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Synthesis of Dendronized Polymers via a“m+n”Grafting-onto Strategy with Reaction-Enhanced Reactivity of Intermediates(RERI)Mechanism

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Chinese Journal of Chemistry 2025年第7期43卷 805-813页

作者： Yingqing Zhou Yanping Xu Xiuzhe Yin Wangmeng Hou Zhijia Liu Yi Shi Yongming Chen Schoolof Materials Science and Engineering Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSun Yat-SenUniversityGuangzhouGuangdong 510006China b Key Laboratory of Harbor&Marine Structure Durability Technology Ministry of TransportGuangzhouGuangdong 510230China Key Laboratory of Construction Material CCC Fourth Harbor Engineering Institute Co.Ltd.GuangzhouGuangdong 510230China College of Chemistry and Molecular Sciences Henan UniversityKaifengHenan 475004China

Dendronized polymers(DenPols)with tunable shape and surface property have been recognized as a type of promising unimolecular ***,it still has lacked a rapid and efficient approach to the facile synthesis of DenPols with high-generation and well-defined ***,we report a“m+n”grafting-onto strategy combined with the copper-catalyzed azide-alkyne cycloaddition(CuAAC)reaction with reaction-enhanced reactivity of intermediates(RERI)mechanism for synthesizing DenPols G_(m+n) by attaching n-generation dendrons(G_(n))onto the m-generation DenPols G_(m).In this“m+n”grafting-onto strategy,the DenPols G_(m)(m=1,2)bearing 1,3-triazido branches on the repeating unit were capable of RERI effect that guaranteed the CuAAC reaction in an extremely efficient way with ultrafast kinetics to synthesize third-,fourth-and fifth-generation DenPols(G_(1+2),G_(1+3),G_(1+4),G_(2+2),and G_(2+3))with near quantitative grafting density and narrow ***,these resultant DenPols G_(m+n) had more terminal groups per repeating unit due to the three branches of 1,3-triazido structure,exhibiting valuable potential opportunities for molecular surface *** development of this“m+n”grafting-onto strategy with RERI mechanism not only presents a new avenue for ultrafast preparing DenPols but also holds great promise for preparing unimolecular materials with more functional terminal groups.

关键词： Dendronized polymers Reaction-enhanced reactivity of intermediates Grafting-onto strategy Copper-catalyzed azide-alkyne cycloaddition Terminal groups Living polymerization functional polymers Nanostructures

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Modification strategies for non-aqueous, highly proton-conductive benzimidazole-based high-temperature proton exchange membranes

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Chinese Chemical Letters 2024年第4期35卷 43-51页

作者： Yunfa Dong Shijie Zhong Yuhui He Zhezhi Liu Shengyu Zhou Qun Li Yashuai Pang Haodong Xie Yuanpeng Ji Yuanpeng Liu Jiecai Han Weidong He National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and StructuresHarbin Institute of TechnologyHarbin 150080China School of Petroleum Engineering Chongqing University of Science and TechnologyChongqing 401331China School of Physics University of Electronic Science and Technology of ChinaChengdu 610054China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China Chongqing Research Institute Harbin Institute of TechnologyChongqing 401151China School of Mechanical Engineering Chengdu UniversityChengdu 610106China

High-temperature proton exchange membranes(HT-PEMs) possess excellent thermal and outstanding electrochemical stability, providing an avenue to realize high-temperature proton exchange membranes fuel cells(HT-PEMFCs) with both superior power density and long-term durability. Unfortunately, polybenzimidazole(PBI), a typical material for conventional HT-PEMs, fails to compromise the high nonaqueous proton conductivity and high mechanical properties, thus hindering their practical *** efficient nonaqueous proton conduction is crucial for HT-PEMFC, and many insightful research works have been done in this area. However, there still lacks a report that integrates the host-guest interactions of phosphoric acid doping and the structural stability of polymers to systematically illustrate modification strategies. Here, we summarize recent advancements in enhancing the nonaqueous proton conduction of HT-PEMs. Various polymer structure modification strategies, including main chain and side group modification, cross-linking, blocking, and branching, are reviewed. composite approaches of polymer, including compounding with organic porous polymers, filling the inorganic components and modifying with ionic liquids, etc., are also covered in this work. These strategies endow the HT-PEMs with more free volume, nanophase-separated structure, and multi-stage proton transfer channels, which can facilitate the proton transportation and improve their performance. Finally, current challenges and future directions for further enhancements are also outlined.

关键词： Benzimidazole Nonaqueous proton conduction Free volume Nanophase-separated structure Structure modification

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Synthesis of a Highly Crystalline Amide-Linked Covalent Organic Framework

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Chinese Journal of Chemistry 2023年第4期41卷 405-410页

作者： Yuyao Li Zhipeng Zhou Yuexian Hong Xin Dong Yonghang Yang Zihao Liang Junliang Sun Xudong Chen Wei Liu Zhikun Zheng Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education School of Chemistryand State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhouGuangdong510275 China College of Chemistry and Molecular Engineering Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing100871 China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhouGuangdong510006 China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory JieyangGuangdong515200 China Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong Province Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSchool of Materials Science and Engineeringand State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhouGuangdong510275 China

The dilemma for the synthesis of covalent organic frameworks(COFs)is crystallinity and ***,we present the synthesis of a single-crystalline amide-linked COF,and demonstrate its excellent chemical as well as thermal *** study will inspire the synthesis of a wide spectrum of highly crystalline and stable COFs,promote their structure-property investigations and boost their applications in selective gas adsorption,storage and separation.

关键词： Covalent organic frameworks Polymers Amides Organic crystals Microporous materials

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Mechanical enhancement and weakening in Mo_(6)S_(6)nanowire by twisting

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Chinese Physics B 2023年第4期32卷 534-542页

作者：徐克林演文石桥付越群杨毅张志森吴建洋 Department of Physics Research Institute for Biomimetics and Soft MatterJiujiang Research Institute and Fujian Provincial Key Laboratory for Soft Functional Materials ResearchXiamen UniversityXiamen 361005China Jiangsu Key Laboratory of Advanced Food Manufacturing Equipment and Technology Jiangnan UniversityWuxi 214122China NTNU Nanomechanical Laboratory Norwegian University of Science and TechnologyTrondheim 7491Norway

The torsional,bending and tensile mechanical properties of Mo_(6)S_(6)nanowire are examined by molecular dynamics(MD)simulations with a first-principles-based reactive force field(ReaxFF).It is found that Mo_(6)S_(6)nanowire shows unique mechanical properties such as high torsional and bending flexibility,high Young's modulus and strength,and negative Poisson's *** Mo_(6)S_(6)nanowire can be strengthened or weakened via twisting,depending on the twist *** Mo_(6)S_(6)nanowire with a slight twist angle shows brittle failure,whereas it with a large twist angle exhibits ductile failure and necking *** Mo_(6)S_(6)nanowires show a crossover in the negative Poisson's ratio at critical strains,that is,Poisson's ratio first decreases but then increases,with a minimum value down to around-0.8 at the strain of 0.01 as the twist angle is 21.0°/*** negative Poisson's ratio and the crossover are explained by the bond transform that makes zero angles to the wire cross-section.

关键词： Mo_(6)S_(6)nanowire mechanical properties twisting negative Poisson's ratio

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Germanium-based monoelemental and binary two-dimensional materials:Theoretical and experimental investigations and promising applications

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InfoMat 2022年第11期4卷 1-82页

作者： Fulai Zhao Yiyu Feng Wei Feng School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin UniversityTianjinPeople's Republic of China Key Laboratory of Advanced Ceramics and Machining Technology Ministry of EducationTianjinPeople's Republic of China Collaborative Innovation Center of Chemical Science and Engineering TianjinPeoples Republic of China

Two-dimensional(2D)materials based on group IVA elements have attracted extensive attention owing to their rich chemical structures and novel *** comprehensive review focuses on the phases of Ge monoelemental and binary 2D materials including germanene and its derivatives,Ge-IVA binary compounds,Ge-VA binary compounds,and Ge-VIA binary *** latest progress in predictive modeling,fabrication,and fundamental and physical property modulation of their stable 2D configurations are ***,various interesting applications of these Ge-based 2D materials are discussed,particularly field effect transistors,photodetectors,optical devices,catalysts,energy storage devices,solar cells,thermoelectric devices,sensors,biomedical materials,and spintronic ***,this review con-cludes with a few perspectives and an outlook for quickly expanding the appli-cation scope Ge-based 2D materials based on recent developments.

关键词： 2D materials binarycompounds electronicproperties germanene groupIVAelements

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Recent Advances in Helical Polyisocyanide-based Block Copolymers:Preparation,Self-assembly and Circularly Polarized Luminescence

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Chemical Research in Chinese Universities 2023年第5期39卷 719-725页

作者： ZHOU Li CHEN Kun ZHOU Xing-Yu WU Zong-Quan Department of Polymer Science and Engineering School of Chemistry and Chemical EngineeringAnhui Key Laboratory of Advanced Functional Materials and DevicesHefei University of TechnologyHefei 230009P.R.China State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012P.R.China

Polyisocyanides and their block copolymers have widespread applications in many fields due to their unique helix and self-assembly *** first,the latest progress in the preparation of helical polyisocyanide-based block copolymers via the method of one-pot sequential controlled synthesis and stepwise polymerization was highlighted in this *** categories of helical polyisocyanide-based copolymers including amphiphilic block copolymers,UV-response block copolymers,π-conjugated block copolymers,etc.,have been prepared ***,recent advances in the self-assembly and circularly polarized luminescence performance of amphiphilic andπ-conjugated helical polyisocyanide-based copolymers have been introduced,*** hope this minireview will not only inspire more interest in developing helical polyisocyanide-based copolymers,but also encourage further progress in the field of building artificial functional materials.

关键词： Helical polyisocyanide Block copolymer Self-assemble Circularly polarized luminescence

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P-doped all-small-molecule organic solar cells with power conversion efficiency of 17.73%

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science China Chemistry 2023年第8期66卷 2371-2379页

作者： Wanying Feng Kangqiao Ma Guangkun Song Tianyin Shao Huazhe Liang Shudi Lu Yu Chen Guankui Long Chenxi Li Xiangjian Wan Zhaoyang Yao Bin Kan Yongsheng Chen State Key Laboratory and Institute of Element-Organic Chemistry The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin300071China School of Materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin300350China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing100043China State Key Laboratory of Luminescent Materials and Devices South China University of TechnologyGuangzhou510640China

All-small organic solar cells(ASM OSCs)inherit the advantages of the distinct merits of small molecules,such as well-defined structures and less batch-to-batch *** comparison with the rapid development of polymer-based OSCs,more efforts are needed to devote to improving the performance of ASM OSCs to close the performance gap between ASM and polymer-based ***,a well-known p-dopant named fluoro-7,7,8,8-tetracyano-p-quinodimethane(FTCNQ)was introduced to a highefficiency system of HD-1:BTP-e C9,and a high power conversion efficiency(PCE)of 17.15%was achieved due to the improved electrical properties as well as better morphology of the active layer,supported by the observed higher fill factor(FF)of 79.45%and suppressed non-radiative recombination ***,combining with the further morphology optimization from solvent additive of 1-iodonaphthalene(IN)in the blend film,the HD-1:BTP-e C9-based device with the synergistic effects of both FTCNQ and IN demonstrates a remarkable PCE of 17.73%(certified as 17.49%),representing the best result of binary ASM OSCs to date.

关键词： organic solar cells all-small-molecule power conversion efficiency p-dopant

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Direct pyrolysis to convert biomass to versatile 3D carbon nanotubes/mesoporous carbon architecture:conversion mechanism and electrochemical performance

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Frontiers of Chemical science and Engineering 2023年第6期17卷 679-690页

作者： Chenxi Xu Shunli Li Zhaohui Hou Liming Yang Wenbin Fu Fujia Wang Yafei Kuang Haihui Zhou Liang Chen College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China Key Laboratory of Hunan Province for Advanced Carbon-Based Functional Materials School of Chemistry and Chemical EngineeringHunan Institute of Science and TechnologyYueyang 414006China Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063China School of Materials Science and Engineering Georgia Institute of TechnologyAtlantaGA 30332USA

The massive conversion of resourceful biomass to carbon nanomaterials not only opens a new avenue to effective and economical disposal of biomass,but provides a possibility to produce highly valued functionalized carbon-based electrodes for energy storage and conversion *** this work,biomass is applied to a facile and scalable one-step pyrolysis method to prepare three-dimensional(3D)carbon nanotubes/mesoporous carbon architecture,which uses transition metal inorganic salts and melamine as initial *** role of each employed component is investigated,and the electrochemical performance of the attained product is *** component and precise regulation of their dosage is proven to be the key to successful conversion of biomass to the desired carbon *** to the unique 3D architecture and integration of individual merits of carbon nanotubes and mesoporous carbon,the as-synthesized carbon nanotubes/mesoporous carbon hybrid exhibits versatile application toward lithium-ion batteries and Zn-air ***,a significant guidance on effective conversion of biomass to functionalized carbon nanomaterials can be shown by this work.

关键词： biomass direct pyrolysis 3D CNTs MC hybrid lithium-ion batteries Zn-air batteries

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Molecular Conformational Isomerization:An Efficient Way to Design Novel Emitters with Dual-Thermally Activated Delayed Fluorescence Characteristics and Their Optoelectronic and Bioimaging Applications

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CCS Chemistry 2024年第4期6卷 912-922页

作者： Yi-Zhong Shi Ya-Fang Xiao Hao Wu Shao-Li Zhang Xiao-Chun Fan Ye Tian Chang-Qing Ye Kai Wang Jia Yu Chun-Sing Lee Xiao-Hong Zhang School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou 215009 Institute of Functional Nano and Soft Materials(FUNSOM) Joint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123Jiangsu Center of Super-Diamond and Advanced Films(COSDAF) Department of ChemistryCity University of Hong KongHong Kong SAR School of Biomedical Engineering The Second Affiliated HospitalGuangzhou Medical UniversityGuangzhou 510260 Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Soochow UniversitySuzhou 215123Jiangsu Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123Jiangsu

Single-molecule luminophores with dual-thermally activated delayed fluorescence(TADF)properties are receiving increasing ***,how to achieve these goals requires more in-depth ***,we demonstrate a novel example emitter,10-(5-(2-(pyridin-3-yl)-[4,5′-bipyrimidin]-6-yl)pyridin-2-yl)-10Hphenoxazine(PmPy-PXZ),enabling dual-TADF properties due to its key feature of conformational *** a pyridine bridge can greatly reduce the steric hindrance and facilitate dual-stable conformations in the ground state,where the quasi-axial(QA)forms ***,unlike previously reported TADF molecules with dual confirmations,both theoretical and experimental measurements show that not only the quasi-equatorial(QE)forms but also the QA forms exhibit distinct TADF characteristics,which can be attributed to an additional higher reverse intersystem crossing *** is the first time that dual-TADF properties of single molecules have been achieved based on conformational *** applications in“self-doping”organic light-emitting diode and biomedical imaging have further been *** these results show the good potential of such dual-band TADF emitters based on molecular conformational isomerization.

关键词： dual-thermally activated delayed fluorescence conformational isomerization organic light-emitting diode biomedical imaging self-doping

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Nanostructured Pt@RuO_(x) catalyst for boosting overall acidic seawater splitting

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Chinese Journal of Structural Chemistry 2024年第1期43卷 6-15页

作者： Zimo Peng Quan Zhang Gaocan Qi Hao Zhang Qian Liu Guangzhi Hu Jun Luo Xijun Liu Institute for New Energy Materials&Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of TechnologyTianjin300384China School of Materials Science and Engineering Tianjin University of TechnologyTianjin 300384China Institute for Advanced Study Chengdu UniversityChengdu610106China Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental ScienceYunnan UniversityKunming650091China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaLonghua DistrictShenzhen518110China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsMOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning530004China

In the domain of acidic water splitting,designing bifunctional catalysts that marry high activity with enduring stability is a formidable ***,we have constructed platinum-containing ruthenium oxide nanoparticles(Pt@RuO_(x)NPs)to achieve excellent overall water splitting performance in acidic ***@RuO_(x)NPs demonstrate exceptional catalytic activity for both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in acidic seawater,requiring overpotentials of only 20 and 157 mV,respectively to achieve a current density of 10 mA cm^(-2).Furthermore,in 0.5 M H_(2)SO_(4),this catalyst exhibits high HER(19 mV)and OER(236 mV)catalytic *** two-electrode water splitting system composed of bifunctional Pt@RuO_(x)NPs requires cell voltages of only 1.442 and 1.465 V to deliver a current density of 10 mA cm^(-2)in acidic seawater and 0.5 M H_(2)SO_(4).Remarkably,this catalyst displays remarkable stability in the water splitting *** is shown that the introduction of Pt could augment oxygen vacancies and enhance catalytic activity *** synergy between Pt and Ru further contributes to the improved ***,we have observed that acidic seawater holds distinct advantages for acidic water splitting,along with a thorough exploration of the relationship between Cl^(-)concentration and catalytic *** study not only provides a strategy to improve the catalytic activity and stability of ruthenium-based catalysts for water splitting in acidic environments,but also unveils the promoting effect of Cl^(-)on the catalytic activity in acidic water splitting.

关键词： Acidic water splitting Bifunctional catalysts Pt@RuOx nanoparticles Synergistic effect

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