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The first issue is scheduled to be published in Dec. 2018.

Call for Papers

CCS Chemistry is the flagship general journal for the cutting edge and fundamental research in the areas of chemica research facing global audiences published by Chinese Chemical Society. We call for excellent papers cover but not limited to synthetic chemistry, catalysis & surface chemistry, chemical theory and mechanism, chemical metrology, materials & energy chemistry, environmental chemistry, chemical biology, chemical engineering and industrial chemistry. Professional arrangement ensures that all papers can be reviewed and published online quickly and efficiently (one or two weeks).

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Dr. Hao Linxiao,;  +86-10-82449177-888

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Zeolite-based Fenton-like catalysis for pollutant removal and reclamation from wastewater
Zichen Shangguan , Xingzhong Yuan , Longbo Jiang , Yanlan Zhao , Lei Qin , Xuerong Zhou , Yan Wu , Jia Wei Chew , Hou Wang
2022, 33(11): 4719-4731  doi: 10.1016/j.cclet.2022.01.001
[Abstract](52) [FullText HTML] [PDF 5754KB](4)
Wastewater treatment and reclamation from wastewater are essential for the sustainable use of water resource. Zeolite-based heterogeneous catalysis shows great potential in circumventing the current limitations on pollutant removal and transformation to useful chemicals, inspiring advancements towards practical water treatment. This paper summarizes the methods for synthesizing zeolite-based catalyst, and the corresponding advantages and disadvantages. In comparison with traditional Fenton-like reaction, the superiority of zeolite-based catalysis lies in less sludge, wide pH range and easy recyclability. Accordingly, applications of zeolite-based Fenton-like catalysis (ZFCs) in pollutant removal and reclamation of wastewater were reviewed. Emphasis was placed on the methodological strategies in improving ZFCs, including the combination of external driving force (e.g., photocatalysis or electrochemistry), as well as the introduction of various transition metals into zeolite-based catalyst. Possible challenges and future perspectives for ZFCs were proposed.
1,n-Thiosulfonylation using thiosulfonates as dual functional reagents
Danhua Ge , Jia-Wei Chen , Pei Xu , Jinyin Pan , Xue-Qiang Chu
2022, 33(11): 4732-4739  doi: 10.1016/j.cclet.2022.02.019
[Abstract](33) [FullText HTML] [PDF 9100KB](1)
In recent years, the direct introduction of sulfonyl and sulfenyl groups into unsaturated substrates by using thiosulfonates as unique dual functional reagents has inarguably provided chemists a new platform for the diverse synthesis of important S-containing derivatives. These 1,n-thiosulfonylation reactions usually feature simple procedures, 100% atom economy, and high regioselectivity. This review focuses on the recent advancements in the transformations of thiosulfonates through 1,n-thiosulfonylation involving the formation of two distinct C-S bonds under transition-metal-catalyzed or metal-free conditions, where thiosulfonates act as both a sulfonyl and a sulfenyl component.
Degradation of florfenicol in a flow-through electro-Fenton system enhanced by wood-derived block carbon (WBC) cathode
Li Tian , Qiongfang Zhuo , Jincheng Lu , Jingjing Liu , Xiaofeng Xu , Xiaolin You , Manman Xu , Bo Yang , Junfeng Niu
2022, 33(11): 4740-4745  doi: 10.1016/j.cclet.2021.12.083
[Abstract](39) [FullText HTML] [PDF 4477KB](1)
The flow-through electro-Fenton (EF-T) reactor with WBC cathode was designed to remove florfenicol (FF). The activated WBC cathode was prepared by facile carbonization and activation methods, and featured high specific surface area, natural multi-channel structure, abundant oxygen-containing groups, good hydrophilicity, and excellent O2 reducing capacity. WBC cathode was located above Ti/Ru-IrO2 mesh anode. O2 evolved at the anode was carried to the inner wall of channel of WBC by the force of buoyancy and water flow, which increases oxygen source of H2O2 generation at the cathode. The flow-through system by using WBC electrode promote the mass transfer of O2 and FF. The production amount of H2O2 at activated WBC was 32.2 mg/L, which was almost twice as much as that at non-activated WBC (15.0 mg/L). FF removal ratio in EF-T system was 98%, which was much higher than that of traditional flow-by electro-Fenton (EF-B, 33%) or single electrooxidation system (EO, 16%). EF-T system has the lowest energy consumption (4.367 kWh/kg) among the three electrochemical systems. The cathodic adsorption, anodic electrooxidation, and EF reaction are responsible for the degradation of FF. After five consecutive cycle experiments, FF removal ratio was still 98%, indicating WBC has the good stability.
Simultaneous determination of indole metabolites of tryptophan in rat feces by chemical labeling assisted liquid chromatography-tandem mass spectrometry
Qin-Feng Zhang , Hua-Ming Xiao , Jin-Tao Zhan , Bi-Feng Yuan , Yu-Qi Feng
2022, 33(11): 4746-4749  doi: 10.1016/j.cclet.2022.01.004
[Abstract](55) [FullText HTML] [PDF 1912KB](1)
As the connecting part of diet and host physiology, intestinal microbes can convert the ingested diet into a huge number of physiologically active small molecules. Indole metabolites of tryptophan are precursors or signal molecules for many biologically active substances, which are involved in serotonin and microbial catabolism pathways. To understand the influence of tryptophan metabolism in the intestinal environment on the neurological and immune systems at the molecular level, it is important to establish a high-coverage analytical method to comprehensively analyze the metabolites involved in tryptophan metabolism. However, due to a small molecular weight and poor response during mass spectrometry analysis, as well as weak retention on the reversed-phase chromatography, determination of indole metabolites of tryptophan is challenging. Here, we proposed a method for the simultaneous determination of 20 indole metabolites of tryptophan in a single run on reversed-phase chromatography by chemical labeling coupled to liquid chromatography-tandem mass spectrometry analysis. 4-(Dimethylamino)benzaldehyde (DMAB) was used for the labeling of indole metabolites of tryptophan, which could significantly improve the detection sensitivities and retention of these metabolites on reversed-phase chromatography. With the developed method, we realized the sensitive detection and comprehensive analysis of 15 endogenous indole metabolites of tryptophan in rat feces samples with functional dyspepsia intervention by acupuncture. The developed method offers a useful tool for studying tryptophan metabolism-related diseases.
Self-powered anti-interference photoelectrochemical immunosensor based on Au/ZIS/CIS heterojunction photocathode with zwitterionic peptide anchoring
Ze Hu , Yaqun Xu , Hao Wang , Gao-Chao Fan , Xiliang Luo
2022, 33(11): 4750-4755  doi: 10.1016/j.cclet.2021.12.088
[Abstract](34) [FullText HTML] [PDF 5204KB](0)
Accurate detection of important biomarkers with ultra-low levels in complex biological matrix is one of the frontier scientific issues because of possible signal interference of potential reductive agents and protein molecules. Herein, a self-powered anti-interference photoelectrochemical (PEC) immunosensor was explored for sensitive and specific detection of model target of cardiac troponin I (cTnI). Specifically, a novel ternary heterojunction served as the photocathode to offer a remarkable current output and a zwitterionic peptide was introduced to build a robust antifouling biointerface. CuInS2 (CIS) film with porous network nanostructure was first prepared and then modified in order with ZnIn2S4 (ZIS) nanocrystals and Au nanoparticles to fabricate the Au/ZIS/CIS heterojunction photocathode. After capture cTnI antibody (Ab) was immobilized, the zwitterionic peptide KAEAKAEAPPPPC was then anchored to compete the immunosensor. The elaborated PEC immunosensor exhibited high sensitivity for target cTnI antigen (Ag) detection, with good anti-interference against reductive agents and nonspecific proteins. This integration strategy of heterojunction photocathode with zwitterionic peptide provides a new sight to develop advanced PEC immunosensors applying in practical biosamples.
The role of Cs dopants for improved activation of molecular oxygen and degradation of tetracycline over carbon nitride
Qian Liu , Hui Li , Hao Zhang , Zhurui Shen , Huiming Ji
2022, 33(11): 4756-4760  doi: 10.1016/j.cclet.2021.12.089
[Abstract](37) [FullText HTML] [PDF 5278KB](0)
Molecular oxygen (O2) is activated to reactive oxygen species (ROS) by transferring energy and carriers in the photocatalytic process, which plays an important role in environmental remediation. Herein, Cs-doped carbon nitride (CN-xCs, x = 0.2, 0.8, 1) was prepared by CsCl directly inducing the structural reconstruction of carbon nitride (CN), which had obvious molecular oxygen activation ability to promote tetracycline (TC) degradation. Besides, we explored the influence of Cs doping concentration. As a consequence, the doping concentration of Cs was an important factor affecting the activation of O2, which could cause changes in the physical and chemical structure of CN, make O enter the CN structure, form N vacancy defects and cyano groups. In addition, a proper amount of Cs doping could reduce the band gap value, increase the light absorption range, have better charge separation and transfer performance, which could remarkably promote the activation of O2. Benefiting from these advantages, CN-0.8Cs could generate a higher concentration of superoxide radicals (O2, 179.30 µmol/L), which was much higher than CN (6.22 µmol/L). Therefore, it exhibited excellent TC degradation photocatalytic performance, and the rate constant k of TC degradation was 0.020 min−1, which was 6.7 times the degradation rate of CN (k = 0.0030 min−1). Furthermore, the possible degradation pathways of TC were proposed based on the results of HPLC-MS.
Heterostructures of NiFe LDH hierarchically assembled on MoS2 nanosheets as high-efficiency electrocatalysts for overall water splitting
Xiao-Peng Li , Li-Rong Zheng , Si-Jie Liu , Ting Ouyang , Siyu Ye , Zhao-Qing Liu
2022, 33(11): 4761-4765  doi: 10.1016/j.cclet.2021.12.095
[Abstract](33) [FullText HTML] [PDF 5335KB](0)
Typically, rational interfacial engineering can effectively modify the adsorption energy of active hydrogen molecules to improve water splitting efficiency. NiFe layered double hydroxide (NiFe LDH) composite, an efficient oxygen evolution reaction (OER) catalyst, suffers from slow hydrogen evolution reaction (HER) kinetics, restricting its application for overall water splitting. Herein, we construct the hierarchical MoS2/NiFe LDH nanosheets with a heterogeneous interface used for HER and OER. Benefiting the hierarchical heterogeneous interface optimized hydrogen Gibbs free energy, tens of exposed active sites, rapid mass- and charge-transfer processes, the MoS2/NiFe LDH displays a highly efficient synergistic electrocatalytic effect. The MoS2/NiFe LDH electrode in 1 mol/L KOH exhibits excellent HER activity, only 98 mV overpotential at 10 mA/cm2. Significantly, when it assembled as anode and cathode for overall water splitting, only 1.61 V cell voltage was required to achieve 10 mA/cm2 with excellent durability (50 h).
Activation of sulfite by ferric ion for the degradation of 2,4,6-tribromophenol with the addition of sulfite in batches
Zongping Wang , Fan Bai , Lisan Cao , Siyang Yue , Jingwen Wang , Songlin Wang , Jun Ma , Pengchao Xie
2022, 33(11): 4766-4770  doi: 10.1016/j.cclet.2022.01.003
[Abstract](31) [FullText HTML] [PDF 708KB](0)
In this work, the removal of 2,4,6-tribromophenol (TBP) by ferric ion-activated sulfite [Fe(III)/S(IV)] process was systematically investigated with determining the intermediate products and evaluating the influences of some operational conditions and water matrices. Our results show that batching addition of S(IV) benefits the S(IV) utilization efficiency and TBP removal, with SO4•‒ being the primary reactive radical accounting for TBA degradation. The maximum TBP removal in the Fe(III)/S(IV) process was observed at pH 4.0 and oxygen is essential in this process. With increasing Fe(III) and S(IV) dosages from 0.05 and 0.1 mmol/L to 0.2 and 2.0 mmol/L, respectively, TBP removal followed trends of first increase then decrease. As the acute toxicity of the TBP solution was significantly reduced, the Fe(III)/S(IV) process was believed to be a good choice in the treatment of TBP.
Graphene enhanced α-MnO2 for photothermal catalytic decomposition of carcinogen formaldehyde
Xiaoshan Zeng , Chuanjia Shan , Mingdi Sun , Danni Ding , Shaopeng Rong
2022, 33(11): 4771-4775  doi: 10.1016/j.cclet.2021.12.085
[Abstract](34) [FullText HTML] [PDF 2634KB](0)
Formaldehyde (HCHO) causes increasing concerns due to its ubiquitously found in indoor air and being irritative and carcinogenic to humans. Photothermal-catalysis developed in recent years has been considered as a significant strategy for enhancing catalytic activity. Manganese oxides, compared with its strong thermocatalytic activity, generally suffer from much lower photocatalytic activity make its photochemical properties less concerned. Herein, α-MnO2 nanowires were composited with the graphene oxide (GO) via mechanical grinding and co-precipitating method, respectively. α-MnO2/GO nanohybrids prepared by co-precipitating method exhibits excellent activity, achieving 100% decomposition of HCHO with the solar-light irradiation at ambient temperature. It is found that, besides the photo-driven thermocatalysis, the photocatalysis mechanism made a major contribution to the decomposition of HCHO. The incorporation of GO, on the one hand, is beneficial to improve the optical absorption capacity and photothermal conversion efficiency; on the other hand, is conductive to electron transfer and effective separation of electrons and holes. These synergistic effects significantly improve the catalytic activity of α-MnO2/GO nanohybrids. This work proposes a new approach for the utilization of solar energy by combining manganese oxides, and also develops an efficient photothermal-catalyst to control HCHO pollution in indoor air.
Electrochemical reaction mechanism of porous Zn2Ti3O8 as a high-performance pseudocapacitive anode for Li-ion batteries
Weijie Cheng , Qi Feng , Zhanglin Guo , Guanjun Chen , Yong Wang , Lixiong Yin , Jiayin Li , Xingang Kong
2022, 33(11): 4776-4780  doi: 10.1016/j.cclet.2022.01.002
[Abstract](39) [FullText HTML] [PDF 3251KB](1)
Zn2Ti3O8, as a new type of anode material for lithium-ion batteries, is attracting enormous attention because of its low cost and excellent safety. Though decent capacities have been reported, the electrochemical reaction mechanism of Zn2Ti3O8 has rarely been studied. In this work, a porous Zn2Ti3O8 anode with considerably high capacity (421 mAh/g at 100 mA/g and 209 mAh/g at 5000 mA/g after 1500 cycles) was reported, which is even higher than ever reported titanium-based anodes materials including Li4Ti5O12, TiO2 and Li2ZnTi3O8. Here, for the first time, the accurate theoretical capacity of Zn2Ti3O8 was confirmed to be 266.4 mAh/g. It was also found that both intercalation reaction and pseudocapacitance contribute to the actual capacity of Zn2Ti3O8, making it possibly higher than the theoretical value. Most importantly, the porous structure of Zn2Ti3O8 not only promotes the intercalation reaction, but also induces high pseudocapacitance capacity (225.4 mAh/g), which boosts the reversible capacity. Therefore, it is the outstanding pseudocapacitance capacity of porous Zn2Ti3O8 that accounts for high actual capacity exceeding the theoretical one. This work elucidates the superiorities of porous structure and provides an example in designing high-performance electrodes for lithium-ion batteries.
Dual modulation of morphology and electronic structures of VN@C electrocatalyst by W doping for boosting hydrogen evolution reaction
Danyang He , Liyun Cao , Liangliang Feng , Shuainan Li , Yongqiang Feng , Guodong Li , Yifei Zhang , Jinhan Li , Jianfeng Huang
2022, 33(11): 4781-4785  doi: 10.1016/j.cclet.2022.01.006
[Abstract](37) [FullText HTML] [PDF 4143KB](1)
Developing high-efficiency and robust durability electrocatalyst for hydrogen evolution reaction (HER) in water electrolysis functions as a crucial role for the construction of green hydrogen economy, herein, ultrafine W-doped vanadium nitride nanoparticles anchored on N-doped graphitic carbon framework (WVN@NGC) are synthesized through a one-step simple pyrolysis protocol. Owing to the enlarged catalytically active sites, enhanced electrical conductivity and optimized electronic structure, the resultant VN/WN@NGC delivered the prominent HER performance with overpotentials of 143 mV and 158 mV at 10 mA/cm2 in acid and alkaline media, respectively, accompanied by the long-term stability for at least 50 h. This work highlights a novel strategy for a metal-triggered modulation of nitride-based HER electrocatalyst for sustainable energy conversion device.
Bromate formation during oxidation of bromide-containing water by the CuO catalyzed peroxymonosulfate process
Jingxin Yang , Hongrui Ma , Chuan Wang , Hong Liu
2022, 33(11): 4786-4791  doi: 10.1016/j.cclet.2022.01.008
[Abstract](37) [FullText HTML] [PDF 951KB](0)
Bromate formation has been found in the SO4•−-based oxidation processes, but previous studies primarily focused on the bromate formation in the homogeneous SO4•−-based oxidation processes. The kinetics and mechanisms of bromate formation are poorly understood in the heterogeneous SO4•−-based oxidation processes, although which have been widely studied in the eliminations of micropollutants. In this work, we found that the presence of CuO, a common heterogeneous catalyst of peroxymonosulfate (PMS), appreciably enhanced the bromate formation from the oxidation of bromide by PMS. The conversion ratio of bromide to bromate achieved over 85% within 10 min in this process. CuO was demonstrated to play a multiple role in the bromate formation: (1) catalyzed PMS to generate SO4•−, which then oxidizes bromide to bromate; (2) catalyzed the formed free bromine to disproportionate to bromate; (3) catalyzed the formed free bromine to decomposed back into bromide. In the CuO-PMS-Br system, bromate formation increases with increasing CuO dosages, initial CuO and bromide concentrations, but decreases with increasing bicarbonate concentrations. The presence of NOM (natural organic matter) resulted in a lower formed bromate accompanied with organic bromine formation. Notably, CuO catalyzes PMS to transform more than 70% of initial bromide to bromate even after recycled used for six times. The formation of bromate in the PMS catalysis by CuO system was also confirmed in real water.
A natural manganese ore as a heterogeneous catalyst to effectively activate peroxymonosulfate to oxidize organic pollutants
Jinchuan Gu , Ping Yin , Yi Chen , Honglin Zhu , Rui Wang
2022, 33(11): 4792-4797  doi: 10.1016/j.cclet.2022.01.029
[Abstract](36) [FullText HTML] [PDF 3710KB](0)
Heterogeneous transition metal catalysts are indispensable in improving environmental pollution. However, their fabrication is often costly and cumbersome, and they can easily pollute the environment. This study proposed using a natural Gabonese ore (GBO) containing MnxOy and FexOy as catalysts to degrade orange Ⅱ (OII) via peroxymonosulfate (PMS) activation. The GBO + PMS system exhibited extraordinarily high stability and catalytic activity towards OII elimination (92.2%, 0.0453 min−1). The reactive oxygen species (ROS) generated in the system were identified using radical scavenging tests and electron spin-resonance (ESR) analysis. Singlet oxygen (1O2) represented the dominant reactive species for OII degradation, while the system presented a lower reaction energy barrier and was effective in a broad pH range (2–10). This work also proposed the activation mechanism for the GBO + PMS system and OII degradation pathways. This study revealed a new approach for exploring inexpensive, eco-friendly, efficient, and stable heterogeneous transition metal catalysts.
High sensitivity ratiometric fluorescence temperature sensing using the microencapsulation of CsPbBr3 and K2SiF6: Mn4+ phosphor
Jingwen Jin , Jie Lin , Yipeng Huang , Linchun Zhang , Yaqi Jiang , Dongjie Tian , Fangyuan Lin , Yiru Wang , Xi Chen
2022, 33(11): 4798-4802  doi: 10.1016/j.cclet.2022.01.017
[Abstract](35) [FullText HTML] [PDF 2757KB](0)
A dual emission sensing film has been prepared for colorimetric temperature sensing using CsPbBr3 perovskite nanocrystals (CsPbBr3 NCs) and manganese doped potassium fluorosilicate (K2SiF6: Mn4+, KSF) encapsulated in polystyrene by a microencapsulation strategy. The CsPbBr3-KSF-PS film shows good temperature sensing response from 30 ℃ to 70 ℃, with a relative temperature sensitivity (Sr) up to 10.31% ℃−1 at 45 ℃. Meanwhile, the film maintains more than 95% intensity after 6 heating-cooling cycles and keeps its fluorescence characteristics after 3 months. The film can be used to monitor temperature change by naked eye under a UV lamp. In particular, the temperature discoloration point of the sensing film can be controlled by the ratio change of CsPbBr3: KSF to expand its applications. The study of the CsPbBr3-KSF-PS sensing mechanism in this work is helpful to provide effective strategies for the design of reliable, high sensitivity and stable temperature sensing system using CsPbBr3 NCs.
CDs assembled metal-organic framework: Exogenous coreactant-free biosensing platform with pore confinement-enhanced electrochemiluminescence
Xiu-Li Tao , Mei-Chen Pan , Xia Yang , Ruo Yuan , Ying Zhuo
2022, 33(11): 4803-4807  doi: 10.1016/j.cclet.2022.01.010
[Abstract](32) [FullText HTML] [PDF 4120KB](0)
Despite the various synthesis approachs to obtain luminous carbon dots (CDs), it is still quite challenging to construct the efficient electrochemiluminescence (ECL) owing to their low ECL reactivity and easy agglomeration. Herein, an efficient and concise ECL system was skillfully constructed by taking advantage of the nitrogen and sulfur co-doped CDs (N, S-CDs) with surfaces rich in hydrazide groups as luminophors to emit intense ECL, and metal-organic framework (MOF) as the matrix to confine CDs in its nanospace. Surprisingly, the proposed CDs assembled MOF (CDs/ZIF-8) enhanced anodic ECL signal up to 250% of pure CDs under the exogenous coreactant-free condition. As a proof of concept, the highly sensitive detection of uric acid (UA) was realized by the constructed ECL platform with a low detection limit of 3.52 nmol/L ranging from 10 nmol/L to 50 µmol/L. This work expanded ideas for the application of pore confinement effect, and provided references for the detection of disease biomarkers of gout and hyperuricemia.
Rapid differentiation of simple saccharides based on cluster ions by paper spray tandem mass spectrometry
Wangmin Hu , Tianyi Li , Yulei Yang , Shanshan Jia , Mei Zhang
2022, 33(11): 4808-4816  doi: 10.1016/j.cclet.2022.01.026
[Abstract](34) [FullText HTML] [PDF 5591KB](1)
Simple saccharides have a variety of biological functions, but their structural diversity and inherent structural features pose a major challenge for rapid analysis. In this work, we developed a derivative-free and ion mobility-free method for the rapid analysis of monosaccharides and disaccharides using paper spray tandem mass spectrometry. Trimeric cluster ions consisting of saccharide analytes, ligands and transition metal ions are used as precursor ions. We defined the R-value as the ratio of the intensity of the product ion that loses one molecule of ligand over the intensity of the product ion that loses one molecule of saccharide via collision induced dissociation (CID). The species and conformation of simple saccharides can be easily differentiated by calculating this R-value. With the capability of directly analyzing clinical samples using paper spray ionization, our method can be used to rapidly quantify the molar ratio of galactose to glucose in dried plasma samples to aid in the diagnosis of galactosemia. The analytical strategy provided herein has good potential to be applied to a wide range of saccharide analysis applications in the future.
A bench-stable reagent for C-4 selective deuteriodifluoromethylation of azines
Junqing Liang , Lefeng Dong , Feng Qian , Yijin Kong , Mingxia Wang , Xiaoyong Xu , Xusheng Shao , Zhong Li
2022, 33(11): 4817-4821  doi: 10.1016/j.cclet.2022.01.085
[Abstract](37) [FullText HTML] [PDF 5758KB](0)
Deuteriodifluoromethyl (CF2D) is a challenging and important functional group due to difficult deuterium incorporation and lack of effective precursor reagents. Herein, we report a bench-stable reagent, deuteriodifluoromethyl phosphine (DDFP) from cheap deuterium source for selectivity deuteriodifluoromethylation of azines with a high deuterium incorporation yield. The late-stage modification of complex molecules further confirmed the potential of this reagent for practical applications. We expect that our reagent to find applications in synthesis of isotope-labelled molecules of interests for drug-discovery and related ilucidation of mechanism of action.
Promotion effect of Au single-atom support graphene for CO oxidation
Ping Yan , Song Shu , Xian Shi , Jianjun Li
2022, 33(11): 4822-4827  doi: 10.1016/j.cclet.2022.01.032
[Abstract](36) [FullText HTML] [PDF 2353KB](0)
CO oxidation is a vital catalytic reaction for environmental purification, facing challenges due to the catalysts applied to oxidize CO are mainly rare and expensive noble catalysts. Since the high atomic availability, catalytic efficiency, and selectivity of single-atom catalysis, it has been widely studied and proven to be brilliant in CO oxidation. Au single-atom catalysts are regarded as excellent single-atom catalysts in oxidizing CO, whose progress is limited by the indistinct understanding of the reaction mechanism and role of the active atom. Hence, DFT calculation was used to investigate CO oxidation processes, active mechanisms, and the role of Au single-atom. Graphene involving prominent physical and chemical properties was selected as a model supporter. The single-atom support graphene materials exhibit better CO oxidation activities than pristine graphene, among which CO oxidation property on Au/GP is the highest with a 0.38 eV rate-determining barrier following ER mechanism. The outstanding performances including excellent electronic structures, adsorption properties, and strong activation of intermediate products contribute to the high CO oxidation activity of Au/GP, and the Au single-atom is the active center. Our work provides a novel guide for single-atom catalytic CO oxidation, accelerating the development of single-atom catalysis.
Effective norfloxacin elimination via photo-Fenton process over the MIL-101(Fe)-NH2 immobilized on α-Al2O3 sheet
Qian Zhao , Chong-Chen Wang , Peng Wang
2022, 33(11): 4828-4833  doi: 10.1016/j.cclet.2022.01.033
[Abstract](41) [FullText HTML] [PDF 1900KB](0)
MIL-101(Fe)-NH2@Al2O3 (MA) catalysts were successfully synthesized by reactive seeding (RS) method on α-Al2O3 substrate, which demonstrated excellent photo-Fenton degradation performance toward fluoroquinolone antibiotics (i.e., norfloxacin, ciprofloxacin, and enrofloxacin). The structure and morphology of the obtained MA were characterized by transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), atomic force microscope (AFM). The as-prepared MA could accomplish > 90% of norfloxacin degradation efficiency for 10 cycles' photo-Fenton processes, owing to its excellent chemical and water stability. In addition, the effects of operational factors including H2O2 concentration, foreign ions, and pH on the photo-Fenton degradation of norfloxacin over MA were clarified. The ESR spectra further document that O2, 1O2 and OH radicals are prominent in the decomposition process of antibiotic molecules. Finally, the plausible photo-Fenton norfloxacin degradation mechanisms were proposed and verified.
A general method for one-step synthesis of monofluoroiodane(Ⅲ) reagents using silver difluoride
Jing Ren , Meng-Cheng Jia , Feng-Huan Du , Chi Zhang
2022, 33(11): 4834-4837  doi: 10.1016/j.cclet.2022.01.070
[Abstract](41) [FullText HTML] [PDF 3169KB](0)
Herein we report a new general method for one-step synthesis of four kinds of fluoroiodane(Ⅲ) reagents by treating the corresponding aryl iodides with silver difluoride (AgF2). This is the first method applicable for the synthesis of all four fluoroiodane(Ⅲ) reagents including p-iodotoluene difluoride (1), fluoro-benziodoxole (2), fluoro-benziodoxolone (3), and fluoro-N-acetylbenziodazole (4). AgF2 was firstly employed in the direct oxidative fluorination of iodobenzene and thus has shown its outstanding oxidation and fluorine-transfer ability. The use of AgF2 has improved the synthesis of fluoroiodane(Ⅲ) reagents by shortening the reaction steps, avoiding the use of hazardous reagents, and simplifying the experimental operations. It was worth noting that we have developed the first one-step direct synthetic method for 3, while 3 can only be synthesized through Cl→F ligand exchange reaction previously.
A cationic amphiphilic tetraphenylethylene derivative with hydrochromic sensitive property: Applications in anti-counterfeiting ink and rewritable paper
Qian Xu , Ziyu Qin , Yiling Bei , Shengyu Feng , Xing-Dong Xu
2022, 33(11): 4838-4841  doi: 10.1016/j.cclet.2022.01.079
[Abstract](35) [FullText HTML] [PDF 4808KB](1)
Since the discovery of aggregation induced emission (AIE) phenomenon, various stimuli-responsive materials have been rapidly developed, but there are still great challenges in the application of ink printing due to the bad water solubility. In this research, a new cationic amphiphilic TPE-functionalized pyridine salt (TPE-OTs) was designed, which shows good water solubility and hydrochromic properties. The optical properties of the compound have been studied, which is equipped with the typical AIEE characteristics and TICT effect. The compound can self-assemble to form aggregates with a particle size of about 30 nm in water. What is more, the compound is responsive to the environmental humidity, whose fluorescent color changes from green to yellow as the humidity gradually increased. Based on this characteristic, we applied it to the fluorescent anti-counterfeiting ink, realizing the protection and encryption of information.
Iron-catalyzed hydroaminocarbonylation of alkynes: Selective and efficient synthesis of primary α, β-unsaturated amides
Zijun Huang , Jia Tang , Xiongwei Jiang , Tianle Xie , Minmin Zhang , Donghui Lan , Shaofeng Pi , Zhengde Tan , Bing Yi , Yuehui Li
2022, 33(11): 4842-4845  doi: 10.1016/j.cclet.2022.01.080
[Abstract](40) [FullText HTML] [PDF 1244KB](1)
α, β-Unsaturated primary amides are important intermediates and building blocks in organic synthesis. Herein, we report a ligand-free iron-catalyzed hydroaminocarbonylation of alkynes using NH4HCO3 as the ammonia source, enabling the highly efficient and regioselective synthesis of linear α, β-unsaturated primary amides. Various aromatic and aliphatic alkynes are transformed into the desired linear α, β-unsaturated primary amides in good to excellent yields. Further studies show that using NH4HCO3 as the ammonia source is key to obtain good yields and selectivity. The utility of this route is demonstrated with the synthesis of linear α, β-unsaturated amides including vanilloid receptor-1 antagonist TRPV-1.
Polymerization of pyrrole induced by pillar[5]arene functionalized graphene for supercapacitor electrode
Fang Guo , Junqiang Guo , Zhiqiang Zheng , Tao Xia , Aadil Nabi Chishti , Liwei Lin , Wang Zhang , Guowang Diao
2022, 33(11): 4846-4849  doi: 10.1016/j.cclet.2022.01.088
[Abstract](36) [FullText HTML] [PDF 2178KB](0)
Conducting polymer is an important electrode material for supercapacitors because of its high initial specific capacitance. Herein, a novel nanocomposite composed of polypyrrole (PPy) film homogeneously immobilized on the pillar[5]arene functionalized reduced graphene oxide nanosheets (RGO-HP5A-PPy) was successfully prepared. RGO-HP5A induced pyrrole to polymerize on the graphene surface and the specific capacitance loss caused by PPy agglomeration was avoided. Noticeably, the specific capacitance of RGO-HP5A-PPy was up to 495 F/g at 1 A/g. Compared with pure PPy (319 F/g), the specific capacitance was increased by 55%. The specific capacitance retention of the assembled symmetric supercapacitor reached 76% after 10,000 cycles at 5 A/g. This study gave full play to the advantages of pillar[5]arene, graphene and PPy, and was expected to promote the development of supramolecular functionalized composites in energy storage.
Palladium-catalyzed base- and solvent-controlled chemoselective allylation of amino acids with allylic carbonates
Yang Zhou , Hang Chen , Panpan Lei , Chunming Gui , Haifeng Wang , Qiongjiao Yan , Wei Wang , Fener Chen
2022, 33(11): 4850-4855  doi: 10.1016/j.cclet.2022.02.029
[Abstract](41) [FullText HTML] [PDF 3627KB](0)
The utilization of readily available amino acids, which is not only an oxygen nucleophile but also a nitrogen nucleophile, in palladium-catalyzed allylic substitution is realized under mild conditions. The chemoselectivity and multiple allylation are controlled by adjusting the reaction conditions. This represents the first example of this convenient access to valuable N,O-diallylated amino acids. Under the title conditions, a range of amino acids (α-, β-, γ-) and dipeptides can be readily converted in to the corresponding allylic products with excellent yields (67 examples, up to 99% yield) as well as good functional group tolerance.
Dimensionally confined nanosheets self-assembled through self-shielding multiple hydrogen bonding interactions in aqueous media
Jing Zhang , Shuaiwei Qi , Hao Yu , Ze Lin , Bao Li , Ming Wang , Zeyuan Dong
2022, 33(11): 4856-4859  doi: 10.1016/j.cclet.2022.02.023
[Abstract](32) [FullText HTML] [PDF 3085KB](0)
Herein, we adopt a simple supramolecular strategy to effectively control the tautomerism of ureidopyrimidinone (UPy) moiety and ultimately realize the complete arrangement of enol configuration. The obtained UPy derivatives containing self-complementary quadruple hydrogen bonding interactions can spontaneously self-assemble towards the formation of well-controlled, self-organized supramolecular nanostructure morphologies in both chloroform and water. The resulting aggregates had been fully characterized by various spectroscopy (absorption, emission) and microscopy (TEM, SEM and AFM) studies. It is anticipated that this study can provide an exact and excellent monomeric unit for controllable and precise supramolecular polymerization. The results achieved here also demonstrate the utility and feasibility of multiple hydrogen bonds to direct the self-assembly of small-molecule building blocks in aqueous media, which provides a strategy for the construction of well-defined and stable supramolecular architectures with chemical functionalities and physical properties as advanced materials for biological applications.
Generation of sulfonylureas under photoredox catalysis and their biological evaluations
Xuefeng Wang , Jun Zhang , Qi Chen , Wei Zhou , Jie Wu
2022, 33(11): 4860-4864  doi: 10.1016/j.cclet.2022.02.025
[Abstract](36) [FullText HTML] [PDF 4111KB](0)
Traditional synthesis of sulfonylureas largely depends on nucleophilic addition of arylsulfonamides to pre-synthesized isocyanates. Now we report a new access to alkylsulfonylureas with good yields and broad substrate scope. With the insertion of commercialized chlorosulfonyl isocyanate under photoredox catalysis, alkylsulfonylureas are synthesized in one-pot from the corresponding anilines and silyl enolates. A reaction mechanism is proposed showing the transformation undergoes a radical process, and the practicality of this methodology is proven via application to bioactive molecules. Additionally, the anti-cancer and anti-virus screening of these compounds is evaluated.
Iridium(Ⅰ)-catalyzed deoxgenation of fluoroalkylsulfoxides with dimethyl diazomalonate to access fluoroalkylthioethers
Wenqing Lu , Wenlin Li , Yicheng Zhou , Yongbin Xie , Wenbo Chen
2022, 33(11): 4865-4869  doi: 10.1016/j.cclet.2022.02.061
[Abstract](37) [FullText HTML] [PDF 1709KB](0)
A new method for the preparation of fluoroalkylthioethers including trifluoromethylthioether and difluoromethylthioether by iridium(Ⅰ)-catalyzed deoxgenation of fluoroalkylsulfoxides with dimethyl diazomalonate was developed. In the reaction system, dimethyl diazomalonate was used as reducing reagent and the corresponding fluoroalkylthioethers were produced through oxygen atom transfer from fluoroalkylsulfoxides to diazomalonate. The protocol featuring effective oxygen atom transfer, mild reaction conditions and good functional groups tolerance offers an alternative strategy for the synthesis of fluoroalkylthioethers.
Palladium-catalyzed cyclization of 1-alkynyl-8-iodonaphthalene and double isocyanides for the synthesis of acenaphtho[1,2-b]pyrroles
Shangfeng Ren , Keke Huang , Jin-Biao Liu , Lianpeng Zhang , Min Hou , Guanyinsheng Qiu
2022, 33(11): 4870-4873  doi: 10.1016/j.cclet.2022.02.028
[Abstract](33) [FullText HTML] [PDF 990KB](0)
A palladium-catalyzed formal [2 + 2 + 1] cyclization of 1-alkynyl-8-iodonaphthalene with double isocyanides is developed herein. The transformation worked well to produce a series of 7H-acenaphtho[1,2-b]pyrrole with a broad reaction scope. Isocyanides play a dual role in the reaction. One is a C1 building block, and another is used as C1N1 component. In the process, the [2 + 2 + 1] cyclization involves imidoylation, regioselective addition of imidoylpalladium species into alkyne, double imidoylation, and another addition of the resulting imidoylpalladium species into imine bonds.
Cross-coupling of 2-methylquinolines and in-situ activated isoquinolines: Construction of 1,2-disubstituted isoquinolinones
Jianyi Shi , Zheng Zeng , Shengting Xu , Zechun Cai , Yuehua Luo , Yongbo Fan , Zhongzhi Zhu , Tingting Wen , Xiuwen Chen
2022, 33(11): 4874-4877  doi: 10.1016/j.cclet.2022.02.032
[Abstract](31) [FullText HTML] [PDF 4153KB](0)
In this study, a method was developed to form C(sp3)–C(sp2) bonds via copper catalyst-promoted cross coupling of 2-methylquinoline and in-situ-activated 3-haloisoquinoline under mild conditions. The multi-component tandem reaction was used to construct new C–N, C=O and C–C bonds in one pot via sequential functionalization of the N1, C3 and C1 positions of 3-haloisoquinoline. This method can be used to efficiently access 1,2-disubstituted isoquinolinones by the three-component reaction of 3-halogen isoquinoline, alkyl halide, and 2-methylquinoline.
Catalytic and highly stereoselective β-mannopyranosylation using a 2,6-lactone-bridged mannopyranosyl ortho-hexynylbenzoate as donor
Yingle Feng , Jie Yang , Chenglin Cai , Taotao Sun , Qi Zhang , Yonghai Chai
2022, 33(11): 4878-4881  doi: 10.1016/j.cclet.2022.02.071
[Abstract](30) [FullText HTML] [PDF 3173KB](0)
An efficient and catalytic protocol for highly stereoselective construction of β-mannopyranosylation has been developed. Glycosylation of 2,6-lactone-bridged mannopyranosyl ortho-hexynylbenzoate with various acceptors proceeded smoothly in the presence of 5% Hg(Ⅱ) at room temperature, resulting in the corresponding β-mannosides in high yield and exclusive β-stereoselectivity.
MUC1 vaccines using β-cyclodextrin grafted chitosan (CS-g-CD) as carrier via host-guest interaction elicit robust immune responses
Hangyan Yu , Han Lin , Yuntian Xie , Mengyuan Qu , Min Jiang , Jie Shi , Haofei Hong , Hongrui Xu , Ling Li , Guochao Liao , Zhimeng Wu , Zhifang Zhou
2022, 33(11): 4882-4885  doi: 10.1016/j.cclet.2022.02.072
[Abstract](31) [FullText HTML] [PDF 1925KB](0)
We construct MUC1 vaccines using β-cyclodextrin grafted chitosan (CS-g-CD) as carrier via host-guest interaction. These vaccines based on non-covalent assembling can provoke robust immune responses, including high level of specific antibodies and cytokines. The induced antibodies can specifically recognize tumor cells and mediate cytotoxicity against tumor cells. These results indicate that CS-g-CD with strong immunostimulatory activities can be a straightforward platform for peptide-based vaccine construction.
Visible-light-irradiated tandem sulfonylation/cyclization of indole tethered alkenes for the synthesis of tetrahydrocarbazoles
Yingjie Yu , Aiyao Liu , Jingrui He , Chengting Wang , Haibo Mei , Jianlin Han
2022, 33(11): 4886-4890  doi: 10.1016/j.cclet.2022.03.038
[Abstract](32) [FullText HTML] [PDF 1262KB](2)
A visible-light-mediated reaction of indole derivatives employing arylsulfonyl chlorides as sulfonyl surrogates has been developed, which proceeds via the sequence of reduction of sulfonyl chloride, sulfonylation, and intramolecular cyclization. This mild protocol transforms a diverse array of indole tethered alkenes and simple sulfonyl chlorides into highly valuable functionalized tetrahydrocarbazoles in good yields. This reaction is also suitable for gram-scale synthesis, which provides an efficient and green access to multi-substituted tetrahydrocarbazoles.
CuBr-promoted domino Biginelli reaction for the diastereoselective synthesis of bridged polyheterocycles: Mechanism studies and in vitro anti-tumor activities
Mengting Zeng , Ying Xue , Yunan Qin , Fen Peng , Quan Li , Ming-Hua Zeng
2022, 33(11): 4891-4895  doi: 10.1016/j.cclet.2022.02.075
[Abstract](35) [FullText HTML] [PDF 2391KB](0)
The low-cost CuBr-promoted domino Biginelli reaction among readily available ketones, salicylaldehyde derivatives and 3-amino-1, 2, 4-triazole was studied under solvothermal conditions, giving the novel bridged polyheterocycles bearing two or three stereocenters depending on the starting ketones. This multicomponent reaction proceeded with high diastereoselectivity (dr > 20:1) based on a combined 1H NMR, crystallographic and supercritical fluid chromatographic (SFC) analysis of the product. Time-dependent high-resolution mass spectrometry (HRMS) was performed to track the reaction process, and several key intermediates were identified, leading to the drawing of a plausible reaction mechanism. Density functional theory (DFT) calculation was supplemented, and two reaction pathways were differentiated. Moreover, in vitro antitumor activity was evaluated using HeLa and HepG2 cell lines, and two of these polyheterocycles demonstrated promising activities against HepG2 cells with EC50 down to 10 µmol/L. Additionally, ESI-MS/MS studies on all the polyheterocycles suggest a common fragmentation pathway (loss of one molecule of amino-triazole) they shared, providing the first-hand fragmentation rules for future rapid structural identification of them. The multicomponent domino reaction presented here may offer prospects for future design of more efficient strategies to access medicinally important bridged polyheterocycles.
Selective recognition of methyl viologen by an endo-functionalized naphthobox
Weier Liu , Linghui Kong , Mao Quan , Huan Yao , Liupan Yang , Ho Yu Au-Yeung , Wei Jiang
2022, 33(11): 4896-4899  doi: 10.1016/j.cclet.2022.02.076
[Abstract](32) [FullText HTML] [PDF 2682KB](1)
Highly selective binding of structurally similar substrates is common for biomolecular recognition, but is often challenging to realize in synthetic hosts. Herein, we report highly selective binding of methyl viologen over other analogues by an endo-functionalized naphthobox. X-ray single crystal structure and Density Functional Theory (DFT) calculations revealed that the endo-functionalized groups in the cavity of the naphthobox is important for the high binding selectivity through the formation of multiple C–H…N, C–H…π, and ππ interactions with methyl viologen.
Simultaneous enhancement of phosphorescence and chirality by host–guest recognition of molecular tweezers
Diankun Jia , Hua Zhong , Sixun Jiang , Risheng Yao , Feng Wang
2022, 33(11): 4900-4903  doi: 10.1016/j.cclet.2022.02.081
[Abstract](36) [FullText HTML] [PDF 2167KB](0)
A novel type of host–guest recognition systems have been developed on the basis of a Au(Ⅲ) molecular tweezer receptor and chiral Pt(Ⅱ) guests. The complementary host–guest motifs display high non-covalent binding affinity (Ka: ~104 L/mol) due to the participation of two-fold intermolecular π–π stacking interactions. Both phosphorescence and chirality signals of the Pt(Ⅱ) guests strengthen in the resulting host–guest complexes, because of the cooperative rigidifying and shielding effects rendered by the tweezer receptor. Their intensities can be reversibly switched toward pH changes, by taking advantage of the electronic repulsion effect between the protonated form of tweezer receptor and the positive-charged guests in acidic environments. Overall, the current study demonstrates the feasibility to enhance and modulate phosphorescence and chirality signals simultaneously via molecular tweezer-based host–guest recognition.
Optically probing molecular shuttling motion of [2]rotaxane by a conformation-adaptive fluorophore
Chengyuan Yu , Xiaodong Wang , Cai-Xin Zhao , Shun Yang , Jiaan Gan , Zhuo Wang , Zhanqi Cao , Da-Hui Qu
2022, 33(11): 4904-4907  doi: 10.1016/j.cclet.2022.03.004
[Abstract](35) [FullText HTML] [PDF 2288KB](0)
A bistable [2]rotaxane with a conformation-adaptive macrocycle bearing a 9, 14-diphenyl-9, 14-dihydrodibenzo[a, c]phenazine (DPAC) unit was synthesized, which could be utilized to optical probe the molecular shuttling motion of the functionalized rotaxane system. The UV–vis, 1H NMR and PL spectroscopic data clearly demonstrated that the DPAC ring was interlocked onto the thread and the fluorescence intensity of the DPAC unit in the macrocycle was effectively regulated by the location change of the macrocycle along the thread under acid/base stimulation, which was attributed to the modulation of the intramolecular photo-induced electron transfer between the DPAC unit and the methyltriazole (MTA) unit. This bistable rotaxane system containing a conformation-adaptive fluorophore unit in the macrocycle moiety opens an alternative way to design functional bistable mechanically interlocked molecules.
Metal coordination to a deep cavitand promotes binding selectivities in water
Yong-Qing Chen , Hua-Wei Guan , Kuppusamy Kanagaraj , Julius Rebek , Yang Yu
2022, 33(11): 4908-4911  doi: 10.1016/j.cclet.2022.03.039
[Abstract](40) [FullText HTML] [PDF 2258KB](1)
One goal of supramolecular chemistry is the creation of synthetic receptors that have a high affinity for hydrophilic molecules in water. We found that cavitands with upper rims extended by pyridyl groups coax hydrophilic guests into the cavity where they are shielded from the aqueous environment. The ability of Pd(Ⅱ) to coordinate adjacent pyridyl groups leads to increased selectivity for highly hydrophilic solvent molecules such as acetone, 1, 4-dioxane and tetrahydrofuran in water. Analysis of the binding behavior indicated that metal-coordination restricts the container entrance, shrinks the effective cavity volume and increases the energetic barrier to guest exchange.
A bio-based epoxy resin derived from p-hydroxycinnamic acid with high mechanical properties and flame retardancy
Xin Song , Ze-Peng Deng , Chun-Bo Li , Fei Song , Xiu-Li Wang , Li Chen , De-Ming Guo , Yu-Zhong Wang
2022, 33(11): 4912-4917  doi: 10.1016/j.cclet.2021.12.067
[Abstract](35) [FullText HTML] [PDF 6091KB](1)
Recent advances in epoxy resins have been forward to achieving high mechanical performance, thermal stability, and flame retardancy. However, seeking sustainable bio-based epoxy precursors and avoiding introduction of additional flame-retardant agents are still of increasing demand. Here we report the synthesis of p-hydroxycinnamic acid-derived epoxy monomer (HCA-EP) via a simple one-step reaction, and the HCA-EP can be cured with 4, 4′-diaminodiphenylmethane (DDM) to prepare epoxy resins. Compared with the typical petroleum-based epoxy resin, bisphenol A epoxy resin, the HCA-EP-DDM shows a relatively high glass transition temperature (192.9 ℃) and impressive mechanical properties (tensile strength of 98.3 MPa and flexural strength of 158.9 MPa). Furthermore, the HCA-EP-DDM passes the V-1 flammability rating in UL-94 test and presents the limiting oxygen index of 32.6%. Notably, its char yield is as high as 31.6% under N2, and the peak heat rate release is 60% lower than that of bisphenol A epoxy resin. Such findings provide a simple way of using p-hydroxycinnamic acid instead of bisphenol A to construct high-performance bio-based thermosets.
Fmoc-protected amino acids as luminescent and circularly polarized luminescence materials based on charge transfer interaction
Yiran Xia , Aiyou Hao , Pengyao Xing
2022, 33(11): 4918-4923  doi: 10.1016/j.cclet.2022.02.077
[Abstract](35) [FullText HTML] [PDF 6524KB](0)
Fluorenylmethyloxycarbonyl (Fmoc)-protected amino acids are effective building blocks in self-assembled architectures at hierarchical levels, which however show limited luminescent properties and chiroptical activities. Here we introduce a charge-transfer strategy to build two-component luminescent materials with emerged circularly polarized luminescence properties. A library of Fmoc-amino acids was built, which selectively form charge-transfer complexes with the electron-deficient acceptor. Embedding in amorphous polymer matrix or physical grinding could trigger the charge-transfer luminescence with adjusted wavelengths in a general manner. X-ray diffraction results suggest the multiple binding modes between donor and acceptor. And, the solution-processed coassembly could selectively exhibit circularly polarized luminescence with high dissymmetry g-factors. This work illustrates a noncovalent charge-transfer strategy to construct luminescent and chiroptical organic composites based on the easy-accessible and economic chiral N-terminal aromatic amino acids.
Oral colon-targeted mucoadhesive micelles with enzyme-responsive controlled release of curcumin for ulcerative colitis therapy
Chen Zhang , Jiaxin Li , Meng Xiao , Di Wang , Yan Qu , Liang Zou , Chuan Zheng , Jinming Zhang
2022, 33(11): 4924-4929  doi: 10.1016/j.cclet.2022.03.110
[Abstract](32) [FullText HTML] [PDF 6137KB](0)
Although multitudinous nanoscale drug-delivery systems (DDSs) have been recommended to improve anti-ulcerative colitis (UC) outcomes, to enhance the mucoadhesion of nanosystems on the colon and specifically release the loaded drugs in response to the colon micro-environment would be critical factors. The application of curcumin (Cur), an acknowledged anti-UC phytochemical compound, for UC therapy requires more efficient nano-carriers to improve its therapeutic outcome. Herein, we developed the colon-targeted nano-micelles with mucoadhesive effect and Azo reductase-triggered drug release profiles for Cur delivery in UC treatment. Specifically, the amphiphilic block polymer containing the Azo-reductase sensitive linkage (PEG-Azo-PLGA), and catechol-modified TPGS (Cat-TPGS) were synthesized respectively. Based on the self-assembly of the mixed polymers, Cur-micelles (142.7 ± 1.7 nm of average size, 72.36% ± 1.54% of DEE) were obtained. Interestingly, the Cur-micelles exhibited the Azo-reductase sensitive particle dissociation and drug release, the enhanced cellular uptake and the prolonged retention on colonic mucosa, mediated by the strong mucoadhesion of catechol structure. Ultimately, Cur-micelles significantly mitigated colitis symptoms and accelerated colitis repair in DSS-treated mice by regulating the intestinal flora and the levels of pro-inflammatory factors (MPO, IL-6, IL-1β, and TNF-α) related to TLR4/MyD88/NF-κB signaling pathway. This work provides an effective drug delivery strategy for anti-UC drugs by oral administration.
Ruthenium-modified porous NiCo2O4 nanosheets boost overall water splitting in alkaline solution
Rui Yang , Xuezhao Shi , Yanyan Wang , Jing Jin , Hanwen Liu , Jie Yin , Yong-Qing Zhao , Pinxian Xi
2022, 33(11): 4930-4935  doi: 10.1016/j.cclet.2021.12.058
[Abstract](37) [FullText HTML] [PDF 4924KB](0)
Exploring efficient oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) electrocatalysts is crucial for developing water splitting devices. The composition and structure of catalysts are of great importance for catalytic performance. In this work, a heterogeneous Ru modified strategy is engineered to improve the catalytic performance of porous NiCo2O4 nanosheets (NSs). Profiting from favorable elements composition and optimized structure property of decreased charge transfer barrier, more accessible active sites and increased oxygen vacancy concentration, the Ru-NiCo2O4 NSs exhibits excellent OER activity with a low overpotential of 230 mV to reach the current density of 10 mA/cm2 and decent durability. Furthermore, Ru-NiCo2O4 NSs show superior HER activity than the pristine NiCo2O4 NSs, as well. When assembling Ru-NiCo2O4 NSs couple as an alkaline water electrolyzer, a cell voltage of 1.60 V can deliver the current density of 10 mA/cm2. This work provides feasible guidance for improving the catalytic performance of spinel-based oxides.
Toward accurate and efficient dynamic computational strategy for heterogeneous catalysis: Temperature-dependent thermodynamics and kinetics for the chemisorbed on-surface CO
Jun Chen , Tan Jin , Yihuang Jiang , Tonghao Shen , Mingjun Yang , Zhe-Ning Chen
2022, 33(11): 4936-4942  doi: 10.1016/j.cclet.2022.03.080
[Abstract](36) [FullText HTML] [PDF 2353KB](2)
Computational tools on top of first principle calculations have played an indispensable role in revealing the molecular details, thermodynamics, and kinetics in catalytic reactions. Here we proposed a highly efficient dynamic strategy for the calculation of thermodynamic and kinetic properties in heterogeneous catalysis on the basis of efficient potential energy surface (PES) and MD simulations. Taking CO adsorbate on Ru(0001) surface as the illustrative model system, we demonstrated the PES-based MD can efficiently generate reliable two-dimensional potential-of-mean-force (PMF) surfaces in a wide range of temperatures, and thus temperature-dependent thermodynamic properties can be obtained in a comprehensive investigation on the whole PMF surface. Moreover, MD offers an effective way to describe the surface kinetics such as adsorbate on-surface movement, which goes beyond the most popular static approach based on free energy barrier and transition state theory (TST). We further revealed that the dynamic strategy significantly improves the predictions of both thermodynamic and kinetic properties as compared to the popular ideal statistic mechanics approaches such as harmonic analysis and TST. It is expected that this accurate yet efficient dynamic strategy can be powerful in understanding mechanisms and reactivity of a catalytic surface system, and further guides the rational design of heterogeneous catalysts.
A TICS-fluorophore based probe for dual-color GSH imaging
Wenjuan Liu , Jie Chen , Qinglong Qiao , Xiaogang Liu , Zhaochao Xu
2022, 33(11): 4943-4947  doi: 10.1016/j.cclet.2022.03.121
[Abstract](41) [FullText HTML] [PDF 4267KB](2)
Cascading reactions in fluorophores accompanied by the replacement of different fluorescence wavelengths can be used to develop luminescent materials and reactive fluorescent probes. Based on multiple signal channels, the selectivity of probes can be improved and the range of response to guest molecule recognition can be expanded. By regulating the position, number, and activity of active sites in fluorophores, fluorescent probes that successively react with thiol and amino groups in cysteine (Cys), homocysteine (Hcy) have been developed, which can only react with the thiol group of GSH. In this paper, we report the first probe capable of cascading nucleophilic substitution reaction with the thiol group and amino group of GSH at a single reaction site, and showed the dual-color recognition of GSH, which improved the selectivity of GSH also was an extension of GSH probes. The probe Rho-DEA was based on a TICS fluorophore, and the intramolecular cascade nucleophilic substitution reaction occurs with Cys/Hcy. The thiol substitution of the first step reaction with Cys/Hcy was quenched due to intersystem crossing to triplet state, so GSH can be selectively recognized from the fluorescence signal. Rho-DEA has the ability of mitochondrial localization, and finally realized in situ dual-color fluorescence recognition of GSH in mitochondria.
Insight into the in vivo fate of intravenous herpetrione amorphous nanosuspensions by aggregation-caused quenching probes
Lingyu Hang , Chengying Shen , Baode Shen , Hailong Yuan
2022, 33(11): 4948-4951  doi: 10.1016/j.cclet.2022.03.108
[Abstract](31) [FullText HTML] [PDF 3162KB](0)
Intravenous nanosuspensions are attracted growing attention as a viable strategy for development of intravenous formulations of poorly water-soluble drugs. However, only few information about the biological fate of intravenous nanosuspensions is currently known, especially amorphous nanosuspensions are not reported yet. In this study, the in vivo fate of herpetrione (HPE) amorphous nanosuspensions following intravenous administration was explored by using an aggregation-caused quenching (ACQ) probe and HPLC methods. The ACQ probe is physically embedded into HPE nanoparticles via anti-solvent method to form HPE hybrid nanosuspensions (HPE-HNSs) for bioimaging. HPE-HNSs emit strong and stable fluorescence, but fluorescence quenches immediately upon the dissolution of HPE-HNSs, confirming the self-discrimination of HPE-HNSs. Following intravenous administration of HPE-HNSs, integral HPE-HNSs and HPE show similar degradation and biodistribution, with rapid clearance from blood circulation and obvious accumulation in liver and lung. Due to the slower dissolution and enhanced recognition by reticulo-endothelial system, 450 nm HPE-HNSs accumulate more in liver, lung and spleen than that of 200 nm HPE-HNSs. These results demonstrate that integral HPE-HNSs determine the in vivo performance of HPE-HNSs. This study provides insight into the in vivo fate of intravenous amorphous nanosuspensions.
Distinct structural characteristics define a new subfamily of Mycoplasma ferritin
Wenming Wang , Xiaojia Liu , Yajie Wang , Yuan Wang , Dan Fu , Hongfang Xi , Yi Zhao , Hongfei Wang
2022, 33(11): 4952-4955  doi: 10.1016/j.cclet.2022.03.119
[Abstract](40) [FullText HTML] [PDF 2815KB](1)
Ferritins can generally be divided into four subfamilies based on their structural characteristics, namely, the classic ferritins (Ftns), bacterioferritins (Bfrs), DNA-binding proteins from starved cells (Dps'), and encapsulated ferritins (EncFtns). However, the ferritin from Mycoplasma penetrans (Mpef) possesses a particular ferroxidase center with an extreme low activity and exhibits unusual characteristics, indicating that it could be a member of a quite different subfamily of ferritins. Hereby, the crystal structure of the ferritin from Ureaplasma urealyticum (Uurf) is presented, Mpef and Uurf have very similar properties, though they display very low sequence similarity. Thus, ferritins from Mycoplasma with these unique properties do not belong to any known subfamily, but they should rather be placed in a novel ferritin subfamily, which we term Mycoplasma Ferritin (Mfr).
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