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Integrating Bimetallic Nanoparticles with Covalent organic Frameworks as Multifunctional Nanozyme for Colorimetric Detection of Hydrogen Peroxide and Glutathione

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Journal of Analysis and Testing 2024年第3期8卷 278-287页

作者： Yuying Yuan Xiaoxue Xi Ting Bao Pingguan Bian Feng Pei Xiuhua Zhang Shengfu Wang Wei Wen Collaborative Innovation Center for Advanced organic chemical Materials Co-constructed by the Province and Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional MoleculesCollege of Chemistry and Chemical EngineeringHubei University Hubei Yihua chemical Co. Ltd

The controllable growth of metal nanoparticles on nanomaterials is becoming an effective strategy for developing nanocomposites with designated performance. Herein, a simple and mild strategy for the in situ growth of Pt–Pd bimetallic nanoparticles on covalent organic frameworks（COFs） to regulate the nanozyme activity was designed for colorimetric detection of hydrogen peroxide（H2O2） and glutathione（GSH）. The COFs not only offer sufficient loading sites for the uniform dispersion of Pt–Pd bimetallic nanoparticles, but also increase the adsorption of substrate to promote the catalytic reaction. With the bimetallic synergistic effect of Pt–Pd nanoparticles, the prepared multifunctional nanozyme（Pt–Pd/COFs nanozyme） simultaneously exhibited superior peroxidase（POD）-like activity and oxidase（OXD）-like activity. Using the multifunctional nanozyme, a colorimetric sensing system was constructed for sensitive detection of H2O2and GSH, with the wide linear ranges of 5–1000 μmol/L and 1–40 μmol/L, and the detection limits were 1.14 μmol/L and 0.43 μmol/L, respectively. It was successfully used for the detection of real samples in environmental water and serum, providing a simple method for disease diagnosis and environmental monitoring.

关键词： Bimetallic synergistic effect H2O2 and GSH detection Oxidase-like activity Peroxidase-like activity Pt–Pd/COFs nanozyme

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Copper Catalyzed Enantioconvergent Nucleophilic Substitutions

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Chinese Journal of chemistry 2024年第10期42卷 1161-1174页

作者： Chunxi Huang Zilong Wan Aoping Zhu Caiyou Chen College of chemistry and Molecular Sciences Wuhan UniversityWuhanHubei 430072China ministry of education key laboratory for the synthesis and application of organic functional molecules and College of chemistry and chemical engineering Hubei UniversityWuhanHubei 430062China

As a versatile earth-abundant transition metal,Cu has long been widely applied in the C—C and C—X bond forming *** for now,low-valent Cu(Ⅰ)is known to reduce the redox active electrophiles via an SET pathway to give the corresponding radical and Cu(Ⅱ)*** resulting Cu(Ⅱ)species can interact with the radical via the out-sphere pathway,affording the coupling ***,Cu(Ⅱ)can trap the radical through the inner-sphere process to generate Cu(Ⅲ)species and then realize challenging bond formations due to the facile reductive elimination of Cu(Ⅲ)*** copper catalysis has been widely applied in arylations of various nucleophiles,copper-catalyzed enantioconvergent nucleophilic substitutions of racemic alkyl electrophiles have been less explored,likely due to the difficulties in overcoming the reduction potential of alkyl electrophiles,elimination of side reactions,and enantiomeric *** order to overcome the high reduction potential of alkyl electrophiles,the photo-induced strategy has been developed under mild *** alternative strategy with new anionic tridentate ligands has also been reported in this *** review summarizes recent developments in copper-catalyzed enantioconvergent nucleophilic substitutions of alkyl electrophiles by various nucleophiles to realize C—N,C—C,C—B,C—P and C—O bond formations and their brief mechanistic studies.

关键词： Enantioconvergent Nucleophilic substitution Copper Radical reactions Photocatalysis Asymmetric catalysis

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Metal-Free synthesis of 2-Aminobenzothiazoles via I2-Catalyzed Tandem Cyclization Reaction of Amines and Carbon Disulfide

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Chinese Journal of chemistry 2024年第8期42卷 846-852页

作者： Ting Chen Wei Feng Ruitong Yang Shanping Chen Guo-Jun Deng key laboratory for Green organic synthesis and application of Hunan Province Key Laboratory of Environmentally Friendly Chemistry and Application of Ministry of EducationCollege of ChemistryXiangtan UniversityXiangtanHunan411105 China school of chemistry and chemical engineering Henan Normal UniversityXinxiangHunan453007 China

Comprehensive Summary,A convenient approach for the construction of 2-aminobenzothiazoles via I2-catalyzed tandem cyclization reaction of amines and carbon disulfide has been *** present approach starts from simple and readily available starting materials,affording a series of 2-aminobenzothiazoles in up to 89%yields under metal-free *** this work,C—H/N—H functionalization was achieved and multiple C-hetero bonds were successfully constructed in one pot.

关键词： Sulfur heterocycles C-H functionalization Cyclization Tandem reaction Transition-metal-free Amines lodine N-Heterocycles

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Transition-metal free trifluoromethylimination of alkenes enabled by direct activation of N-unprotected ketimines

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Chinese chemical Letters 2024年第9期35卷 155-159页

作者： Boqiang Wang Yongzhuo Xu Jiajia Wang Muyang Yang Guo-Jun Deng Wen Shao key laboratory for Green organic synthesis and application of Hunan Province Key Laboratory of Environmentally Friendly Chemistry and Application of Ministry of EducationCollege of ChemistryXiangtan UniversityXiangtan 411105China Department school of chemistry and chemical engineering Henan Normal UniversityXinxiang 453007China

A highly site-selective intermolecular trifluoromethylimination of activated and unactivated olefins was reported under transition-metal-and photosensitizer-free *** newly developed strategy provides straightforward and efficient access to diverse value-added vicinal trifluoromethyl amines without resorting to the pre-functionalized *** experiments demonstrate that the approach proceeded through CF_(3)and iminyl two-radicals process,which were generated directly from commercially available benzophenone imine in a novel electron-donor mode via a SET process activated by the bifunctional hypervalent iodine *** synthetic potential of the protocols was further showcased via the condensation/amination sequential cascade,and transformations to accessβ-CF_(3)primary amines.

关键词： Transition-metal free Alkenes difunctionalization Amination Trifluoromethylation Single-electron transfer

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Green synthesis of luminescent La-MOF nanoparticle from waste poly(ethylene terephthalate) for high-performance in Fe(Ⅲ) detection

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Rare Metals 2024年第8期43卷 3833-3843页

作者： Zhi Gong Zhi-Kui Dai Zhi-Yue Dong Qiu-Xuan Liu Valentin A.Milichko Hua-Jian Liu Jie Liu Ran Niu Jiang Gong key laboratory of Material chemistry for Energy Conversion and Storage Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringMinistry of EducationHuazhong University of Science and TechnologyWuhan 430074China school of chemical engineering and Pharmacy Wuhan Institute of TechnologyWuhan 430073China Collaborative Innovation Center for Advanced organic chemical Materials Co-constructed by the Province and ministry Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules and College of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062China school of Physics and engineering ITMO UniversitySt.Petersburg197101Russia school of Materials Science and engineering Hubei UniversityWuhan430062China Guangdong Provincial key laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing School of Mechanical and Automotive EngineeringKey Laboratory of Polymer Processing EngineeringMinistry of EducationSouth China University of TechnologyGuangzhou 510641China

Developing luminescent metal-organic frameworks(MOFs) capable of high-efficiency Fe^(3+)sensing has aroused great attraction in the fields of biology,chemistry,***,previous solvothermal methods are limited by organic solvent usage,time consuming,high pressure,and high-energy ***,we propose the waste-toMOF strategy towards the scale-up production of La-MOF nanoparticles through the ball milling of recycled poly(-ethylene terephthalate)(PET) bottles and La(NO_(3))_(3)·_(6)H_(2)*** goes on alkaline hydrolysis to form 1,4-benzenedicarboxylic acid sodium salt(Na_(2)BDC) and ethylene glycol by ball ***,BDC reacts with La^(3+)to form *** as-prepared La-MOF crystal nanoparticles possess a rod-like morphology with the size of few hundred ***,La-MOF nanoparticles display high selectivity and sensitivity for Fe^(3+)*** quenching constant and limit of detection are 5.29×10^(3)(mol·L^(-1))^(-1) and 0.147 μmol·L^(-1),respectively,thus surpassing many advanced Fe^(3+) *** to the result of density functional theory,the high Fe^(3+) detection performance of La-MOF is related to the complexing of Fe^(3+)with La-MOF,which leads to the gradual dissociation of the coordination bond between terephthalic acid and La^(3+).It is anticipated that the mechanochemistry milling-based wasteto-MOF strategy provides a new platform for the massive production of functional MOFs in a green manner.

关键词： Metal-organic framework Waste polyester Mechanochemistry milling Fluorescence sensor

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From charge storage mechanism to performance:A strategy toward boosted lithium/sodium storage through heterostructure optimization

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Journal of Energy chemistry 2024年第1期88卷 112-124,I0003页

作者： Xiaoke Zhang Guangfa Deng Mianying Huang Zhaohui Xu Jianlin Huang Xuan Xu Zhiguang Xu Maochan Li Lei Hu Xiaoming Lin key laboratory of Theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina Anhui laboratory of functional Coordinated Complexes for Materials chemistry and application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000AnhuiChina National engineering Research Center for Carbohydrate synthesis Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022JiangxiChina

Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent *** this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and *** optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active ***_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in *** functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical *** heterostructure building technique may pave the way for the development of high-performance LIBs and ***,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.

关键词： Metal-organic framework Heterostructure Lithium-ion batteries Sodium-ion batteries DFT calculation

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具有超高碱性稳定性和尺寸稳定性的聚芳烃N-甲基奎宁基阴离子交换膜

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Science China Materials 2024年第3期67卷 965-973页

作者：文菊贺显颖张干兵曾梦莹钱宇黎明 Collaborative Innovation Center for Advanced organic chemical Materials Co-constructed by the Province and ministry Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional MoleculesHubei Key Laboratory of Polymer MaterialsCollege of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062China

阴离子交换膜水电解槽的阴离子交换膜成本低、无需铂族贵金属催化剂,有望取代高成本的质子交换膜水电解槽.然而,阴离子交换膜的尺寸稳定性差以及在高温、高浓度碱液中的稳定性差,阻碍了阴离子交换膜水电解槽的发展.最近,我们合成了一种... 详细信息

阴离子交换膜水电解槽的阴离子交换膜成本低、无需铂族贵金属催化剂,有望取代高成本的质子交换膜水电解槽.然而,阴离子交换膜的尺寸稳定性差以及在高温、高浓度碱液中的稳定性差,阻碍了阴离子交换膜水电解槽的发展.最近,我们合成了一种具有优异碱性稳定性的聚(三苯基-N-甲基奎宁基)阴离子交换膜,为了进一步提高这种阴离子交换膜的机械强度和尺寸稳定性,在本工作中,我们添加了三氟苯乙酮来制备聚(三苯基-三氟苯乙酮-N-甲基奎宁基)阴离子交换膜.这种共聚阴离子交换膜具有超高的碱性稳定性(在80℃,10 mol L^(-1)的NaOH溶液中浸泡1600小时后OH^(-)电导率和机械强度不发生衰减),优异的尺寸稳定性(30–80℃温度下,纯水中溶胀率不超过7%;10 mol L^(-1)的NaOH溶液中溶胀率不超过2%),高氢氧根电导率(80°C时达134.5 mS cm^(-1))和高机械强度(抗拉伸强度达43.2 MPa).这种阴离子交换膜和镍合金泡沫电极组装的简易水电解槽在80°C下,2.0 V和5 mol L^(-1)的KOH水电解质中具有1780 mA cm^(-2)的优异电流密度,并且具有高耐久性.

关键词： anion exchange membrane N-methylquinuclidinium alkaline stability dimensional stability water electrolyser

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Copper/Photoredox-Catalyzed Regioselective 1,4-Addition to 1,3-Enynes: A Convenient Access to Perfluoroalkylated Allenes

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Chinese Journal of chemistry 2024年第17期42卷 2023-2028页

作者： Ya Chen Quanyuan Wang keyi Peng Lilei Cheng Ziyi She Guo-Jun Deng key laboratory for Green organic synthesis and application of Hunan Province Key Laboratory of EnvironmentallyFriendly Chemistry andApplication of Ministryof EducationCollege of ChemistryXiangtan UniversityXiangtanHunan 411105China Department school of chemistry and chemical engineering Henan Normal UniversityXinxiangHenan 453007China

A general and broadly applicable copper and photoredox dual-catalyzed multicomponent 1,4-perfluoroalkylcyanation of 1,3-enynes has been *** protocol enjoys success with high regioselectivity,mild reaction conditions,and excellent functional-group tolerance,allowing the facile synthesis of structurally diverse perfluoroalkylated allenes from readily available fluoroalkyl halides,1,3-enynes and TMscN in a one-pot manner.A reasonable mechanism has been proposed according to a series of control experiments.

关键词： Fluorinated allenes 1 3-Enynes Photoredox Fluoroalkylation Multicomponent reactions Difunctionalization Radicals Regioselectivity

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Research advancement of DNA-based intelligent hydrogels:Manufacture, characteristics, application of disease diagnosis and treatment

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Chinese chemical Letters 2024年第10期35卷 92-101页

作者： Zhe-Han Yang Jie Yin Lei Xin Yuanfang Li Yijie Huang Ruo Yuan Ying Zhuo Chongqing key laboratory of Catalysis and functional organic molecules College of Environment and ResourcesChongqing Technology and Business UniversityChongqing 400067China key laboratory of Luminescence and Real-Time Analytic chemistry(Southwest University) Ministry of EducationCollege of Chemistry and Chemical EngineeringSouthwest UniversityChongqing 400715China

DNA-based hydrogels are exceptional materials for biological applications because of their numerous advantages such as biodegradability,biocompatibility,hydrophilicity,super absorbency,porosity,and *** these advantages,the ability of DNA-based hydrogels to respond to specific physical and chemical triggers and undergo reversible phase transitions has garnered significant attention in the fields of disease diagnosis(biosensors)and treatment(drug delivery).This article focuses on the recent advancements in the research of DNA-based hydrogels and discusses the different types of these hydrogels,the synthetic methods,their unique properties,and their applications in biosensors and drug *** types of DNA hydrogels are categorized based on their building blocks,and the process of synthesis as well as the unique characteristics of DNA-based hydrogels are ***,DNA-based responsive hydrogels utilized as intelligent materials for the development of biosensors are ***,this article also presents the current status of DNA-based responsive hydrogels in drug delivery for cancer treatment,wound healing,and other therapeutic ***,this paper discusses the current challenges in expanding the practical application of DNA-based hydrogels.

关键词： DNA-based hydrogel Intelligent hydrogel Manufacture Characteristics Diseasediagnosis and treatment

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Bio-soft matter derived from traditional Chinese medicine:Characterizations of hierarchical structure,assembly mechanism,and beyond

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Journal of Pharmaceutical Analysis 2024年第6期14卷 823-839页

作者： Guiya Yang Yue Liu Yuying Hu Yue Yuan Yunan Qin Quan Li Shuangcheng Ma school of Traditional Chinese Medicine Beijing University of Chinese MedicineBeijing102488China Institute for Control of Chinese Traditional Medicine and Ethnic Medicine National Institutes for Food and Drug ControlBeijing100050China Tianjin key laboratory of Therapeutic Substance of Traditional Chinese Medicine School of Chinese Materia MedicaTianjin University of Traditional Chinese MedicineTianjin301617China Collaborative Innovation Center for Advanced organic chemical Materials Co-constructed by the Province and ministry Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional MoleculesCollege of Chemistry and Chemical EngineeringHubei UniversityWuhan430062China

Structural and functional explorations on bio-soft matter such as micelles,vesicles,nanoparticles,aggregates or polymers derived from traditional Chinese medicine(TCM)has emerged as a new topic in the field of *** discovery of such cross-scaled bio-soft matter may provide a unique perspective for unraveling the new effective material basis of TCM as well as developing innovative medicine and *** the rapid rise of TCM-derived bio-soft matter,their hierarchical structure and assembly mechanism must be unambiguously probed for a further in-depth understanding of their pharmacological *** this review,the current emerged TCM-derived bio-soft matter assembled from either small molecules or macromolecules is introduced,and particularly the unambiguous elucidation of their hierarchical structure and assembly mechanism with combined electron microscopic and spectroscopic techniques is *** pros and cons of each technique are also *** future challenges and perspective of TCM-derived bio-soft matter are outlined,particularly the requirement for their precise in situ structural determination is highlighted.

关键词： Electron microscopy Spectroscopy Traditional Chinese medicine Bio-soft matter Structural characterization

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