photoluminescence (PL) emission from red to yellow orange. Meanwhile, the band gap continued to decrease below 20.0 GPa, accompanied by piezochromism, which was associated the shrinkage and distortion of inorganic, which enhances the crystal field splitting energy and reduces the energy gap of the 4T1 to 6A1 transition. The unique octahedral corner- and edge-sharing structure of (TDMP)PbBr4, the synergistic effect of Mn doping and pressure induces local lattice distortion in TPBM-14, leading to a significant enhancement of the STE emission at 8.1 GPa. Our research explores the intrinsic connection between the band structure and optical properties of TPBM-14 under high pressure and offers valuable insights for performance optimization.
2026, 37(2): 111607
doi: 10.1016/j.cclet.2025.111607
Abstract:
Although the combination of chemotherapy and immunotherapy can improve the treatment of breast cancer, traditional drugs are highly toxic because they do not specifically target tumors. In this study, we developed a self-driving bacteria/nanoparticle biohybrid called Bif@PDA-aPD1/DOX-Lip by attaching polydopamine (PDA) coated doxorubicin (DOX) liposomes and the immune checkpoint inhibitor anti-programmed cell death protein 1 antibody (aPD-1) to Bifidobacterium infantis (B. infantis, Bif). Using the homing abilities of bacteria, Bif@PDA-aPD1/DOX-Lip could actively accumulate in tumor tissue, releasing DOX and aPD-1 in the acidic environment to have a synergistic anti-tumor effect. Results show that the concentration of DOX in tumors of the Bif@PDA-aPD1/DOX-Lip group was 6.31 times higher than in the free DOX group. The combination of DOX and aPD-1 not only killed tumor cells but also promoted immune normalization by maturing dendritic cells (DCs), increasing M1 macrophage ratio, and enhancing infiltration of CD8+ and CD4+ T cells in tumors and spleen. Therefore, Bif@PDA-aPD1/DOX-Lip therapy significantly inhibited tumor growth and increased the average survival time of mice to over 80 days. The Bif@PDA-aPD1/DOX-Lip biomotors offer a highly effective method for enhancing chemo-immunotherapy in solid tumors.
Although the combination of chemotherapy and immunotherapy can improve the treatment of breast cancer, traditional drugs are highly toxic because they do not specifically target tumors. In this study, we developed a self-driving bacteria/nanoparticle biohybrid called Bif@PDA-aPD1/DOX-Lip by attaching polydopamine (PDA) coated doxorubicin (DOX) liposomes and the immune checkpoint inhibitor anti-programmed cell death protein 1 antibody (aPD-1) to Bifidobacterium infantis (B. infantis, Bif). Using the homing abilities of bacteria, Bif@PDA-aPD1/DOX-Lip could actively accumulate in tumor tissue, releasing DOX and aPD-1 in the acidic environment to have a synergistic anti-tumor effect. Results show that the concentration of DOX in tumors of the Bif@PDA-aPD1/DOX-Lip group was 6.31 times higher than in the free DOX group. The combination of DOX and aPD-1 not only killed tumor cells but also promoted immune normalization by maturing dendritic cells (DCs), increasing M1 macrophage ratio, and enhancing infiltration of CD8+ and CD4+ T cells in tumors and spleen. Therefore, Bif@PDA-aPD1/DOX-Lip therapy significantly inhibited tumor growth and increased the average survival time of mice to over 80 days. The Bif@PDA-aPD1/DOX-Lip biomotors offer a highly effective method for enhancing chemo-immunotherapy in solid tumors.
2026, 37(2): 111613
doi: 10.1016/j.cclet.2025.111613
Abstract:
Organic ambipolar emitting materials hold immense potential for application in integrated optoelectrical devices yet challenging to design and synthesize. Cocrystals exhibit significant superiority in designing such materials because the properties of emission and transport can be flexibly tailored through the strategic pairing of donor and acceptor units. In this study, we report a new cocrystal system, DPA-5FDPA, derived from two high-mobility emissive molecules, 2,6-diphenylanthracene (DPA) and 2,6-diperfluorophenyl anthracene (5FDPA). This cocrystal system exhibits outstanding emission and ambipolar semiconducting properties. Notably, the single-crystal field-effect transistor devices based on DPA-5FDPA achieve maximum hole and electron mobilities of 0.298 cm2 V-1 s-1 and 0.009 cm2 V-1 s-1, respectively. In comparison, the reference compound of 2-perfluorophenyl-6-phenylanthracene (5FBA) exhibits unipolar p-type transport with the hole mobility of 0.008 cm2 V-1 s-1. In addition, DPA-5FDPA exhibits excellent optical waveguide behavior with a small optical loss coefficient of 0.079 dB/µm at 508 nm, which is lower than most reported cocrystal systems. These results underscore the promise of co-crystallization as a versatile strategy for developing advanced ambipolar emissive semiconductors and provide deeper insights into the relationships among molecular structures, packing modes, intermolecular interactions, and charge-transport properties.
Organic ambipolar emitting materials hold immense potential for application in integrated optoelectrical devices yet challenging to design and synthesize. Cocrystals exhibit significant superiority in designing such materials because the properties of emission and transport can be flexibly tailored through the strategic pairing of donor and acceptor units. In this study, we report a new cocrystal system, DPA-5FDPA, derived from two high-mobility emissive molecules, 2,6-diphenylanthracene (DPA) and 2,6-diperfluorophenyl anthracene (5FDPA). This cocrystal system exhibits outstanding emission and ambipolar semiconducting properties. Notably, the single-crystal field-effect transistor devices based on DPA-5FDPA achieve maximum hole and electron mobilities of 0.298 cm2 V-1 s-1 and 0.009 cm2 V-1 s-1, respectively. In comparison, the reference compound of 2-perfluorophenyl-6-phenylanthracene (5FBA) exhibits unipolar p-type transport with the hole mobility of 0.008 cm2 V-1 s-1. In addition, DPA-5FDPA exhibits excellent optical waveguide behavior with a small optical loss coefficient of 0.079 dB/µm at 508 nm, which is lower than most reported cocrystal systems. These results underscore the promise of co-crystallization as a versatile strategy for developing advanced ambipolar emissive semiconductors and provide deeper insights into the relationships among molecular structures, packing modes, intermolecular interactions, and charge-transport properties.
2026, 37(2): 111634
doi: 10.1016/j.cclet.2025.111634
Abstract:
Improving the optoelectronic behavior and stress-deformation stability of conjugated materials is crucial for the realization of their potential applications in flexible optoelectronics. To tune the emission behavior and mechanical property of molecular crystals simultaneously via supramolecular salt strategy is rarely reported, which is very important to improve their photophysical behavior and softness for the fabrication of flexible light-emitting device. Herein, supramolecular salt approach has been successfully applied to synthesize two elastic organic fluorescent crystals (CMOH-Py-Cl and CMOH-Py-Br) derived from non-emissive and brittle pyridine-substituted coumarin derivative (CMOH-Py). Their elastic properties can be attributed to the prevalent presence of numerous weak interactions introduced by halogen atoms, which are beneficial to the absorption and release of mechanical energy. Furthermore, density functional theory (DFT) calculations demonstrated a narrowing of the HOMO–LUMO energy gaps from CMOH-Py to CMOH-Py-Cl/CMOH-Py-Br via supramolecular salt approach. Finally, the application of flexible crystal materials in the field of optical waveguides has been investigated. The transformation of crystals in terms of photophysical and mechanical properties, achieved by the supramolecular salt approach, offers novel insights into the design and construction of flexible crystalline materials, providing a new path for the development of next-generation smart materials.
Improving the optoelectronic behavior and stress-deformation stability of conjugated materials is crucial for the realization of their potential applications in flexible optoelectronics. To tune the emission behavior and mechanical property of molecular crystals simultaneously via supramolecular salt strategy is rarely reported, which is very important to improve their photophysical behavior and softness for the fabrication of flexible light-emitting device. Herein, supramolecular salt approach has been successfully applied to synthesize two elastic organic fluorescent crystals (CMOH-Py-Cl and CMOH-Py-Br) derived from non-emissive and brittle pyridine-substituted coumarin derivative (CMOH-Py). Their elastic properties can be attributed to the prevalent presence of numerous weak interactions introduced by halogen atoms, which are beneficial to the absorption and release of mechanical energy. Furthermore, density functional theory (DFT) calculations demonstrated a narrowing of the HOMO–LUMO energy gaps from CMOH-Py to CMOH-Py-Cl/CMOH-Py-Br via supramolecular salt approach. Finally, the application of flexible crystal materials in the field of optical waveguides has been investigated. The transformation of crystals in terms of photophysical and mechanical properties, achieved by the supramolecular salt approach, offers novel insights into the design and construction of flexible crystalline materials, providing a new path for the development of next-generation smart materials.
2026, 37(2): 111676
doi: 10.1016/j.cclet.2025.111676
Abstract:
Possessing excellent mechanical properties, a high-coverage slide-ring conductive gel is constructed by in situ polymerization of α-cyclodextrin (α-CD) polyrotaxane (PR) and 1-vinyl-3-ethylimidazolium bromide ([VEIM]Br) ionic liquid (IL), using 1-ethyl-3-methylimidazolium bromide ([EMIM]Br) IL as solvent. Benefiting from the compatibility of ILs and alkene-PR, the cross-linked network slide-ring gel not only maintains excellent conductivity (1.52 × 10−2 S/m), but also has effectively improved mechanical properties (513% fracture strain, 0.713 MPa fracture stress, 211 kPa elastic modulus and 1366 kJ/m3 toughness) and adhesive properties (472.3 ± 25.9 kPa). The supramolecular gel can be used as a strain sensor to efficiently monitor deformation signals in real-time at least 200 times. Especially, the slide-ring gel can self-power generated by triboelectric effect and electrostatic induction between the skin layer and the polydimethylsiloxane (PDMS) layer that encapsulates the gel, achieving reversible and durable motion sensing, which provides a convenient pathway for constructing supramolecular self-powered flexible electronic materials.
Possessing excellent mechanical properties, a high-coverage slide-ring conductive gel is constructed by in situ polymerization of α-cyclodextrin (α-CD) polyrotaxane (PR) and 1-vinyl-3-ethylimidazolium bromide ([VEIM]Br) ionic liquid (IL), using 1-ethyl-3-methylimidazolium bromide ([EMIM]Br) IL as solvent. Benefiting from the compatibility of ILs and alkene-PR, the cross-linked network slide-ring gel not only maintains excellent conductivity (1.52 × 10−2 S/m), but also has effectively improved mechanical properties (513% fracture strain, 0.713 MPa fracture stress, 211 kPa elastic modulus and 1366 kJ/m3 toughness) and adhesive properties (472.3 ± 25.9 kPa). The supramolecular gel can be used as a strain sensor to efficiently monitor deformation signals in real-time at least 200 times. Especially, the slide-ring gel can self-power generated by triboelectric effect and electrostatic induction between the skin layer and the polydimethylsiloxane (PDMS) layer that encapsulates the gel, achieving reversible and durable motion sensing, which provides a convenient pathway for constructing supramolecular self-powered flexible electronic materials.
2026, 37(2): 111677
doi: 10.1016/j.cclet.2025.111677
Abstract:
Boron (B) doping serves as a promising strategy to enhance the quantum yield, photostability and environmental robustness of graphene quantum dots (GQDs). In this study, we reported a light-driven strategy for the facile synthesis of boron-doped graphene quantum dots (B-GQDs). Specifically, under continuous stirring at room temperature, ultraviolet irradiation induces the progressive polymerization of o-phenylenediamine (o-PDA) precursors, resulting in the formation of GQDs; meanwhile, 2-hydroxyphenylboronic acid (2-HPBA), acting as the B source, participates in the polymerization reaction with o-PDA intermediates, ultimately yielding B-GQDs. This approach significantly improves the technology of preparing QDs, yielding B-GQDs with a remarkably high fluorescence quantum yield of 71.2%. Detailed investigations reveal that the abundant surface functional groups on B-GQDs facilitate hydrogen-bonding interactions with water molecules, enabling their application as fluorescent probes for the quantitative detection of water content in various organic solvents. By integrating B-GQDs, a paper-based fluorescent sensor was successfully designed, achieving ultra-portable water content detection with excellent performance (0%-100%).
Boron (B) doping serves as a promising strategy to enhance the quantum yield, photostability and environmental robustness of graphene quantum dots (GQDs). In this study, we reported a light-driven strategy for the facile synthesis of boron-doped graphene quantum dots (B-GQDs). Specifically, under continuous stirring at room temperature, ultraviolet irradiation induces the progressive polymerization of o-phenylenediamine (o-PDA) precursors, resulting in the formation of GQDs; meanwhile, 2-hydroxyphenylboronic acid (2-HPBA), acting as the B source, participates in the polymerization reaction with o-PDA intermediates, ultimately yielding B-GQDs. This approach significantly improves the technology of preparing QDs, yielding B-GQDs with a remarkably high fluorescence quantum yield of 71.2%. Detailed investigations reveal that the abundant surface functional groups on B-GQDs facilitate hydrogen-bonding interactions with water molecules, enabling their application as fluorescent probes for the quantitative detection of water content in various organic solvents. By integrating B-GQDs, a paper-based fluorescent sensor was successfully designed, achieving ultra-portable water content detection with excellent performance (0%-100%).
2026, 37(2): 111710
doi: 10.1016/j.cclet.2025.111710
Abstract:
Azobenzene-winged phenanthrolines (L1 and L2) were designed, synthesized, and fully characterized. Ligand L1 forms an in-situ cobalt complex, which has been effectively employed as a circular dichroism (CD)-active chiral sensor. The resulting ternary complex (L1–Co2+–amino alcohol) exhibits pronounced exciton-coupled circular dichroism (ECCD) signals at the characteristic azobenzene absorption bands. These signals arise from efficient chirality transfer from the chiral amino alcohol to the azobenzene chromophores, enabling the determination of the absolute configuration of chiral amino alcohols. Accordingly, the L1–Co2+ coordination system demonstrates considerably potential in chirality sensing applications. Remarkably, the induced ECCD signals are highly responsive to multiple external stimuli, including photoirradiation, solvent polarity, temperature, and redox conditions. In particular, temperature and redox changes can induce a reversible inversion of the ECCD signal, thereby establishing this system as a multifunctional, stimuli-responsive chiroptical molecular switch.
Azobenzene-winged phenanthrolines (L1 and L2) were designed, synthesized, and fully characterized. Ligand L1 forms an in-situ cobalt complex, which has been effectively employed as a circular dichroism (CD)-active chiral sensor. The resulting ternary complex (L1–Co2+–amino alcohol) exhibits pronounced exciton-coupled circular dichroism (ECCD) signals at the characteristic azobenzene absorption bands. These signals arise from efficient chirality transfer from the chiral amino alcohol to the azobenzene chromophores, enabling the determination of the absolute configuration of chiral amino alcohols. Accordingly, the L1–Co2+ coordination system demonstrates considerably potential in chirality sensing applications. Remarkably, the induced ECCD signals are highly responsive to multiple external stimuli, including photoirradiation, solvent polarity, temperature, and redox conditions. In particular, temperature and redox changes can induce a reversible inversion of the ECCD signal, thereby establishing this system as a multifunctional, stimuli-responsive chiroptical molecular switch.
2026, 37(2): 111815
doi: 10.1016/j.cclet.2025.111815
Abstract:
Polymer-electrolyte-based solid-state Li metal batteries with high-voltage Ni-rich cathodes are promising energy storage technologies owing to their favorable security and high energy densities. However, operating in wide temperature range and at high voltage is a tough challenge for them. Herein, F/N donating fluorinated-amide-based plasticizers regulated polymer electrolyte capable of enabling high-voltage Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) batteries with excellent performance in wide temperature range is developed. F/N donating fluorinated-amide-based plasticizers significantly improve ionic conductivity (1.52 mS/cm at 30 ℃), enhance oxidation stability (5.0 V vs. Li+/Li) and fabricate robust LiF/Li3N-rich electrode-electrolyte interphases, which significantly improve the interface stability of Li metal anode and NCM811 cathode. The designed polymer electrolyte is nonflammable and has excellent dimensional stability at 200 ℃. Capitalizing on these advantageous attributes, the Li||NCM811 cells show excellent cycle stability and rate capability from −20 ℃ to 60 ℃ at high voltages (~4.6 V), and under high-loading full cell condition, which display impressive capacity retention of 84.4% after 1000 cycles and ultrahigh capacity of 154.8 mAh/g at 10 C. This work provides a rational design strategy of polymer electrolytes for wide-temperature high-energy solid-state Li metal batteries.
Polymer-electrolyte-based solid-state Li metal batteries with high-voltage Ni-rich cathodes are promising energy storage technologies owing to their favorable security and high energy densities. However, operating in wide temperature range and at high voltage is a tough challenge for them. Herein, F/N donating fluorinated-amide-based plasticizers regulated polymer electrolyte capable of enabling high-voltage Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) batteries with excellent performance in wide temperature range is developed. F/N donating fluorinated-amide-based plasticizers significantly improve ionic conductivity (1.52 mS/cm at 30 ℃), enhance oxidation stability (5.0 V vs. Li+/Li) and fabricate robust LiF/Li3N-rich electrode-electrolyte interphases, which significantly improve the interface stability of Li metal anode and NCM811 cathode. The designed polymer electrolyte is nonflammable and has excellent dimensional stability at 200 ℃. Capitalizing on these advantageous attributes, the Li||NCM811 cells show excellent cycle stability and rate capability from −20 ℃ to 60 ℃ at high voltages (~4.6 V), and under high-loading full cell condition, which display impressive capacity retention of 84.4% after 1000 cycles and ultrahigh capacity of 154.8 mAh/g at 10 C. This work provides a rational design strategy of polymer electrolytes for wide-temperature high-energy solid-state Li metal batteries.
2026, 37(2): 111824
doi: 10.1016/j.cclet.2025.111824
Abstract:
Organic pollutants, a pivotal factor in water pollution, have persistently menaced the aquatic ecosystem, as well as the sustainable development of human health, economy, and society. Consequently, there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water. Here, we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions. These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants, characterized by high apparent adsorption rate constants (kobs) and maximum adsorption capacities (qmax, e). Notably, Compound NCCP-1 demonstrated a remarkable qmax, e of 459 mg/g for bisphenol A (BPA), ranking among the highest values reported for organic polymer adsorbents. In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them, primarily mediated by the hydrophobic effect. Furthermore, NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles, highlighting its potential for practical applications in water treatment.
Organic pollutants, a pivotal factor in water pollution, have persistently menaced the aquatic ecosystem, as well as the sustainable development of human health, economy, and society. Consequently, there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water. Here, we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions. These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants, characterized by high apparent adsorption rate constants (kobs) and maximum adsorption capacities (qmax, e). Notably, Compound NCCP-1 demonstrated a remarkable qmax, e of 459 mg/g for bisphenol A (BPA), ranking among the highest values reported for organic polymer adsorbents. In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them, primarily mediated by the hydrophobic effect. Furthermore, NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles, highlighting its potential for practical applications in water treatment.
2026, 37(2): 111875
doi: 10.1016/j.cclet.2025.111875
Abstract:
Pseudomonas aeruginosa is an opportunistic pathogen responsible for severe nosocomial infections. This multidrug-resistant bacterium can cause pneumonia and cystic fibrosis, both of which are associated with high morbidity and mortality rates. The lipopolysaccharide of P. aeruginosa serves as an attractive target for the development of effective glycoconjugate vaccines. In this article, we report the first chemical synthesis of the highly challenging tetrasaccharide repeating unit of the P. aeruginosa serotype O3 O-antigen using a two-directional [1+(2 + 1)] glycosylation strategy. The synthesis is particularly challenging due to the poor nucleophilicity of the axial C4 hydroxyl group of L-galactose and the steric hindrance imposed by the 3S-hydroxybutyryl (Hb) chain. Furthermore, the presence of an acetyl group at the ortho position relative to the glycosylation site on L-galactose can lead to undesirable acetyl migration. Additionally, it is noteworthy that the selective removal of a 2-naphthylmethyl ether (Nap) during the late stages of synthesis, particularly in the presence of multiple benzyl groups, can be somewhat challenging to predict. Through the careful selection of synthetic strategies, building blocks, and optimized reaction conditions, we achieved the stereoselective glycosylations, selective oxidation of primary alcohols, remarkable enhancement of acceptor activity, and efficient introduction of the 3S-Hb group. The synthetic methodology presented in this work serves as a valuable reference for the preparation of structurally related oligosaccharides. By incorporating an aminopropyl linker, the target tetrasaccharide facilitates glycan microarray preparation and in vivo immunological assessments, thereby accelerating progress toward a synthetic glycoconjugate vaccine for P. aeruginosa.
Pseudomonas aeruginosa is an opportunistic pathogen responsible for severe nosocomial infections. This multidrug-resistant bacterium can cause pneumonia and cystic fibrosis, both of which are associated with high morbidity and mortality rates. The lipopolysaccharide of P. aeruginosa serves as an attractive target for the development of effective glycoconjugate vaccines. In this article, we report the first chemical synthesis of the highly challenging tetrasaccharide repeating unit of the P. aeruginosa serotype O3 O-antigen using a two-directional [1+(2 + 1)] glycosylation strategy. The synthesis is particularly challenging due to the poor nucleophilicity of the axial C4 hydroxyl group of L-galactose and the steric hindrance imposed by the 3S-hydroxybutyryl (Hb) chain. Furthermore, the presence of an acetyl group at the ortho position relative to the glycosylation site on L-galactose can lead to undesirable acetyl migration. Additionally, it is noteworthy that the selective removal of a 2-naphthylmethyl ether (Nap) during the late stages of synthesis, particularly in the presence of multiple benzyl groups, can be somewhat challenging to predict. Through the careful selection of synthetic strategies, building blocks, and optimized reaction conditions, we achieved the stereoselective glycosylations, selective oxidation of primary alcohols, remarkable enhancement of acceptor activity, and efficient introduction of the 3S-Hb group. The synthetic methodology presented in this work serves as a valuable reference for the preparation of structurally related oligosaccharides. By incorporating an aminopropyl linker, the target tetrasaccharide facilitates glycan microarray preparation and in vivo immunological assessments, thereby accelerating progress toward a synthetic glycoconjugate vaccine for P. aeruginosa.
2026, 37(2): 111891
doi: 10.1016/j.cclet.2025.111891
Abstract:
Portable ratiometric fluorescent platforms have emerged as promising tools for multifarious detection, yet remain unexplored for point-of-care monitoring doxorubicin (DOX), one of clinically antineoplastic drugs. To this end, we herein develop a portable self-calibrating platform namely carbon dots (C-dots)-embedded hydrogel sensors with a smartphone-assisted high-throughput imaging device, for DOX sensing. The prepared green-emitting (λem = 508 nm) and negatively-charged C-dots (−11.40 ± 1.21 mV), which have sufficient spectral overlap with the absorption band of DOX (~500 nm), can strongly bind with positively-charged DOX molecules by electrostatic attraction effects. As a result, DOX molecules are selectively and rapid (20 s) determined with a detection limit of 10.26 nmol/L via Förster resonance energy transfer processes, demonstrating a remarkably chromatic shift from green to red. Further integrated with a 3D-printed smartphone-assisted device, the platform enabled high-throughput quantification, achieving recoveries of 96.40%–101.85% in human urine/serum (RSDs < 2.94%, n = 3). Notably, the dual linear detection ranges of the platform align with the reported clinical DOX concentrations in urine and plasma (0–4 h post-administration), validating their capability for direct quantification of DOX in clinical samples without special pre-treatment processes. By virtue of attractive analytical performances and robust feasibility, this platform bridges laboratory precision and point-of-care testing needs, offering promising potential for personalized chemotherapy and multiplexed analyte screening.
Portable ratiometric fluorescent platforms have emerged as promising tools for multifarious detection, yet remain unexplored for point-of-care monitoring doxorubicin (DOX), one of clinically antineoplastic drugs. To this end, we herein develop a portable self-calibrating platform namely carbon dots (C-dots)-embedded hydrogel sensors with a smartphone-assisted high-throughput imaging device, for DOX sensing. The prepared green-emitting (λem = 508 nm) and negatively-charged C-dots (−11.40 ± 1.21 mV), which have sufficient spectral overlap with the absorption band of DOX (~500 nm), can strongly bind with positively-charged DOX molecules by electrostatic attraction effects. As a result, DOX molecules are selectively and rapid (20 s) determined with a detection limit of 10.26 nmol/L via Förster resonance energy transfer processes, demonstrating a remarkably chromatic shift from green to red. Further integrated with a 3D-printed smartphone-assisted device, the platform enabled high-throughput quantification, achieving recoveries of 96.40%–101.85% in human urine/serum (RSDs < 2.94%, n = 3). Notably, the dual linear detection ranges of the platform align with the reported clinical DOX concentrations in urine and plasma (0–4 h post-administration), validating their capability for direct quantification of DOX in clinical samples without special pre-treatment processes. By virtue of attractive analytical performances and robust feasibility, this platform bridges laboratory precision and point-of-care testing needs, offering promising potential for personalized chemotherapy and multiplexed analyte screening.
2026, 37(2): 111917
doi: 10.1016/j.cclet.2025.111917
Abstract:
The hydrogen evolution reaction (HER) is crucial for hydrogen production and sustainable energy storage. Molybdenum disulfide (MoS2), a representative transition metal dichalcogenides (TMDs), shows potential as an HER catalyst but suffers from limited performance due to poor charge transfer and interfacial effects. Here, we report a salt-assisted chemical vapor deposition (CVD) method for synthesizing high-quality tungsten ditelluride (WTe2) with tunable morphologies using alkali halides (NaCl, KCl and LiCl). The prepared WTe2 nanoribbons and hexagonal nanosheets exhibit morphology-dependent electrical conductivity, with nanosheets showing superior performance. To evaluate WTe2 as a contact electrode, WTe2−MoS2 heterostructures were fabricated and compared with graphene-MoS2 counterparts. The WTe2−MoS2 heterostructure exhibits a superior Tafel slope of 111.57 mV/dec and an overpotential of 298 mV at -10 mA/cm2, significantly outperforming graphene-based electrodes. This improvement is attributed to the excellent conductivity of WTe2 and reduced interfacial Schottky barriers. Moreover, we systematically investigate the influence of WTe2 thickness on HER performance and assess the electrochemical durability and structural stability of the heterostructure, further confirming the effectiveness of WTe2 as a contact electrode for enhancing the HER activity of MoS2. This study offers a novel approach for enhancing the HER performance of MoS2 through controlled WTe2 growth and application as a contact electrode. Our findings provide valuable insights into the synthesis of high-quality WTe2 and broaden the potential applications of two-dimensional materials in energy catalysis.
The hydrogen evolution reaction (HER) is crucial for hydrogen production and sustainable energy storage. Molybdenum disulfide (MoS2), a representative transition metal dichalcogenides (TMDs), shows potential as an HER catalyst but suffers from limited performance due to poor charge transfer and interfacial effects. Here, we report a salt-assisted chemical vapor deposition (CVD) method for synthesizing high-quality tungsten ditelluride (WTe2) with tunable morphologies using alkali halides (NaCl, KCl and LiCl). The prepared WTe2 nanoribbons and hexagonal nanosheets exhibit morphology-dependent electrical conductivity, with nanosheets showing superior performance. To evaluate WTe2 as a contact electrode, WTe2−MoS2 heterostructures were fabricated and compared with graphene-MoS2 counterparts. The WTe2−MoS2 heterostructure exhibits a superior Tafel slope of 111.57 mV/dec and an overpotential of 298 mV at -10 mA/cm2, significantly outperforming graphene-based electrodes. This improvement is attributed to the excellent conductivity of WTe2 and reduced interfacial Schottky barriers. Moreover, we systematically investigate the influence of WTe2 thickness on HER performance and assess the electrochemical durability and structural stability of the heterostructure, further confirming the effectiveness of WTe2 as a contact electrode for enhancing the HER activity of MoS2. This study offers a novel approach for enhancing the HER performance of MoS2 through controlled WTe2 growth and application as a contact electrode. Our findings provide valuable insights into the synthesis of high-quality WTe2 and broaden the potential applications of two-dimensional materials in energy catalysis.
2026, 37(2): 111920
doi: 10.1016/j.cclet.2025.111920
Abstract:
Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2 to various high value-added C2 products like ethylene and alcohols. However, realizing high selectivity of C2 products are still a main challenge due to complex CO2 electroreduction pathways and small opportunity of C–C coupling reactions. Here, we found the origin of enhanced CO2 electroreduction reaction activity and product selectivity towards C2 products and C–C coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces, the corresponding CO2 electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations. The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer, especially Cl−-adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer, subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2 into C2H4 product. The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl− can enhance selectivity of C2H4 product. The determinations of onset potentials indicate that electroreduction pathways of CO2 towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity. This work on selective realization of CO2 electroreduction towards C2H4 product via Cl−-modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products.
Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2 to various high value-added C2 products like ethylene and alcohols. However, realizing high selectivity of C2 products are still a main challenge due to complex CO2 electroreduction pathways and small opportunity of C–C coupling reactions. Here, we found the origin of enhanced CO2 electroreduction reaction activity and product selectivity towards C2 products and C–C coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces, the corresponding CO2 electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations. The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer, especially Cl−-adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer, subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2 into C2H4 product. The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl− can enhance selectivity of C2H4 product. The determinations of onset potentials indicate that electroreduction pathways of CO2 towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity. This work on selective realization of CO2 electroreduction towards C2H4 product via Cl−-modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products.
2026, 37(2): 111933
doi: 10.1016/j.cclet.2025.111933
Abstract:
Charge-transfer complexes (CTCs) have emerged as promising n-type organic thermoelectric (TE) materials due to their inherent high electrical conductivity and tunable transport polarities. In this study, we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes (CnBTBT, n = 4, 8, 12) as donors and fluorinated derivatives of tetracyanoquinodimethane (FmTCNQ, m = 0, 2, 4) as acceptors, aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure–property relationships. Our calculation results, based on the Boltzmann transport equation and deformation potential theory, reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties. Notably, the CnBTBT–FmTCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics, particularly C4BTBT–F4TCNQ, which achieves an excellent power factor of 671 µW cm-1 K-2 at an optimal charge carrier concentration. Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.
Charge-transfer complexes (CTCs) have emerged as promising n-type organic thermoelectric (TE) materials due to their inherent high electrical conductivity and tunable transport polarities. In this study, we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes (CnBTBT, n = 4, 8, 12) as donors and fluorinated derivatives of tetracyanoquinodimethane (FmTCNQ, m = 0, 2, 4) as acceptors, aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure–property relationships. Our calculation results, based on the Boltzmann transport equation and deformation potential theory, reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties. Notably, the CnBTBT–FmTCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics, particularly C4BTBT–F4TCNQ, which achieves an excellent power factor of 671 µW cm-1 K-2 at an optimal charge carrier concentration. Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.
2026, 37(2): 111945
doi: 10.1016/j.cclet.2025.111945
Abstract:
We report an immobilized enzyme-catalyzed batch and continuous-flow synthesis of optically pure ethyl (R)-pantothenate ((R)-PaOEt), the direct precursor of D-pantothenic acid. Firstly, a ketoreductase mutant designated as M2, carrying two-point mutations of F97L and M242F relative to the wild-type SSCR, was constructed by site-directed mutagenesis, exhibited simultaneously improved activity toward ethyl 2′-ketopantothenate (K-PaOEt) and isopropanol, and could effectively catalyze the stereoselective reduction of K-PaOEt to (R)-PaOEt by using isopropanol as the sacrificial co-substrate to regenerate NADPH. After screening six commercially available carriers, an amino resin LXTE-700 was identified as the best solid support for the immobilization of M2 via the glutaraldehyde activation method. Upon optimization of the immobilization process and reaction conditions, the fabricated immobilized enzyme M2@amino resin demonstrated excellent recyclability and reusability, with the complete conversion of K-PaOEt to (R)-PaOEt being still realized after 12 cycles of reuse. Finally, M2@amino resin-catalyzed synthesis of (R)-PaOEt was successfully implemented in continuous-flow, accomplishing a 6.3 times higher space-time yield than that with the batch synthesis (529.2 versus 84 g L-1 d-1). Our developed flow biocatalysis system also features an outstanding operational stability, as evidenced by the 100% conversion rate achieved after 15 consecutive days of operation.
We report an immobilized enzyme-catalyzed batch and continuous-flow synthesis of optically pure ethyl (R)-pantothenate ((R)-PaOEt), the direct precursor of D-pantothenic acid. Firstly, a ketoreductase mutant designated as M2, carrying two-point mutations of F97L and M242F relative to the wild-type SSCR, was constructed by site-directed mutagenesis, exhibited simultaneously improved activity toward ethyl 2′-ketopantothenate (K-PaOEt) and isopropanol, and could effectively catalyze the stereoselective reduction of K-PaOEt to (R)-PaOEt by using isopropanol as the sacrificial co-substrate to regenerate NADPH. After screening six commercially available carriers, an amino resin LXTE-700 was identified as the best solid support for the immobilization of M2 via the glutaraldehyde activation method. Upon optimization of the immobilization process and reaction conditions, the fabricated immobilized enzyme M2@amino resin demonstrated excellent recyclability and reusability, with the complete conversion of K-PaOEt to (R)-PaOEt being still realized after 12 cycles of reuse. Finally, M2@amino resin-catalyzed synthesis of (R)-PaOEt was successfully implemented in continuous-flow, accomplishing a 6.3 times higher space-time yield than that with the batch synthesis (529.2 versus 84 g L-1 d-1). Our developed flow biocatalysis system also features an outstanding operational stability, as evidenced by the 100% conversion rate achieved after 15 consecutive days of operation.
2026, 37(2): 111946
doi: 10.1016/j.cclet.2025.111946
Abstract:
Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science. Recently, supramolecular polymeric materials (SPMs) have drawn increased attention due to their unique properties and potential applications in self-healing, shape memory, sensors, and flexible electronics. Here, we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers. The mechanical properties, including Young’s modulus and toughness, are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone (UPy) induced microphase separation with iron(Ⅲ)-to-carboxylate ionic clusters. By combining established chemical approaches with adjustable polymer phase ratios, it is revealed that the synergistic effect of these factors expands the interchain spacing, facilitates the formation of microphase domains, and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli, meeting the practical requirements for industrial plastic applications. Moreover, the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature. Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.
Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science. Recently, supramolecular polymeric materials (SPMs) have drawn increased attention due to their unique properties and potential applications in self-healing, shape memory, sensors, and flexible electronics. Here, we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers. The mechanical properties, including Young’s modulus and toughness, are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone (UPy) induced microphase separation with iron(Ⅲ)-to-carboxylate ionic clusters. By combining established chemical approaches with adjustable polymer phase ratios, it is revealed that the synergistic effect of these factors expands the interchain spacing, facilitates the formation of microphase domains, and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli, meeting the practical requirements for industrial plastic applications. Moreover, the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature. Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.
2026, 37(2): 111949
doi: 10.1016/j.cclet.2025.111949
Abstract:
As a common electronic adhesive, ultraviolet (UV) curing polyurethane acrylate adhesive has both flexibility and wear resistance of polyurethane, excellent weather resistance and optical properties of acrylate. Despite the extensive applications, it is still difficult to solve the problems caused by the shrinkage of adhesive. Here, a new type of photosensitive adhesive for bonding electronic components based on supramolecular interaction was designed and synthesized. The supramolecular interaction of cyclodextrin and adamantane moieties introduced into the adhesive polymer entitles the viscosity of the adhesive to rise rapidly during use, thereby preventing adhesive loss and dislocation of electronic components. UV light could further cure the adhesive and position the electronic components. The adhesive shrunk < 2% when cured by UV light, so it can be used for electronic packaging and high-resolution, defect-free lithography.
As a common electronic adhesive, ultraviolet (UV) curing polyurethane acrylate adhesive has both flexibility and wear resistance of polyurethane, excellent weather resistance and optical properties of acrylate. Despite the extensive applications, it is still difficult to solve the problems caused by the shrinkage of adhesive. Here, a new type of photosensitive adhesive for bonding electronic components based on supramolecular interaction was designed and synthesized. The supramolecular interaction of cyclodextrin and adamantane moieties introduced into the adhesive polymer entitles the viscosity of the adhesive to rise rapidly during use, thereby preventing adhesive loss and dislocation of electronic components. UV light could further cure the adhesive and position the electronic components. The adhesive shrunk < 2% when cured by UV light, so it can be used for electronic packaging and high-resolution, defect-free lithography.
2026, 37(2): 111959
doi: 10.1016/j.cclet.2025.111959
Abstract:
Shape memory polymers used in 4D printing only had one permanent shape after molding, which limited their applications in requiring multiple reconstructions and multifunctional shapes. Furthermore, the inherent stability of the triazine ring structure within cyanate ester (CE) crosslinked networks after molding posed significant challenges for both recycling, repairing, and degradation of resin. To address these obstacles, dynamic thiocyanate ester (TCE) bonds and photocurable group were incorporated into CE, obtaining the recyclable and 3D printable CE covalent adaptable networks (CANs), denoted as PTCE1.5. This material exhibits a Young’s modulus of 810 MPa and a tensile strength of 50.8 MPa. Notably, damaged printed PTCE1.5 objects can be readily repaired through reprinting and interface rejoining by thermal treatment. Leveraging the solid-state plasticity, PTCE1.5 also demonstrated attractive shape memory ability and permanent shape reconfigurability, enabling its reconfigurable 4D printing. The printed PTCE1.5 hinges and a main body were assembled into a deployable and retractable satellite model, validating its potential application as a controllable component in the aerospace field. Moreover, printed PTCE1.5 can be fully degraded into thiol-modified intermediate products. Overall, this material not only enriches the application range of CE resin, but also provides a reliable approach to addressing environmental issue.
Shape memory polymers used in 4D printing only had one permanent shape after molding, which limited their applications in requiring multiple reconstructions and multifunctional shapes. Furthermore, the inherent stability of the triazine ring structure within cyanate ester (CE) crosslinked networks after molding posed significant challenges for both recycling, repairing, and degradation of resin. To address these obstacles, dynamic thiocyanate ester (TCE) bonds and photocurable group were incorporated into CE, obtaining the recyclable and 3D printable CE covalent adaptable networks (CANs), denoted as PTCE1.5. This material exhibits a Young’s modulus of 810 MPa and a tensile strength of 50.8 MPa. Notably, damaged printed PTCE1.5 objects can be readily repaired through reprinting and interface rejoining by thermal treatment. Leveraging the solid-state plasticity, PTCE1.5 also demonstrated attractive shape memory ability and permanent shape reconfigurability, enabling its reconfigurable 4D printing. The printed PTCE1.5 hinges and a main body were assembled into a deployable and retractable satellite model, validating its potential application as a controllable component in the aerospace field. Moreover, printed PTCE1.5 can be fully degraded into thiol-modified intermediate products. Overall, this material not only enriches the application range of CE resin, but also provides a reliable approach to addressing environmental issue.
2026, 37(2): 111989
doi: 10.1016/j.cclet.2025.111989
Abstract:
Cyclo[n]Thiophenes (CnTs) are a distinctive class of π-conjugated macrocyclic molecules that have attracted growing attention owing to their structural aesthetics and organic electronic characteristics. However, the development of CnTs has been largely impeded by inefficient synthetic route. In this work, we employ a bridge strategy using bipyridine as bridge to link two quaterthiophene units resulting in Φ-shaped bicyclosystem. This strain-retaining approach improves the synthesis efficiency of the macrocycles. Two new macrocyclic molecules, (4T-2hexyl-2Me)2-DPBP and (4T-2hexyl)2-DPBP, were successfully synthesized in total yield 17% and 16%, respectively. Single-crystal structure of (4T-2hexyl-2Me)2-DPBP reveals that the bipyridine bridge is orthogonally strapped by two quaterthiophene units. Notably, both compounds exhibit aggregation-induced emission enhancement (AIEE) behavior-an unprecedented feature among CnT-based macrocycles. Theoretical calculations reveal that this AIE phenomenon originates from the restriction of intramolecular motion (RIM) in the aggregated state, which suppresses the non-radiative decay channels. These results demonstrate a generalized strategy for the synthesis of functional π-conjugated macrocyclic molecules based fluorescent materials.
Cyclo[n]Thiophenes (CnTs) are a distinctive class of π-conjugated macrocyclic molecules that have attracted growing attention owing to their structural aesthetics and organic electronic characteristics. However, the development of CnTs has been largely impeded by inefficient synthetic route. In this work, we employ a bridge strategy using bipyridine as bridge to link two quaterthiophene units resulting in Φ-shaped bicyclosystem. This strain-retaining approach improves the synthesis efficiency of the macrocycles. Two new macrocyclic molecules, (4T-2hexyl-2Me)2-DPBP and (4T-2hexyl)2-DPBP, were successfully synthesized in total yield 17% and 16%, respectively. Single-crystal structure of (4T-2hexyl-2Me)2-DPBP reveals that the bipyridine bridge is orthogonally strapped by two quaterthiophene units. Notably, both compounds exhibit aggregation-induced emission enhancement (AIEE) behavior-an unprecedented feature among CnT-based macrocycles. Theoretical calculations reveal that this AIE phenomenon originates from the restriction of intramolecular motion (RIM) in the aggregated state, which suppresses the non-radiative decay channels. These results demonstrate a generalized strategy for the synthesis of functional π-conjugated macrocyclic molecules based fluorescent materials.
2026, 37(2): 112022
doi: 10.1016/j.cclet.2025.112022
Abstract:
Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction (HER). Here, we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black, synthesized using the high-temperature liquid shock (HTLS) method. This approach offers significant advantages over conventional synthesis methods, including high scalability, rapid reaction rates, and precise control over the size and shape of nanocrystals. Importantly, the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER, achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm2, respectively. The superior performance can be attributed to the combination of a refined particle size, lattice strains, and synergistic effects between Pt and Ni. This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.
Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction (HER). Here, we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black, synthesized using the high-temperature liquid shock (HTLS) method. This approach offers significant advantages over conventional synthesis methods, including high scalability, rapid reaction rates, and precise control over the size and shape of nanocrystals. Importantly, the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER, achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm2, respectively. The superior performance can be attributed to the combination of a refined particle size, lattice strains, and synergistic effects between Pt and Ni. This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.
2026, 37(2): 112039
doi: 10.1016/j.cclet.2025.112039
Abstract:
Chiral amino acids (AAs) serve as essential building blocks of proteins and play vital physiological roles in living organisms. To achieve accurate, rapid, and high-throughput analysis of chiral AAs, this work proposed a methylbenzyl isocyanate (MBIC) derivatization strategy coupled with ultra-high performance liquid chromatography-mass spectrometry or trapped ion mobility spectrometry-mass spectrometry. The integration of a chiral carbon atom with a rigid urea-based structure can significantly enhance the separation of chiral MBIC-labeled AA enantiomers. This phenomenon can be attributed to the labeled l-AAs allow the carboxyl group to form intramolecular hydrogen bonds with the amino group in the rigid urea-based structure, whereas labeled d-AAs are unable to form such bonds. The method based on MBIC derivatization coupled with ultra-performance liquid chromatography-tandem mass spectrometry achieved simultaneous separation of 19 pairs of chiral AAs using only a C18 column within 30 min, enabling quantitatively detect twelve types of chiral AAs in the serum of healthy humans and Parkinson's patients. The distribution of twenty-four chiral AAs is observed in mouse brain using MBIC labeling-based matrix-assisted laser desorption/ionization-trapped ion mobility spectrometry-mass spectrometry imaging without prior separation. Our work elucidates the principles governing the separation of chiral AAs using derivatization methods, providing valuable guidance for the separation of chiral compounds.
Chiral amino acids (AAs) serve as essential building blocks of proteins and play vital physiological roles in living organisms. To achieve accurate, rapid, and high-throughput analysis of chiral AAs, this work proposed a methylbenzyl isocyanate (MBIC) derivatization strategy coupled with ultra-high performance liquid chromatography-mass spectrometry or trapped ion mobility spectrometry-mass spectrometry. The integration of a chiral carbon atom with a rigid urea-based structure can significantly enhance the separation of chiral MBIC-labeled AA enantiomers. This phenomenon can be attributed to the labeled l-AAs allow the carboxyl group to form intramolecular hydrogen bonds with the amino group in the rigid urea-based structure, whereas labeled d-AAs are unable to form such bonds. The method based on MBIC derivatization coupled with ultra-performance liquid chromatography-tandem mass spectrometry achieved simultaneous separation of 19 pairs of chiral AAs using only a C18 column within 30 min, enabling quantitatively detect twelve types of chiral AAs in the serum of healthy humans and Parkinson's patients. The distribution of twenty-four chiral AAs is observed in mouse brain using MBIC labeling-based matrix-assisted laser desorption/ionization-trapped ion mobility spectrometry-mass spectrometry imaging without prior separation. Our work elucidates the principles governing the separation of chiral AAs using derivatization methods, providing valuable guidance for the separation of chiral compounds.
2026, 37(2): 112051
doi: 10.1016/j.cclet.2025.112051
Abstract:
The structural principles of traditional Chinese mortise-and-tenon joints have inspired breakthroughs in supramolecular engineering. Nevertheless, substantial challenges remain in constructing nanoscale supramolecular architectures with precisely controlled giant dimensions. Herein, we report a precision-guided synthetic strategy for constructing giant 2D and 3D supramolecular architectures with rhomboidal motifs, which was achieved through a dovetail joint strategy. Initial assembly of bis-mortise ligand L1 with dovetail tenon ligand L2 in the presence of Cd2+ ions yielded the fundamental bis-rhombic supramolecule R1. Subsequent structural elaboration of the dovetail tenon motif enabled the development of multitopic ligands L3 and L4, which facilitated the construction of expanded architectures of the giant bis-propeller supramolecule R2 and tris-propeller supramolecule R3. The synthesized supramolecules R1–R3 were fully characterized multidimensional NMR spectroscopy, electrospray ionization mass spectrometry (ESI-MS), traveling wave ion mobility mass spectrometry (TWIM-MS), transmission electron microscopy (TEM), and atomic force microscopy (AFM). This work develops an innovative dovetail-joint assembly strategy for constructing rigid giant supramolecular architectures, establishing a new paradigm for precision engineering of complex 3D molecular systems.
The structural principles of traditional Chinese mortise-and-tenon joints have inspired breakthroughs in supramolecular engineering. Nevertheless, substantial challenges remain in constructing nanoscale supramolecular architectures with precisely controlled giant dimensions. Herein, we report a precision-guided synthetic strategy for constructing giant 2D and 3D supramolecular architectures with rhomboidal motifs, which was achieved through a dovetail joint strategy. Initial assembly of bis-mortise ligand L1 with dovetail tenon ligand L2 in the presence of Cd2+ ions yielded the fundamental bis-rhombic supramolecule R1. Subsequent structural elaboration of the dovetail tenon motif enabled the development of multitopic ligands L3 and L4, which facilitated the construction of expanded architectures of the giant bis-propeller supramolecule R2 and tris-propeller supramolecule R3. The synthesized supramolecules R1–R3 were fully characterized multidimensional NMR spectroscopy, electrospray ionization mass spectrometry (ESI-MS), traveling wave ion mobility mass spectrometry (TWIM-MS), transmission electron microscopy (TEM), and atomic force microscopy (AFM). This work develops an innovative dovetail-joint assembly strategy for constructing rigid giant supramolecular architectures, establishing a new paradigm for precision engineering of complex 3D molecular systems.
2026, 37(2): 112099
doi: 10.1016/j.cclet.2025.112099
Abstract:
PEGylation, the controlled covalent conjugation of polyethylene glycol to therapeutics, enhances therapeutic efficacy through optimized pharmacokinetics. However, to date no high-molecular-weight PEGylated small-molecule prodrugs have received regulatory approval. This technological gap can be partially attributed to the exponential proliferation of metabolic intermediates resulting from multi-payload conjugation strategies, which introduces unprecedented analytical complexities in metabolite profiling and pharmacokinetic characterization. To address this challenge, we developed a liquid chromatography-triple-quadrupole/time-of-flight mass spectrometry platform for PEG20k-(irinotecan)3, a Phase Ⅲ clinical candidate. Our methodology employs payload stoichiometry-based chromatographic resolution for clustering isomeric PEG species. Complementarily, diagnostic product ions at m/z 699.83, 569.27, and 587.28 enable systematic differentiation between double-loaded, single-loaded, and released irinotecan payload. This approach successfully identifies eight metabolic clusters spanning from PEG-conjugates, cleaved PEG segments, and released small-molecule species. Its demonstrated capacity to deconvolute complex metabolic profiles—through payload-stoichiometry based chromatographic resolution coupled with diagnostic ion analysis—positions this workflow as an attractive tool for accelerating the development of PEGylated small-molecule therapeutics.
PEGylation, the controlled covalent conjugation of polyethylene glycol to therapeutics, enhances therapeutic efficacy through optimized pharmacokinetics. However, to date no high-molecular-weight PEGylated small-molecule prodrugs have received regulatory approval. This technological gap can be partially attributed to the exponential proliferation of metabolic intermediates resulting from multi-payload conjugation strategies, which introduces unprecedented analytical complexities in metabolite profiling and pharmacokinetic characterization. To address this challenge, we developed a liquid chromatography-triple-quadrupole/time-of-flight mass spectrometry platform for PEG20k-(irinotecan)3, a Phase Ⅲ clinical candidate. Our methodology employs payload stoichiometry-based chromatographic resolution for clustering isomeric PEG species. Complementarily, diagnostic product ions at m/z 699.83, 569.27, and 587.28 enable systematic differentiation between double-loaded, single-loaded, and released irinotecan payload. This approach successfully identifies eight metabolic clusters spanning from PEG-conjugates, cleaved PEG segments, and released small-molecule species. Its demonstrated capacity to deconvolute complex metabolic profiles—through payload-stoichiometry based chromatographic resolution coupled with diagnostic ion analysis—positions this workflow as an attractive tool for accelerating the development of PEGylated small-molecule therapeutics.
2026, 37(2): 110606
doi: 10.1016/j.cclet.2024.110606
Abstract:
As the chemical industry expands, the use of benzene, toluene, and xylene (collectively known as BTX) in industrial production has increased greatly. Meanwhile, the toxic nature and potential health hazards of BTX gases cannot be ignored due to low-concentration leaks underline the critical need for rapid and real-time monitoring of these gases. Chemiresistive metal oxide semiconductor (MOS)-based gas sensors, which are extensively used for gas detection in both industrial settings and everyday life, emerge as one of the optimal solutions for trace BTX detection. These sensors are highly valued for their high sensitivity and low detection limits. Nevertheless, the improvement of selectivity towards specific BTX gases to achieve efficient and precise detection still remains challenging. This review summarizes the chemiresistive MOS-based gas sensors designed for BTX detection, categorizing them based on the components of sensing materials-basically into three groups: single-component, single heterojunction, and multiple heterojunctions gas sensing materials. Further, the review proposes the future application prospects of chemiresistive MOS-based BTX gas sensors, with specific emphasis on their significance in promoting industrial safety and environmental monitoring.
As the chemical industry expands, the use of benzene, toluene, and xylene (collectively known as BTX) in industrial production has increased greatly. Meanwhile, the toxic nature and potential health hazards of BTX gases cannot be ignored due to low-concentration leaks underline the critical need for rapid and real-time monitoring of these gases. Chemiresistive metal oxide semiconductor (MOS)-based gas sensors, which are extensively used for gas detection in both industrial settings and everyday life, emerge as one of the optimal solutions for trace BTX detection. These sensors are highly valued for their high sensitivity and low detection limits. Nevertheless, the improvement of selectivity towards specific BTX gases to achieve efficient and precise detection still remains challenging. This review summarizes the chemiresistive MOS-based gas sensors designed for BTX detection, categorizing them based on the components of sensing materials-basically into three groups: single-component, single heterojunction, and multiple heterojunctions gas sensing materials. Further, the review proposes the future application prospects of chemiresistive MOS-based BTX gas sensors, with specific emphasis on their significance in promoting industrial safety and environmental monitoring.
2026, 37(2): 110960
doi: 10.1016/j.cclet.2025.110960
Abstract:
Cancer is the second leading cause of death globally. Its treatment remains a major challenge due to the disease's complexity, heterogeneity, and adaptive nature. Among the array of available treatments, targeted therapy emerges as a paramount approach to address this substantial unmet clinical need, owing to its precise tumor targeting capabilities and potential for mitigating tumor progression risks. Drug conjugates are in high demand for targeted therapy due to their unique ligand specificity and potent cytotoxicity, thereby significantly enhancing therapeutic efficacy and reducing the incidence of adverse effects. Therefore, as a burgeoning field in biomedical research, it is timely to outline the latest advances in drug conjugates-driven cancer treatment. Herein, we aim to present the emerging breakthroughs in this exciting field at the intersection of target ligands, linkers, payloads, and cancer treatments. This review focuses on several drug conjugates-related strategies, including antibody-drug conjugates (ADCs), peptide-drug conjugates (PDCs), small molecule-drug conjugates (SMDCs), aptamer-drug conjugates (ApDCs) and radionuclide-drug conjugates (RDCs). Finally, we discuss the fundamentals behind drug conjugate-based anticancer therapeutics, along with their inherent advantages and associated challenges, as well as recent research advances.
Cancer is the second leading cause of death globally. Its treatment remains a major challenge due to the disease's complexity, heterogeneity, and adaptive nature. Among the array of available treatments, targeted therapy emerges as a paramount approach to address this substantial unmet clinical need, owing to its precise tumor targeting capabilities and potential for mitigating tumor progression risks. Drug conjugates are in high demand for targeted therapy due to their unique ligand specificity and potent cytotoxicity, thereby significantly enhancing therapeutic efficacy and reducing the incidence of adverse effects. Therefore, as a burgeoning field in biomedical research, it is timely to outline the latest advances in drug conjugates-driven cancer treatment. Herein, we aim to present the emerging breakthroughs in this exciting field at the intersection of target ligands, linkers, payloads, and cancer treatments. This review focuses on several drug conjugates-related strategies, including antibody-drug conjugates (ADCs), peptide-drug conjugates (PDCs), small molecule-drug conjugates (SMDCs), aptamer-drug conjugates (ApDCs) and radionuclide-drug conjugates (RDCs). Finally, we discuss the fundamentals behind drug conjugate-based anticancer therapeutics, along with their inherent advantages and associated challenges, as well as recent research advances.
2026, 37(2): 110990
doi: 10.1016/j.cclet.2025.110990
Abstract:
The stimulator of interferon genes (STING), as a critical innate immune sensor, has been widely and continually explored in immune-related disease treatment. As lipid bilayer-closed particles derived from cells, extracellular vesicles (EVs) inherently function in target-guided intercellular communication. To incorporate the native merits of EVs into STING pathways, i.e., engineered EV@STING, poor bioavailability and off-target issues that STING activators possess could be significantly overcome. In this review, emerged STING activators such as nitrogen-containing heterocyclic structures and the universal STING activation strategy (uniSTING) are firstly summarized. Diverse EVs sources from mesenchymal stem cells (MSCs) and innate and adaptive immune cells may evoke distinct regulatory results. Concurrently, how the EVs contents including double-stranded DNA (dsDNA), microRNA (miRNA), cyclic GMP-AMP synthase (cGAS) and 2′3′-cyclic GMP-AMP (2′3′-cGAMP) proteins participate in the regulation of STING activation are widely studied. After mastering the two pivotal aspects of EV@STING, their immunomodulatory roles including in pathogen infection, inflammatory diseases, and cancer therapy are comprehensively summed up and discussed. Finally, in cancer study field, therapeutic challenges and clinical translational opportunities of EV@STING are thoroughly evaluated.
The stimulator of interferon genes (STING), as a critical innate immune sensor, has been widely and continually explored in immune-related disease treatment. As lipid bilayer-closed particles derived from cells, extracellular vesicles (EVs) inherently function in target-guided intercellular communication. To incorporate the native merits of EVs into STING pathways, i.e., engineered EV@STING, poor bioavailability and off-target issues that STING activators possess could be significantly overcome. In this review, emerged STING activators such as nitrogen-containing heterocyclic structures and the universal STING activation strategy (uniSTING) are firstly summarized. Diverse EVs sources from mesenchymal stem cells (MSCs) and innate and adaptive immune cells may evoke distinct regulatory results. Concurrently, how the EVs contents including double-stranded DNA (dsDNA), microRNA (miRNA), cyclic GMP-AMP synthase (cGAS) and 2′3′-cyclic GMP-AMP (2′3′-cGAMP) proteins participate in the regulation of STING activation are widely studied. After mastering the two pivotal aspects of EV@STING, their immunomodulatory roles including in pathogen infection, inflammatory diseases, and cancer therapy are comprehensively summed up and discussed. Finally, in cancer study field, therapeutic challenges and clinical translational opportunities of EV@STING are thoroughly evaluated.
2026, 37(2): 111032
doi: 10.1016/j.cclet.2025.111032
Abstract:
Pulmonary diseases have long posed a severe threat to human life and health. The incidence and mortality rates of pulmonary diseases have shown a rising trend year by year, highlighting the urgency of developing safe and effective therapeutic approaches. In recent years, to address the challenges faced by traditional treatment strategies for pulmonary diseases, the interdisciplinary integration has greatly promoted the rapid development of biomedical polymer materials in the field of pulmonary disease treatment. This review provides a detailed description of the structural characteristics of lung tissue, types of pulmonary diseases, traditional treatment methods, the categories and properties of biomedical polymer materials applied to pulmonary diseases. We systematically elaborate on the applications of biomedical polymer materials in the treatment of different pulmonary diseases and thoroughly discuss their functional roles in pulmonary diseases, particularly in the delivery of therapeutic agents to diseased sites, the formation of pulmonary aerosol formulations, and the facilitation of the effective accumulation of therapeutic agents. The latest research progresses of biomedical polymer materials are also introduced in pulmonary disease treatment. We have highlighted the current challenges and development opportunities of biomedical polymer materials in the treatment of pulmonary diseases, and provide future research directions for biomedical polymer materials in this field. This review will provide valuable reference for the basic research and clinical application of biomedical polymer materials in pulmonary disease treatment.
Pulmonary diseases have long posed a severe threat to human life and health. The incidence and mortality rates of pulmonary diseases have shown a rising trend year by year, highlighting the urgency of developing safe and effective therapeutic approaches. In recent years, to address the challenges faced by traditional treatment strategies for pulmonary diseases, the interdisciplinary integration has greatly promoted the rapid development of biomedical polymer materials in the field of pulmonary disease treatment. This review provides a detailed description of the structural characteristics of lung tissue, types of pulmonary diseases, traditional treatment methods, the categories and properties of biomedical polymer materials applied to pulmonary diseases. We systematically elaborate on the applications of biomedical polymer materials in the treatment of different pulmonary diseases and thoroughly discuss their functional roles in pulmonary diseases, particularly in the delivery of therapeutic agents to diseased sites, the formation of pulmonary aerosol formulations, and the facilitation of the effective accumulation of therapeutic agents. The latest research progresses of biomedical polymer materials are also introduced in pulmonary disease treatment. We have highlighted the current challenges and development opportunities of biomedical polymer materials in the treatment of pulmonary diseases, and provide future research directions for biomedical polymer materials in this field. This review will provide valuable reference for the basic research and clinical application of biomedical polymer materials in pulmonary disease treatment.
2026, 37(2): 111275
doi: 10.1016/j.cclet.2025.111275
Abstract:
Human health is seriously jeopardized by infections caused by pathogenic microorganisms. The current traditional disinfection technologies have many defects, such as producing harmful by-products, being affected by water turbidity, and high energy consumption. The growing concern for microbial safety has brought non-thermal plasma (NTP) disinfection technology into the spotlight. NTP is a promising disinfection technology with advantages such as environmental protection, safety, room temperature disinfection, short disinfection cycle, and wide applicability. Researchers are continuously optimizing NTP reactions to improve disinfection efficiency. This paper provides an integrated analysis of both plasma disinfection in water and plasma-activated water (PAW) disinfection on object surfaces. NTP can directly treat bacterial contaminated water, and can also be employed to produce PAW as a disinfectant for treating bacteria on surfaces. This review introduces the fundamental concepts and commonly used equipment related to NTP technology, analyzes the influencing factors and mechanisms of disinfection, and concludes by outlining the future directions of NTP technology in the field of disinfection. We hope to provide a reference for the research and practice of bacterial pollution issues.
Human health is seriously jeopardized by infections caused by pathogenic microorganisms. The current traditional disinfection technologies have many defects, such as producing harmful by-products, being affected by water turbidity, and high energy consumption. The growing concern for microbial safety has brought non-thermal plasma (NTP) disinfection technology into the spotlight. NTP is a promising disinfection technology with advantages such as environmental protection, safety, room temperature disinfection, short disinfection cycle, and wide applicability. Researchers are continuously optimizing NTP reactions to improve disinfection efficiency. This paper provides an integrated analysis of both plasma disinfection in water and plasma-activated water (PAW) disinfection on object surfaces. NTP can directly treat bacterial contaminated water, and can also be employed to produce PAW as a disinfectant for treating bacteria on surfaces. This review introduces the fundamental concepts and commonly used equipment related to NTP technology, analyzes the influencing factors and mechanisms of disinfection, and concludes by outlining the future directions of NTP technology in the field of disinfection. We hope to provide a reference for the research and practice of bacterial pollution issues.
2026, 37(2): 111305
doi: 10.1016/j.cclet.2025.111305
Abstract:
Pyrimidine is a widely used compound in pesticides and medicine, with over 60 commercial pesticides containing a pyrimidine structure. Examples include the insecticide flufenerim, herbicide nicosulfuron, fungicide mepanipyrim, antiviral agent ningnanmycin, and plant growth regulator ancymidol. This paper reviews the characteristics from 2014 to 2024 of highly active pyrimidine-containing compounds and their biological activities, focusing on insecticidal, herbicidal, antibacterial, antiviral, and plant growth regulation properties. The goal is to provide insights for the design and synthesis of new pyrimidine-based pesticide candidates.
Pyrimidine is a widely used compound in pesticides and medicine, with over 60 commercial pesticides containing a pyrimidine structure. Examples include the insecticide flufenerim, herbicide nicosulfuron, fungicide mepanipyrim, antiviral agent ningnanmycin, and plant growth regulator ancymidol. This paper reviews the characteristics from 2014 to 2024 of highly active pyrimidine-containing compounds and their biological activities, focusing on insecticidal, herbicidal, antibacterial, antiviral, and plant growth regulation properties. The goal is to provide insights for the design and synthesis of new pyrimidine-based pesticide candidates.
2026, 37(2): 111315
doi: 10.1016/j.cclet.2025.111315
Abstract:
Among various advanced oxidation processes (AOPs), heterogeneous catalytic ozonation has garnered extensive attention in wastewater treatment owing to its broad pH range applicability and the elimination of the need for additional energy input. Enhancing catalyst activity by introducing oxygen vacancies has been used extensively in heterogeneous catalytic ozonation. This paper reviews prevalent methods for the construction and characterization of oxygen vacancies. Based on a thorough examination of existing research, the role of oxygen vacancies is categorized according to their primary mechanisms of action in heterogeneous catalytic ozonation. For example, modulation of the catalyst electronic structure to enhance electron transfer; participation in the reaction as an active site to generate radicals and non-radicals; and exposure of more metal sites to enhance the reaction. Lastly, the paper delineates the limitations and future research directions concerning the role of oxygen vacancies in catalytic ozonation. This review addresses the gap in existing literature concerning the role of oxygen vacancies in catalytic ozone systems, establishes a comprehensive theoretical framework to aid in the design of efficient ozone catalysts, and delves into the functionality of oxygen vacancies in heterogeneous catalytic ozone reactions.
Among various advanced oxidation processes (AOPs), heterogeneous catalytic ozonation has garnered extensive attention in wastewater treatment owing to its broad pH range applicability and the elimination of the need for additional energy input. Enhancing catalyst activity by introducing oxygen vacancies has been used extensively in heterogeneous catalytic ozonation. This paper reviews prevalent methods for the construction and characterization of oxygen vacancies. Based on a thorough examination of existing research, the role of oxygen vacancies is categorized according to their primary mechanisms of action in heterogeneous catalytic ozonation. For example, modulation of the catalyst electronic structure to enhance electron transfer; participation in the reaction as an active site to generate radicals and non-radicals; and exposure of more metal sites to enhance the reaction. Lastly, the paper delineates the limitations and future research directions concerning the role of oxygen vacancies in catalytic ozonation. This review addresses the gap in existing literature concerning the role of oxygen vacancies in catalytic ozone systems, establishes a comprehensive theoretical framework to aid in the design of efficient ozone catalysts, and delves into the functionality of oxygen vacancies in heterogeneous catalytic ozone reactions.
2026, 37(2): 111371
doi: 10.1016/j.cclet.2025.111371
Abstract:
Vacuum-ultraviolet (VUV) radiation is high-energy UV radiation with a wavelength of 100–200 nm capable of decomposing/mineralizing hazardous emerging organic pollutants (EPs) in water through direct photolysis and/or by generating reactive free radicals (RFRs) during photolysis. However, due to the unsatisfactory photoelectric conversion rate, strong absorption by oxygen and water molecules, and other characteristics of VUV radiation, its application and development are hindered, leading to misconceptions regarding high energy consumption and insufficient free radical yield. The objectives of our assessment in this review are as follows: The illumination of the photochemical characteristics of VUV and the reactivity of aqueous solutions. Summarization of accurate UV dose and energy evaluation criteria. Comparison and analysis of the photochemical mechanisms and reaction kinetics of different types of EPs via VUV direct photolysis, as well as the interference origins of typical substrates in water for VUV decontamination. We found that quantities typically reported in VUV photochemical reactions of engineered systems are underreported in low-pressure mercury lamp (LPUV) photochemical reactions, especially a quantitative indicator of the species or energy that induces a chemical reaction. The absence of these quantities has made it difficult to assess the fundamental performance of VUV photolysis fully compared with that of UV-C. Some studies have sought to optimize VUV-advanced reduction processes (VUV-ARP) or VUV reactor treatment of these contaminants; however, an abundant evaluation of the reaction origins and processes between VUV-derived main RFRs and reactants (H2O, O2, organic matter, inorganic ions, etc.) is essential, cause these scientific elements will provide the possibility to break the application gap for VUV in the field of EPs treating. Overall, the data compilation, analysis, and research recommendations provided in this review will form the basis for all photochemical reactions initiated by VUV radiation with water as the backing agent.
Vacuum-ultraviolet (VUV) radiation is high-energy UV radiation with a wavelength of 100–200 nm capable of decomposing/mineralizing hazardous emerging organic pollutants (EPs) in water through direct photolysis and/or by generating reactive free radicals (RFRs) during photolysis. However, due to the unsatisfactory photoelectric conversion rate, strong absorption by oxygen and water molecules, and other characteristics of VUV radiation, its application and development are hindered, leading to misconceptions regarding high energy consumption and insufficient free radical yield. The objectives of our assessment in this review are as follows: The illumination of the photochemical characteristics of VUV and the reactivity of aqueous solutions. Summarization of accurate UV dose and energy evaluation criteria. Comparison and analysis of the photochemical mechanisms and reaction kinetics of different types of EPs via VUV direct photolysis, as well as the interference origins of typical substrates in water for VUV decontamination. We found that quantities typically reported in VUV photochemical reactions of engineered systems are underreported in low-pressure mercury lamp (LPUV) photochemical reactions, especially a quantitative indicator of the species or energy that induces a chemical reaction. The absence of these quantities has made it difficult to assess the fundamental performance of VUV photolysis fully compared with that of UV-C. Some studies have sought to optimize VUV-advanced reduction processes (VUV-ARP) or VUV reactor treatment of these contaminants; however, an abundant evaluation of the reaction origins and processes between VUV-derived main RFRs and reactants (H2O, O2, organic matter, inorganic ions, etc.) is essential, cause these scientific elements will provide the possibility to break the application gap for VUV in the field of EPs treating. Overall, the data compilation, analysis, and research recommendations provided in this review will form the basis for all photochemical reactions initiated by VUV radiation with water as the backing agent.
2026, 37(2): 111556
doi: 10.1016/j.cclet.2025.111556
Abstract:
The Smiles rearrangement is an exceptionally versatile method in organic synthesis, providing a broad canvas for designing cascade reactions that construct new Csp2-Y (Y = C, O, N, S, CO, etc.) bonds. Among the various types of Smiles rearrangement, the radical-type variant has emerged as a more powerful, mild, efficient, and modern synthetic technique compared to its traditional ionic counterpart. This approach excels in generating new (hetero)aromatic migration products, enabling significant advancements in recent years. This tutorial review focuses on the recent progress, since 2016, in the development and application of radical Smiles rearrangement in organic chemistry. Special attention is paid to novel transformations achieved through photochemical, electrochemical, and transition metal catalysis methods.
The Smiles rearrangement is an exceptionally versatile method in organic synthesis, providing a broad canvas for designing cascade reactions that construct new Csp2-Y (Y = C, O, N, S, CO, etc.) bonds. Among the various types of Smiles rearrangement, the radical-type variant has emerged as a more powerful, mild, efficient, and modern synthetic technique compared to its traditional ionic counterpart. This approach excels in generating new (hetero)aromatic migration products, enabling significant advancements in recent years. This tutorial review focuses on the recent progress, since 2016, in the development and application of radical Smiles rearrangement in organic chemistry. Special attention is paid to novel transformations achieved through photochemical, electrochemical, and transition metal catalysis methods.
2026, 37(2): 111593
doi: 10.1016/j.cclet.2025.111593
Abstract:
Polyimide-linkage covalent organic frameworks (PI-COFs), as a subclass of the COFs material family, featuring the unique combination of excellent thermal stability of polyimide, tunable pore sizes, as well as high crystallinity and surface area of COFs, are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation, catalysis, chemical sensing, and energy storage. Therefore, it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development. In this review, we offer a comprehensive overview of recent advancements in PI-COFs, emphasizing their synthesis methods, design principles and applications. Finally, our brief outlooks on the current challenges and future developments of PI-COFs are provided. Overall, this review aims to guide the recent and future development of PI-COFs.
Polyimide-linkage covalent organic frameworks (PI-COFs), as a subclass of the COFs material family, featuring the unique combination of excellent thermal stability of polyimide, tunable pore sizes, as well as high crystallinity and surface area of COFs, are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation, catalysis, chemical sensing, and energy storage. Therefore, it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development. In this review, we offer a comprehensive overview of recent advancements in PI-COFs, emphasizing their synthesis methods, design principles and applications. Finally, our brief outlooks on the current challenges and future developments of PI-COFs are provided. Overall, this review aims to guide the recent and future development of PI-COFs.
2026, 37(2): 111608
doi: 10.1016/j.cclet.2025.111608
Abstract:
Adjuvants enhance and prolong the immune response to therapeutic agents, such as drugs and vaccines. However, conventional adjuvants have limitations in terms of immune specificity and duration. Nanoadjuvants can leverage their nanoscale size to increase the capture efficacy of antigens by antigen-presenting cells and improve immunogen presentation for targeted delivery. Furthermore, noninvasive visualization of bifunctional nanoadjuvants with integrated efficacy and imaging postdelivery can provide insights into in vivo distribution and performance, aiding in the optimization and design of new dosage forms. This review systematically summarizes the structure, assembly, and function of nanoadjuvants alongside contrast agents. It delves into the impact of complex structures formed by nanoadjuvant-contrast agent interactions on antigen presentation, migration, imaging tracking, and visualization of immune cell recruitment. It also discusses how imaging can determine optimal immune intervals, vaccine safety, and toxicity while enabling diagnostic and therapeutic integration. Moreover, this paper discusses potential applications of novel adjuvants and promising imaging technologies that could have implications for future vaccine and drug development endeavors.
Adjuvants enhance and prolong the immune response to therapeutic agents, such as drugs and vaccines. However, conventional adjuvants have limitations in terms of immune specificity and duration. Nanoadjuvants can leverage their nanoscale size to increase the capture efficacy of antigens by antigen-presenting cells and improve immunogen presentation for targeted delivery. Furthermore, noninvasive visualization of bifunctional nanoadjuvants with integrated efficacy and imaging postdelivery can provide insights into in vivo distribution and performance, aiding in the optimization and design of new dosage forms. This review systematically summarizes the structure, assembly, and function of nanoadjuvants alongside contrast agents. It delves into the impact of complex structures formed by nanoadjuvant-contrast agent interactions on antigen presentation, migration, imaging tracking, and visualization of immune cell recruitment. It also discusses how imaging can determine optimal immune intervals, vaccine safety, and toxicity while enabling diagnostic and therapeutic integration. Moreover, this paper discusses potential applications of novel adjuvants and promising imaging technologies that could have implications for future vaccine and drug development endeavors.
2026, 37(2): 111629
doi: 10.1016/j.cclet.2025.111629
Abstract:
Carbon-rich cycloarene macrocycles can adopt multiple atropisomeric forms due to steric hindrance restricting σ-bond rotation. These distinct conformations exhibit variations in cavity structure, electronic properties, and functional site distribution, leading to diverse molecular recognition and self-assembly behaviors. In recent years, research on carbon-rich cycloarene macrocyclic compounds has emerged as a cutting-edge and interdisciplinary focus in the fields of carbon-rich functional molecules and macrocyclic chemistry. This review provides a comprehensive overview of the development of atropisomers in carbon-rich cycloarene macrocycles, spanning their design and synthesis, optoelectronic properties, and supramolecular chemistry.
Carbon-rich cycloarene macrocycles can adopt multiple atropisomeric forms due to steric hindrance restricting σ-bond rotation. These distinct conformations exhibit variations in cavity structure, electronic properties, and functional site distribution, leading to diverse molecular recognition and self-assembly behaviors. In recent years, research on carbon-rich cycloarene macrocyclic compounds has emerged as a cutting-edge and interdisciplinary focus in the fields of carbon-rich functional molecules and macrocyclic chemistry. This review provides a comprehensive overview of the development of atropisomers in carbon-rich cycloarene macrocycles, spanning their design and synthesis, optoelectronic properties, and supramolecular chemistry.
2026, 37(2): 111678
doi: 10.1016/j.cclet.2025.111678
Abstract:
Peptides play important roles in chemistry, medicinal chemistry and life science, due to their high efficiency and specificity, unusual biological and therapeutic properties. As naturally occurring peptides often face with their intrinsic limitations including metabolic instability and low membrane permeability, the strategies for synthesizing unnatural amino acids and peptides are explored. Among the methods for modifying amino acids and peptides, chemo- and site-selective approaches are preferred because of the ability to fine-tuning structural features. Recently, transition metal-catalyzed C-H activation has been employed for the functionalization of amino acids and peptides. Through domino C-H activation/annulation, a series of structurally complex and diverse amino acids and peptides is constructed. This review highlights recent advances in the synthesis of unnatural amino acids and peptides via transition metal-catalyzed C-H activation/annulation.
Peptides play important roles in chemistry, medicinal chemistry and life science, due to their high efficiency and specificity, unusual biological and therapeutic properties. As naturally occurring peptides often face with their intrinsic limitations including metabolic instability and low membrane permeability, the strategies for synthesizing unnatural amino acids and peptides are explored. Among the methods for modifying amino acids and peptides, chemo- and site-selective approaches are preferred because of the ability to fine-tuning structural features. Recently, transition metal-catalyzed C-H activation has been employed for the functionalization of amino acids and peptides. Through domino C-H activation/annulation, a series of structurally complex and diverse amino acids and peptides is constructed. This review highlights recent advances in the synthesis of unnatural amino acids and peptides via transition metal-catalyzed C-H activation/annulation.
2026, 37(2): 111728
doi: 10.1016/j.cclet.2025.111728
Abstract:
The application of DNA hybridization technology, grounded in Watson-Crick base pairing, has facilitated the rational design of framework nucleic acids (FNAs) featuring adaptable shapes and dimensions. These nanostructures exhibit remarkable stability and reproducibility, making them promising candidates for biomedical applications. Among various FNAs, tetrahedral FNAs (tFNAs), first introduced by Turberfield, are nanoscale assemblies of oligonucleotides that possess unique physical, chemical, and biological properties. Previous studies have demonstrated that tFNAs exhibit excellent cellular uptake, enhanced tissue permeability, and strong capabilities to promote cell migration, proliferation, and differentiation. Moreover, the intrinsic ability of tFNAs to efficiently penetrate cell membranes allows tFNAs to serve as versatile carriers for small-molecule drugs or functional oligonucleotides, thereby exerting significant anti-inflammatory, antioxidant, antibacterial, and immunomodulatory effects. These features highlight the therapeutic potential of tFNA-based complexes in skin, mucosal, and barrier tissue repair and regeneration. This review provides a comprehensive analysis of recent advances in the application of tFNAs for the prevention and treatment of skin, mucosal, and barrier tissue diseases, with a focus on their mechanisms of action and future prospects in regenerative medicine and targeted therapies.
The application of DNA hybridization technology, grounded in Watson-Crick base pairing, has facilitated the rational design of framework nucleic acids (FNAs) featuring adaptable shapes and dimensions. These nanostructures exhibit remarkable stability and reproducibility, making them promising candidates for biomedical applications. Among various FNAs, tetrahedral FNAs (tFNAs), first introduced by Turberfield, are nanoscale assemblies of oligonucleotides that possess unique physical, chemical, and biological properties. Previous studies have demonstrated that tFNAs exhibit excellent cellular uptake, enhanced tissue permeability, and strong capabilities to promote cell migration, proliferation, and differentiation. Moreover, the intrinsic ability of tFNAs to efficiently penetrate cell membranes allows tFNAs to serve as versatile carriers for small-molecule drugs or functional oligonucleotides, thereby exerting significant anti-inflammatory, antioxidant, antibacterial, and immunomodulatory effects. These features highlight the therapeutic potential of tFNA-based complexes in skin, mucosal, and barrier tissue repair and regeneration. This review provides a comprehensive analysis of recent advances in the application of tFNAs for the prevention and treatment of skin, mucosal, and barrier tissue diseases, with a focus on their mechanisms of action and future prospects in regenerative medicine and targeted therapies.
2026, 37(2): 111834
doi: 10.1016/j.cclet.2025.111834
Abstract:
Carbenes as one of the most important class of intermediates have been widely utilized in various organic synthetic transformations. Carbene insertion-initiated ring-opening reactions of cyclic ethers offer a valuable strategy for constructing new carbon-oxygen bonds. In comparison with traditional thermal or metal-mediated carbene transfer reactions, visible-light-promoted multi-component reaction strategy provides a mild and eco-friendly approach to access densely functionalized molecules. Recently, visible-light-induced multi-component carbene transfer reactions of diazo compounds have been rapidly developed and attracted a great deal of research interest of chemists owing to their advantages of simple operation, mild condition, high atom economy and rich structural diversity. This paper summarizes the recent research progress on the visible-light-promoted multi-component carbene transfer reactions of diazo compounds via ring-opening of cyclic ethers with various nucleophiles. The reaction patterns of different nucleophiles and their corresponding mechanism are described in this review. The future research direction and challenges in this area are also discussed.
Carbenes as one of the most important class of intermediates have been widely utilized in various organic synthetic transformations. Carbene insertion-initiated ring-opening reactions of cyclic ethers offer a valuable strategy for constructing new carbon-oxygen bonds. In comparison with traditional thermal or metal-mediated carbene transfer reactions, visible-light-promoted multi-component reaction strategy provides a mild and eco-friendly approach to access densely functionalized molecules. Recently, visible-light-induced multi-component carbene transfer reactions of diazo compounds have been rapidly developed and attracted a great deal of research interest of chemists owing to their advantages of simple operation, mild condition, high atom economy and rich structural diversity. This paper summarizes the recent research progress on the visible-light-promoted multi-component carbene transfer reactions of diazo compounds via ring-opening of cyclic ethers with various nucleophiles. The reaction patterns of different nucleophiles and their corresponding mechanism are described in this review. The future research direction and challenges in this area are also discussed.
2026, 37(2): 111859
doi: 10.1016/j.cclet.2025.111859
Abstract:
Catalytic CO2-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis. Single-atom catalysts (SACs) with maximized atomic utilization, tailored electronic configurations and unique metal-support interactions, exhibit superior performance in CO2 activation and methanol synthesis. This review systematically compares reaction mechanisms and pathways across thermal, photocatalytic and electrocatalytic systems, emphasizing structure-activity relationships governed by active sites, coordination microenvironments and support functionalities. Through case studies of representative SACs, we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity. A critical analysis of reaction parameters (e.g., temperature, pressure) reveals condition-dependent catalytic behaviors in thermal system, with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps. While thermal catalysis achieves industrially viable methanol yields, the scalability is constrained by energy-intensive operation and catalyst sintering. Conversely, photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations. To address the challenges, we propose strategic research priorities on precise design of active sites, synergy of multiple technological pathways, development of intelligent catalytic systems and diverse CO2 feedstock compatibility. These insights establish a framework for developing next-generation SACs, offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.
Catalytic CO2-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis. Single-atom catalysts (SACs) with maximized atomic utilization, tailored electronic configurations and unique metal-support interactions, exhibit superior performance in CO2 activation and methanol synthesis. This review systematically compares reaction mechanisms and pathways across thermal, photocatalytic and electrocatalytic systems, emphasizing structure-activity relationships governed by active sites, coordination microenvironments and support functionalities. Through case studies of representative SACs, we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity. A critical analysis of reaction parameters (e.g., temperature, pressure) reveals condition-dependent catalytic behaviors in thermal system, with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps. While thermal catalysis achieves industrially viable methanol yields, the scalability is constrained by energy-intensive operation and catalyst sintering. Conversely, photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations. To address the challenges, we propose strategic research priorities on precise design of active sites, synergy of multiple technological pathways, development of intelligent catalytic systems and diverse CO2 feedstock compatibility. These insights establish a framework for developing next-generation SACs, offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.
2026, 37(2): 111957
doi: 10.1016/j.cclet.2025.111957
Abstract:
Carbon dots (CDs), a class of emerging fluorescent nanomaterials, have garnered notable attention in the biomedical field owing to their outstanding photoluminescence properties, excellent biocompatibility, and ease of synthesis and functionalization. Recently, numerous CDs have been developed that allow precise subcellular localization through surface modifications or covalent conjugation with targeting ligands such as peptides, small molecules, Golgi-specific agents, and cell membrane-specific agents. This review begins with an overview of the synthesis strategies of CDs, highlighting their exceptional optical properties, stability, biocompatibility, and significance for subcellular imaging. The mechanisms by which CDs target specific organelles, including the nucleus, mitochondrion, lysosomes, Golgi apparatus, and cell membrane, are discussed. These mechanisms include specific targeting molecules, pH-sensitive targeting, charge-driven interactions, and hydrophobic and hydrophilic dynamics. Furthermore, we summarize their applications in subcellular imaging, such as the long-term dynamic monitoring of organelles, sensing, reactive oxygen species scavenging, and therapy. By presenting a comprehensive review of CDs in subcellular imaging, we aim to pave the way for further development of CDs in bioimaging and related biomedical applications.
Carbon dots (CDs), a class of emerging fluorescent nanomaterials, have garnered notable attention in the biomedical field owing to their outstanding photoluminescence properties, excellent biocompatibility, and ease of synthesis and functionalization. Recently, numerous CDs have been developed that allow precise subcellular localization through surface modifications or covalent conjugation with targeting ligands such as peptides, small molecules, Golgi-specific agents, and cell membrane-specific agents. This review begins with an overview of the synthesis strategies of CDs, highlighting their exceptional optical properties, stability, biocompatibility, and significance for subcellular imaging. The mechanisms by which CDs target specific organelles, including the nucleus, mitochondrion, lysosomes, Golgi apparatus, and cell membrane, are discussed. These mechanisms include specific targeting molecules, pH-sensitive targeting, charge-driven interactions, and hydrophobic and hydrophilic dynamics. Furthermore, we summarize their applications in subcellular imaging, such as the long-term dynamic monitoring of organelles, sensing, reactive oxygen species scavenging, and therapy. By presenting a comprehensive review of CDs in subcellular imaging, we aim to pave the way for further development of CDs in bioimaging and related biomedical applications.
2026, 37(2): 111990
doi: 10.1016/j.cclet.2025.111990
Abstract:
In 2024, the MOE Key Laboratory of Macromolecular Synthesis and Functionalization at Zhejiang University continued its impactful researches across five core areas. In controllable catalytic polymerization, organoboron catalysts were developed for CO2 copolymerization and novel photoresist materials. Studies in microstructure and rheology elucidated universal deformation modes in graphene-based 2D membranes and improved graphene fiber properties through shear alignment engineering, defect control, and enhanced interlayer entanglement. For separating functional polymers, Janus membranes and channels were created for multiphase separation, liquid-phase molecular layer-by-layer deposition technique was developed to fabricate aromatic polyamide nanofilms, and the harmonic amide bond density was established as a valuable parameter for polyamide structural analysis. In biomedical functional polymers, a sustainable carboxyl-ester transesterification strategy was proposed for upcycling poly(ethylene terephthalate) (PET) waste into biodegradable plastics. Additionally, immunocompatible biomaterials were designed utilizing zwitterionic polypeptides and albumin-derived coatings, and Cu2+-phenolic nanoflower was designed to combat fungal infections by combining cuproptosis and cell wall digestion. Further, the researchers developed a gelatin-DOPA-knob/fibrinogen hydrogel to achieve rapid and robust hemostatic sealing, utilized a double-network polyelectrolyte-coated hydrogel for enhancing endothelialization of left atrial appendage (LAA) occluders, and the researchers also demonstrated that image-guided high-intensity focused ultrasound enables manipulation of shape-memory polymers. Finally, in the realm of photo-electro-magnetic functional polymers, precise control of through-space conjugation was shown to enhance organic luminescence. Topologically structured hydrogels were revealed to exhibit autonomous actuation. Also, solar-driven photothermal ion pumps were developed for selective lithium extraction from seawater, and high-performance non-solvated C60 single-crystal films were prepared via facile bar coating. Lastly, the researchers demonstrated outstanding dielectric properties of polyethylene (PE) lamellar single crystals. The relevant works are reviewed in this paper.
In 2024, the MOE Key Laboratory of Macromolecular Synthesis and Functionalization at Zhejiang University continued its impactful researches across five core areas. In controllable catalytic polymerization, organoboron catalysts were developed for CO2 copolymerization and novel photoresist materials. Studies in microstructure and rheology elucidated universal deformation modes in graphene-based 2D membranes and improved graphene fiber properties through shear alignment engineering, defect control, and enhanced interlayer entanglement. For separating functional polymers, Janus membranes and channels were created for multiphase separation, liquid-phase molecular layer-by-layer deposition technique was developed to fabricate aromatic polyamide nanofilms, and the harmonic amide bond density was established as a valuable parameter for polyamide structural analysis. In biomedical functional polymers, a sustainable carboxyl-ester transesterification strategy was proposed for upcycling poly(ethylene terephthalate) (PET) waste into biodegradable plastics. Additionally, immunocompatible biomaterials were designed utilizing zwitterionic polypeptides and albumin-derived coatings, and Cu2+-phenolic nanoflower was designed to combat fungal infections by combining cuproptosis and cell wall digestion. Further, the researchers developed a gelatin-DOPA-knob/fibrinogen hydrogel to achieve rapid and robust hemostatic sealing, utilized a double-network polyelectrolyte-coated hydrogel for enhancing endothelialization of left atrial appendage (LAA) occluders, and the researchers also demonstrated that image-guided high-intensity focused ultrasound enables manipulation of shape-memory polymers. Finally, in the realm of photo-electro-magnetic functional polymers, precise control of through-space conjugation was shown to enhance organic luminescence. Topologically structured hydrogels were revealed to exhibit autonomous actuation. Also, solar-driven photothermal ion pumps were developed for selective lithium extraction from seawater, and high-performance non-solvated C60 single-crystal films were prepared via facile bar coating. Lastly, the researchers demonstrated outstanding dielectric properties of polyethylene (PE) lamellar single crystals. The relevant works are reviewed in this paper.
2026, 37(2): 112054
doi: 10.1016/j.cclet.2025.112054
Abstract:
In recent years, AgBiS2 nanocrystals (NCs) have emerged as a research hotspot in the field of solar cells due to their excellent optoelectronic properties and environmentally friendly characteristics. Although the theoretical power conversion efficiency (PCE) of AgBiS2 NC solar cells can reach up to 26%, the current best device only achieved a PCE of 10.84%. Such an enormous efficiency gap is primarily caused by the complex surface defects, severe carrier recombination, and undesirable energy-level mismatches. Therefore, this review comprehensively summarizes recent advancements in AgBiS2 NCs, including their crystal structures, optoelectronic properties, synthesis methods, ligand engineering, and device optimization. By fine-tuning synthesis conditions (e.g., temperature, precursor ratios) and employing ligand exchange strategies (solid-state/liquid-state), significant improvements in material performance have been realized. Furthermore, device structure optimization (e.g., transport layer selection, interface modification) and energy-level alignment engineering have further enhanced efficiency. Despite decent stabilities of AgBiS2 NCs, several challenges such as large-area uniformity and long-term device durability remain unraveled, which may be the major obstacles for their further commercialization. Future advancements in defect control, the development of novel ligands, and encapsulation technologies are expected to expand the applications of AgBiS2 NCs in flexible electronics, aerospace, and wearable devices.
In recent years, AgBiS2 nanocrystals (NCs) have emerged as a research hotspot in the field of solar cells due to their excellent optoelectronic properties and environmentally friendly characteristics. Although the theoretical power conversion efficiency (PCE) of AgBiS2 NC solar cells can reach up to 26%, the current best device only achieved a PCE of 10.84%. Such an enormous efficiency gap is primarily caused by the complex surface defects, severe carrier recombination, and undesirable energy-level mismatches. Therefore, this review comprehensively summarizes recent advancements in AgBiS2 NCs, including their crystal structures, optoelectronic properties, synthesis methods, ligand engineering, and device optimization. By fine-tuning synthesis conditions (e.g., temperature, precursor ratios) and employing ligand exchange strategies (solid-state/liquid-state), significant improvements in material performance have been realized. Furthermore, device structure optimization (e.g., transport layer selection, interface modification) and energy-level alignment engineering have further enhanced efficiency. Despite decent stabilities of AgBiS2 NCs, several challenges such as large-area uniformity and long-term device durability remain unraveled, which may be the major obstacles for their further commercialization. Future advancements in defect control, the development of novel ligands, and encapsulation technologies are expected to expand the applications of AgBiS2 NCs in flexible electronics, aerospace, and wearable devices.
2026, 37(2): 112116
doi: 10.1016/j.cclet.2025.112116
Abstract:
Sustainable development for our life is important task, which is driven by key materials and technologies. In this roadmap, we discuss three main aspects in addressing environmental questions, green chemical processes and energy challenges. They are included, such as gas treatment and separation, wastewater treatment, waste gas treatment, solid waste treatment, lithium extraction, hydrogen production, water splitting, CO2 reduction, photocatalytic clean technologies, plastic degradation, fuel cells, lithium batteries, sodium batteries, aqueous batteries, solid state batteries, metal air batteries and supercapacitors. Their status, challenges, progress and future perspectives are also discussed. We hope that this paper can give clear views on sustainable development in materials and technologies.
Sustainable development for our life is important task, which is driven by key materials and technologies. In this roadmap, we discuss three main aspects in addressing environmental questions, green chemical processes and energy challenges. They are included, such as gas treatment and separation, wastewater treatment, waste gas treatment, solid waste treatment, lithium extraction, hydrogen production, water splitting, CO2 reduction, photocatalytic clean technologies, plastic degradation, fuel cells, lithium batteries, sodium batteries, aqueous batteries, solid state batteries, metal air batteries and supercapacitors. Their status, challenges, progress and future perspectives are also discussed. We hope that this paper can give clear views on sustainable development in materials and technologies.
2026, 37(2): 111925
doi: 10.1016/j.cclet.2025.111925
Abstract:
2026, 37(2): 112045
doi: 10.1016/j.cclet.2025.112045
Abstract:
