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Science China Chemistry 2025年

作者： Panke Zhou Yuxing Huang Ziyue Yu Cong Zhang Qian Chen Yiping Li Chao Lin Xiong Chen State key laboratory of Photocatalysis on Energy and Environment Key Laboratory of Advanced Carbon-Based Functional MaterialsCollege of Chemistry Fuzhou University

The development of stimuli-responsive switching memory devices and the elucidation of their switching mechanisms in specific environments are crucial for advancing the field of molecular electronics. Herein, we propose two distinct two-dimensional covalent organic frameworks (COFs), namely Py-EDA and Py-BDA, incorporating acetylene (-C≡C-) or diacetylene(-C≡C-C≡C-) moieties, respectively, targeting fabricate memory devices exhibiting stimuli-responsive switching *** findings demonstrate that the incorporation of acetylene units effectively modulates the electronic band structure and enhances the degree ofπ-conjugation, resulting in devices that exhibit typical bipolar nonvolatile memory performance. Notably,upon thermal treatment, the memory behavior of the ITO/Py-BDA/Ag device transitions to a write-once-read-many-times(WORM) mode, displaying decreased SET voltage, increased ON/OFF current ratio, and remarkable retention reliability and cycle stability. This switching behavior is attributed to the occurrence of interlayer solid-state topological polymerization at 350℃, leading to the transformation of diacetylene columnar arrays into enyne chains within Py-BDA, thereby further promoting interlayer charge transfer and separation.

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Tuning the ion-dipole interactions between fluoro and carbonyl(EC)by electrolyte design for stable lithium metal batteries

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Chinese Chemical Letters 2025年第1期36卷 579-584页

作者： Guihuang Fang Ying Liu Yangyang Feng Ying Pan Hongwei Yang Yongchuan Liu Maoxiang Wu Faculty of Metallurgy and Energy Engineering Kunming University of Science and TechnologyKunming 650093China key laboratory of Optoelectronic materials Chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Ethylene carbonate(EC)is the conventional and promising solvent to achieve high energy lithium metal ***,the innate low energy level of lowest unoccupied molecular orbital(LUMO)in EC makes it incompatible with lithium metal,causing uncontrolled lithium growth and low Coulombic efficiency(CE).Herein,we introduced bis(2,2,2-trifluoroethyl)carbonate(TFEC),a carbonate with a strong electron-withdrawing effect(-CF_(3)),which enhances the stability of EC at electrode interface by reducing ion-dipole interactions between Li^(+)and *** the interaction between Li and EC weakens,TFEC and more PF_(6)^(-)anions coordinate with Li^(+),promoting the formation of contact ion pairs(CIPs)and aggregates(AGGs),thereby increasing the inorganic composition within the solid electrolyte ***,the distinct solvated sheath structure favors the decomposition of fluorinated solvents and PF_(6)^(-)anions,forming inorganic-rich electrode-electrolyte interfaces(SEI and CEI),thereby ensuring high stability for both the Li anode and high-voltage ***,when applied in the full-cell Li||LiMn_(0.8)Fe_(0.2)PO_(4),it displays consistent cycling performance,exhibiting minimal capacity decay with a retention rate of 62.5%after800 cycles,substantially surpassing that of cells using base electrolytes(29.8%).

关键词： Lithium-ion batteries LiMn_(0.8)Fe_(0.2)PO_(4) High-voltage Solvation structure Ethylene carbonate Bis(2,2,2-trifluoroethyl)carbonate

Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China Chemistry 2025年第1期68卷 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State key laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China State key laboratory of Natural Medicines China Pharmaceutical UniversityNanjing 211198China

Selective modification of peptides has always been a challenging *** selective alkylation of peptides can alter the biological activity and physical properties of molecules,and it has gained significant research *** herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis.A wide range of structurally diverse primary,secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with theα-C(sp^(3))–H in glycine residue of *** protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups.A series of relay transformations to construct cyclic peptides,to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic *** addition,mechanistic studies and density functional theory(DFT)calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET)mechanism.

关键词： gold catalysis peptide alkylation C-C coupling radical

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Spatially confined synthesis of TiNb_(2)O_(7)quantum dots onto mesoporous carbon and Ti_(3)C_(2)T_(X)MXene for boosting lithium storage

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Green Energy & Environment 2025年第2期10卷 358-366页

作者： Daoguang Sun Cheng Tang Haitao Li Xinlin Zhang Guanjia Zhu Zhen-Dong Huang Aijun Du Haijiao Zhang Institute of Nanochemistry and Nanobiology School of Environmental and Chemical EngineeringShanghai UniversityShanghai200444China School of Chemistry and Physics and Centre for materials Science Queensland University of TechnologyBrisbaneQLD4001Australia State key laboratory for Organic Electronics and Information Displays&Jiangsu key laboratory for Biosensors Institute of Advanced Materials(IAM)Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)Nanjing University of Posts and Telecommunications9 Wenyuan RoadNanjing210023China

TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion ***,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage ***,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)***,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous *** strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.

关键词： TiNb_(2)O_(7)quantum dots Ti_(3)C_(2)T_(X)MXene Mesoporous carbon Confined synthesis Lithium-ion batteries

Improving structure stability of single-crystalline Ni-rich cathode at high voltage by element gradient doping and interfacial modifcation

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Journal of Energy Chemistry 2025年第2期101卷 630-640页

作者： Ruijuan Wang Yixu Zhang Zhi Li Lei Wu Jiarui Chen Xiaolin Liu Hui Hu Hao Ding Shuang Cao Qiliang Wei Xianyou Wang National Base for International Science & Technology Cooperation of New Energy Equipment Energy Storage Materials and Devices National Local Joint Engineering Laboratory for Key Materials of New Energy Storage Battery Hunan Province Key Laboratory of Electrochemical Energy Storage & Conversion School of Chemistry Xiangtan University Institute of micro/Nano materials and Devices Ningbo University of Technology

Single-crystalline Ni-rich cathodes can provide high energy density and capacity retention rates for lithium-ion batteries（LIBs）.However,single-crystalline Ni-rich cathodes experience severe transition metal dissolution,irreversible phase transitions,and reduced structural stability during prolonged cycling at high voltage,which will significantly hinder their practical ***,a Li4TeO5surface coating along with bulk Te-gradient doping strategy is proposed and developed to solve these issues for single-crystalline Ni-rich LiNi0.90Co0.05Mn0.05O2cathode（LTeO-1.0）.It has been found that the bulk Te6+gradient doping can lead to the formation of robust Te-O bonds that effectively inhibit H2-H3 phase transformations and reinforce the lattice framework,and the in-situ Li4TeO5coating layer can act as a protective layer that suppresses the parasitic reactions and grain ***,the modified material exhibits a higher Young's modulus,which will be conducive to maintaining significant structural and electrochemical stability under high-voltage conditions,Especially,the LTeO-1.0 electrode shows the improved Li+diffusion kinetics and thermodynamic stability as well as high capacity retention of 95.83%and 82.12% after 200 cycles at the cut-off voltage of 4.3 and 4,5 ***,the efficacious dualmodification strategy will definitely contribute to enhancing the structural and electrochemical stability of single-crystalline Ni-rich cathodes and developing their application in LIBs.

关键词： High cut-off voltage Li4TeO5 coating layer Material fragmentation Single-crystalline Ni-rich cathode Te6+ doping

Auxiliary ligand-induced assembly of atomically precise silver clusters

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Science China Chemistry 2025年第2期68卷 580-589页

作者： Yeqin Feng Xuemeng Jing Fangyu Fu Mengyun Zhao Manzhou Chi Hongjin Lv Guo-Yu Yang MOE key laboratory of Cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

Establishing the correlation between inter-cluster assembly and auxiliary ligands at the atomic level is crucial for the development of metal cluster *** this work,we report the successful preparation and characterization of three Ag clusters,discrete 0-D Ag_(51)S_(6)Cl_(3)(i PrS)_(21)(TsO)_(15)CH_(3)CN(0-D Ag_(51),i PrS–=isopropanethiolate,TsO–=toluenesulfonate),1-D{Ag_(38)S_(4)-(i PrS)_(18)(PhCOO)_(12)}n(1-D Ag_(38),PHCOO–=benzoate),and 2-D{Ag_(2)0(SO_(4))Cl_(2)(i PrS)10(NO_(3))6}n(2-D Ag_(20)),using a delicate auxiliary-ligand-induced *** analyses reveal that the types of auxiliary ligands can readily affect the structure and dimensionality of resulting Ag *** addition of different surface auxiliary ligands from TsO–to PhCOO–and then to NO_(3)–leads to the formation of 0-D Ag_(51) to 1-D Ag_(38) and then to 2-D Ag_(2)0 clusters under otherwise identical reaction conditions,*** resulting Ag clusters exhibited structure-related optical/luminescence properties and distinct bathochromic shifts as revealed by the temperature-dependent luminescence and single-crystal X-ray diffraction studies.

关键词： silver(I)clusters auxiliary ligand effect silver cluster synthesis luminescence

Conversion-type cathode materials for high energy density solid-state lithium batteries

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Journal of Energy Chemistry 2025年第1期100卷 409-425页

作者： Yuhao Ma Shihong Qing Hongyu Liu Chuntao Ma Yuan Yu Chuang Yu Liping Wang School of materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina Zhejiang Provincial key laboratory of Fiber materials and Manufacturing Technology Zhejiang Sci-Tech UniversityHangzhou 310018ZhejiangChina State key laboratory of advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy *** particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and *** the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing *** review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in ***,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical ***,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type ***,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.

关键词： Conversion-type cathode Lithium-free cathode Solid-state electrolyte Solid-state lithium battery High energy density

AlO2: A novel two-dimensional material with a high negative Poisson's ratio for the adsorption of volatile organic compounds

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Chinese Chemical Letters 2025年第2期36卷 557-563页

作者： Xinghong Cai Qiang Yang Yao Tong Lanyin Liu Wutang Zhang Sam Zhang Min Wang Chongqing key laboratory for advanced materials and Technologies of Clean Energies School of Materials and EnergySouthwest University BatteroTech Co. Ltd. School of Astronautics Harbin Institute of Technology Zhengzhou Research Institute Harbin Institute of Technology

We propose and investigate a novel stable two-dimensional（2D） AlO2with anomalous stoichiometric ratios based on first-principles calculation. 2D AlO2has metallic properties. It possesses the rare in-plane and out-of-plane negative Poisson's ratio（NPR） phenomenon, originating from its special sawtooth-like structure. The absolute value of the NPR decreases as the number of layers increases. The adsorption of volatile organic compounds（VOCs） including CH2O, C2H3Cl and C6H6by AlO2exhibit small adsorption distance, large adsorption energy, large charge transfer and significant density of states（DOS） changes,indicating the presence of strong interactions. The desorption time of each gas molecule on the AlO2surface is also evaluated, and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO2. These interesting properties make 2D AlO2a promising material for electronic, mechanical and sensing applications for VOCs.

关键词： AlO2 First-principles calculations Negative Poisson's ratio Two-dimensional material VOCs

micro-strain regulation strategy to stabilize perovskite lattice based on the categories and impact of strain on perovskite solar cells

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Journal of Energy Chemistry 2025年第1期100卷 578-604页

作者： Caixia Li Wenwu Liu Shiji Da Lingbin Kong Fen Ran State key laboratory of advanced Processing and Recycling of Nonferrous Metals Lanzhou University of TechnologyLanzhou 730050GansuChina School of materials Science and Engineering Lanzhou University of TechnologyLanzhou 730050GansuChina

Photovoltaic metal halide perovskite solar cells(PSCs) convert light to electricity more efficiently than crystalline silicon cells, and the cost of materials used to make them is lower than that of silicon *** efficiency is not a core issue affecting the application of perovskite solar cells in special *** present, stability is the major technical encounters that hinders its further commercial development. microstrain in PSCs is currently a significant factor responsible for the device's instability. Strain-induced ion migration is widely believed to accelerate perovskite degradation even when external stimuli are ***, it is imperative to study strain to enhance the stability of PSCs. This paper reviews recent developments to understand strain's origin and effect mechanisms on performance of PSCs, including ion migration,failure behavior, defect formation, and its effect on photoelectric properties, stability, and ***, several well-known strain management strategies are systematically introduced based on the strain effect mechanism and strain engineering on the film, providing more clues for further preparation with increased stability. The manipulation of external physical strain applied from films to entire devices has been extensively studied. Furthermore, recommendations for future research directions and chemical approaches have been provided. It is emphasized that strain engineering plays a crucial role in improving the efficiency and longevity of PSCs. Tensile strain causes rapid degradation, while moderate compressive strain and external strain control could improve properties and stability. Efforts should focus on controlling compressive strain to mitigate residual tensile strain and introducing it in a controlled manner. Future research endeavors may focus on exploring these pathways to improve the efficiency and lifespan of PSCs.

关键词： Halide perovskite solar cells Strain origins Strain effects Strain management

Effect of surface species on the alcohol-acid adsorption from FTS wastewater on graphene:A structure-capacity study

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Journal of Environmental Sciences 2025年第3期149卷 651-662页

作者： Xiao Liu Xiaolong Zhang Chunyu Geng Qinglan Hao Jie Chang Xin Hu Yongwang Li Botao Teng Tianjin key laboratory of Brine Chemical Engineering and Resource Eco-utilization College of Chemical Engineering and Materials ScienceTianjin University of Science and TechnologyTianjin 300457China State key laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer MaterialsCollege of ChemistryNankai UniversityTianjin 300071China National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Beijing 101407China Institute of Sustainability of Chemical Energy and EnvironmentAgency for ScienceTechnology and Research627833Singapore key laboratory of the Ministry of Education for advanced Catalysis materials Zhejiang Normal UniversityJinhua 321004China

Fischer-Tropsch synthesis(FTS)wastewater retaining low-carbon alcohols and acids are organic pollutants as a limiting factor for FTS *** this work,the structurecapacity relationships between alcohol-acid adsorption and surface species on graphene were reported,shedding light into their intricate *** graphene oxide(GO)and reduced graphene oxide(rGO)were synthesized via improved Hummers method with flake graphite(G).The physicochemical properties of samples were characterized via SEM,XRD,XPS,FT-IR,and *** alcohol-acid adsorption behaviors and adsorption quantities on G,GO,and rGO weremeasured via theoretical and *** was revealed that the presence of COOH,C=O and C–O species on graphene occupy the adsorption sites and increase the interactions of water with graphene,which are unfavorable for alcoholacid *** equilibrium adsorption quantities of alcohols and acids grow in pace with carbon *** monolayer adsorption occurs on graphene was verified viamodel *** has the highest FTS modeling wastewater adsorption quantity(110 mg/g)due to the reduction of oxygen *** novel findings provide a foundation for the alcoholacid wastewater treatment,as well as the design and development of high-performance carbon-based adsorbent materials.

关键词： Alcohol-acid adsorption Fischer-Tropsch synthesis wastewater Graphene Surface species Density functional theory