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Evolution of Stabilized 1T-MoS2by Atomic-Interface Engineering of 2H-MoS2/Fe−Nxtowards Enhanced Sodium Ion Storage

Angewandte Chemie 2023年第14期135卷

作者： Huicong Xia Lingxing Zan Pengfei Yuan Gan Qu Hongliang Dong Yifan Wei Yue Yu Zeyu Wei Wenfu Yan Jin-Song Hu Dehui Deng Jia-Nan Zhang College of Materials Science and Engineering Zhengzhou University Zhengzhou 450001 P. R. China State Key Laboratory of Catalysis iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China Key Laboratory of Chemical Reaction Engineering of Shaanxi Province College of Chemistry & Chemical Engineering Yan'an University Yan'an 716000 P. R. China College of Physics and Engineering Zhengzhou University Zhengzhou 450001 P. R. China Center for High Pressure Science and Technology Advanced Research Pudong Shanghai 201203 P. R. China State Key Lab of Inorganic Synthesis & Preparative Chemistry Jilin University Changchun 130012 P. R. China Chinese Academy of Sciences Key Laboratory of Molecular Nanostructure and Nanotechnology Institute of Chemistry Chinese Academy of Science Beijing 100190 P. R. China Key Laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou City Zhengzhou 450012 P. R. China

Metallic conductive 1T phase molybdenum sulfide (MoS 2 ) has been identified as promising anode for sodium ion (Na + ) batteries, but its metastable feature makes it difficult to obtain and its restacking during the charge/discharge processing result in part capacity reversibility. Herein, a synergetic effect of atomic-interface engineering is employed for constructing 2H-MoS 2 layers assembled on single atomically dispersed Fe−N−C (SA Fe−N−C) anode material that boosts its reversible capacity. The work-function-driven-electron transfer occurs from SA Fe−N−C to 2H-MoS 2 via the Fe−S bonds, which enhances the adsorption of Na + by 2H-MoS 2 , and lays the foundation for the sodiation process. A phase transfer from 2H to 1T/2H MoS 2 with the ferromagnetic spin-polarization of SA Fe−N−C occurs during the sodiation/desodiation process, which significantly enhances the Na + storage kinetics, and thus the 1T/2H MoS 2 /SA Fe−N−C display a high electronic conductivity and a fast Na + diffusion rate.

关键词： Atomic Interface Engineering Evolution Fe−N−C Phase Transform of MoS2 Sodium Ion Storage

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Photo-responsive Helical Motion by Light-Driven Molecular Motors in a Liquid-Crystal Network

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Angewandte Chemie 2021年第15期133卷

作者： Jiaxin Hou Anirban Mondal Guiying Long Dr. Laurens de Haan Dr. Wei Zhao Prof. Guofu Zhou Dr. Danqing Liu Prof. Dirk J. Broer Prof. Jiawen Chen Prof. Ben L. Feringa SCNU-UG International Joint Laboratory of Molecular Science and Displays National Center for International Research on Green Optoelectronics South China Normal University Guangzhou 510006 China Stratingh Institute for Chemistry University of Groningen Nijenborgh 4 9747 AG Groningen The Netherlands SCNU-TUE Joint lab of Device Integrated Responsive Materials (DIRM) Guangdong Provincial Key Laboratory of Optical Information Materials and Technology & Institute of Electronic Paper Displays South China Academy of Advanced Optoelectronics South China Normal University Guangzhou 510006 China Stimuli-responsive Functional Materials and Devices Department of Chemical Engineering and Chemistry Eindhoven University of Technology Den Dolech 2 5600 MB Eindhoven The Netherlands

Controlling sophisticated motion by molecular motors is a major goal on the road to future actuators and soft robotics. Taking inspiration from biological motility and mechanical functions common to artificial machines, responsive small molecules have been used to achieve macroscopic effects, however, translating molecular movement along length scales to precisely defined linear, twisting and rotary motions remain particularly challenging. Here, we present the design, synthesis and functioning of liquid-crystal network (LCN) materials with intrinsic rotary motors that allow the conversion of light energy into reversible helical motion. In this responsive system the photochemical-driven molecular motor has a dual function operating both as chiral dopant and unidirectional rotor amplifying molecular motion into a controlled and reversible left- or right-handed macroscopic twisting movement. By exploiting the dynamic chirality, directionality of motion and shape change of a single motor embedded in an LC-network, complex mechanical motions including bending, walking and helical motion, in soft polymer materials are achieved which offers fascinating opportunities toward inherently photo-responsive materials.

关键词： chirality helical motion liquid-crystal network molecular motors photo-responsive motion

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Frenkel and Charge-Transfer Excitonic Couplings Strengthened by Thiophene-Type Solvent Enables Binary Organic Solar Cells with 19.8 % Efficiency

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Angewandte Chemie 2024年第44期136卷

作者： Prof. Xin Song Le Mei Xinjie Zhou Prof. Hongxiang Li Hao Xu Xingting Liu Shenzheng Gao Shanlei Xu Yahui Yang Prof. Weiguo Zhu Prof. Jianpu Wang Prof. Xiao-Hong Zhang Prof. Xian-Kai Chen School of Materials Science and Engineering Jiangsu Engineering Research Center of Light-Electricity-Heat Energy-Converting Materials and Applications Jiangsu Collaborative Innovation Center of Photovoltaic Science and Engineering Changzhou University Changzhou 213164 P.R. China State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 P. R. China These authors contributed equally to this work Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou Jiangsu 215123 P.R. China. Department of Chemistry City University of Hong Kong Kowloon Hong Kong 999077 P.R. China. State Key Laboratory of Polymer Materials Engineering College of Polymer Science and Engineering Sichuan University Chengdu 610065 P.R. China Key Laboratory of Flexible Electronics (KLOFE) and Institute of Advanced Materials (IAM) Nanjing Tech University (NanjingTech) 30 South Puzhu Road Nanjing 211816 P.R. China

Overcoming the trade-off between short-circuited current ( J sc ) and open-circuited voltage ( V oc ) is important to achieving high-efficiency organic solar cells (OSCs). Previous works modulated the energy gap between Frenkel local exciton (LE) and charge-transfer (CT) exciton, which served as the driving force of exciton splitting. Differently, our current work focuses on the modulation of LE-CT excitonic coupling (t LE-CT ) via a simple but effective strategy that the 2-chlorothiophene (2Cl−Th) solvent utilizes in the treatment of OSC active-layer films. The results of our experimental measurements and theoretical simulations demonstrated that 2Cl−Th solvent initiates tighter intermolecular interactions with non-fullerene acceptor in comparison with that of traditional chlorobenzene solvent, thus suppressing the acceptor's over-aggregation and retarding the acceptor crystallization with reduced trap. Critically, the resulting shorter distances between donor and acceptor molecules in the 2Cl−Th treated blend efficiently strengthen t LE-CT , which not only promotes exciton splitting but also reduces non-radiative recombination. The champion efficiencies of 19.8 % (small-area) with superior operational reliability (T80: 586 hours) and 17.0 % (large-area) were yielded in 2Cl−Th treated cells. This work provided a new insight into modulating the exciton dynamics to overcome the trade-off between J sc and V oc , which can productively promote the development of the OSC field.

关键词： organic solar cells exciton splitting non-radiative loss excitonic coupling morphology regulation

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Stable Interface Chemistry and Multiple Ion Transport of composite Electrolyte Contribute to Ultra-long Cycling Solid-State LiNi0.8Co0.1Mn0.1O2/Lithium Metal Batteries

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Angewandte Chemie 2021年第46期133卷

作者： Ke Yang Likun Chen Jiabin Ma Dr. Chen Lai Dr. Yanfei Huang Jinshuo Mi Jie Biao Danfeng Zhang Peiran Shi Heyi Xia Prof. Guiming Zhong Prof. Feiyu Kang Prof. Yan-Bing He Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center Institute of Materials Research (IMR) Tsinghua Shenzhen International Graduate School Shenzhen 518055 P. R. China School of Materials Science and Engineering Tsinghua University Beijing 100084 P. R. China Key Lab of Advanced Functional Materials Ministry of Education Faculty of Materials and Manufacturing Beijing University of Technology Beijing 100084 P. R. China College of Materials Science and Engineering Shenzhen University Shenzhen 518055 P. R. China Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China

Severe interfacial side reactions of polymer electrolyte with LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode and Li metal anode restrict the cycling performance of solid-state NCM811/Li batteries. Herein, we propose a chemically stable ceramic-polymer-anchored solvent composite electrolyte with high ionic conductivity of 6.0×10 −4 S cm −1 , which enables the solid-state NCM811/Li batteries to cycle 1500 times. The Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 nanowires (LNs) can tightly anchor the essential N, N-dimethylformamide (DMF) in poly(vinylidene fluoride) (PVDF), greatly enhancing its electrochemical stability and suppressing the side reactions. We identify the ceramic-polymer-liquid multiple ion transport mechanism of the LNs-PVDF-DMF composite electrolyte by tracking the 6 Li and 7 Li substitution behavior via solid-state NMR. The stable interface chemistry and efficient ion transport of LNs-PVDF-DMF contribute to superior performances of the solid-state batteries at wide temperature range of −20–60 °C.

关键词： composite electrolytes interface chemistry multiple ion transport solid-state lithium metal batteries

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Molecular Iron Oxide Clusters Boost the Oxygen Reduction Reaction of Platinum Electrocatalysts at Near-Neutral pH

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Angewandte Chemie 2022年第38期134卷

作者： Dr. Jia-Qi Lv Dr. Zhong-Ling Lang Jia-Qi Fu Dr. Qiao Lan Dr. Rongji Liu Prof. Hong-Ying Zang Prof. Yang-Guang Li Prof. Dr. Ding-Ding Ye Prof. Carsten Streb Key Lab of Polyoxometalate Science of Ministry of Education Key Laboratory of Nanobiosensing and Nanobioanalysis at Universities of Jilin Province Institute of Functional Material Chemistry Faculty of Chemistry Northeast Normal University Changchun 130024 China Centre for Advanced Optoelectronic Functional Materials Research and Key Laboratory for UV Light-Emitting Materials and Technology of Ministry of Education Northeast Normal University Changchun 130024 China Institute of Engineering Thermophysics School of Energy and Power Engineering Chongqing University No. 174 Shazheng Street Shapingba District Chongqing 400030 China Institute of Inorganic Chemistry I Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany Helmholtz-Institute Ulm (HIU) Helmholtzstr. 11 89081 Ulm Germany Department of Chemistry Johannes Gutenberg University Mainz Duesbergweg 10-14 55131 Mainz Germany

The oxygen reduction reaction (ORR) is a key energy conversion process, which is critical for the efficient operation of fuel cells and metal–air batteries. Here, we report the significant enhancement of the ORR-performance of commercial platinum-on-carbon electrocatalysts when operated in aqueous electrolyte solutions (pH 5.6), containing the polyoxoanion [Fe 28 (μ 3 -O) 8 (L-(−)-tart) 16 (CH 3 COO) 24 ] 20− . Mechanistic studies provide initial insights into the performance-improving role of the iron oxide cluster during ORR. Technological deployment of the system is demonstrated by incorporation into a direct formate microfluidic fuel cell (DFMFC), where major performance increases are observed when compared with reference electrolytes. The study provides the first examples of iron oxide clusters in electrochemical energy conversion and storage.

关键词： Electrocatalysis Iron Oxide Oxygen Reduction Reaction Polyoxometalates Self-Assembly

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Author Correction: Stabilization of layered lithium-rich manganese oxide for anion exchange membrane fuel cells and water electrolysers

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Nature Catalysis 2024年 604页

作者： Xuepeng Zhong Lijun Sui Menghao Yang Jiwei Ma Toshinari Koketsu Malte Klingenhof Peter Strasser Sören Selve Kyle G. Reeves Chuangxin Ge Lin Zhuang Wang Hay Kan Maxim Avdeev Miao Shu Nicolas Alonso-Vante Jin-Ming Chen Shu-Chih Haw Chih-Wen Pao Yu-Chung Chang Yunhui Huang Zhiwei Hu Shanghai Key Laboratory for R&D and Application of Metallic Functional Materials Institute of New Energy for Vehicles School of Materials Science and Engineering Tongji University Shanghai China Department of Chemistry Technical University Berlin Berlin Germany Battery Materials Development Section Business Creation Sector R&D Center Mitsui Mining and Smelting Company Limited Saitama Japan Center for Electron Microscopy (ZELMI) Technical University Berlin Berlin Germany Maison de la Simulation CEA CNRS Université Paris-Sud UVSQ Université Paris-Saclay Gif-sur-Yvette France The Institute for Advanced Studies Wuhan University Wuhan China Spallation Neutron Source Science Center Dongguan China Institute of High Energy Physics Chinese Academy of Sciences Beijing China Australian Nuclear Science and Technology Organisation Kirrawee DC New South Wales Australia School of Chemistry The University of Sydney Sydney Australia Institute of Advanced Science Facilities Shenzhen China IC2MP UMR-CNRS 7285 University of Poitiers Poitiers France National Synchrotron Radiation Research Center Hsinchu Taiwan State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan China Max Planck Institute for Chemical Physics of Solids Dresden Germany

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DNA Nanoribbon‐Templated Self‐Assembly of Ultrasmall Fluorescent Copper Nanoclusters with Enhanced Luminescence

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Angewandte Chemie 2020年第29期132卷

作者： Xiangyuan Ouyang Meifang Wang Linjie Guo Chengjun Cui Ting Liu Yongan Ren Yan Zhao Zhilei Ge Xiniu Guo Gang Xie Jiang Li Chunhai Fan Lihua Wang Key Laboratory of Synthetic and Natural Functional Molecule of Ministry of Education College of Chemistry & Materials Science Northwest University Xi'an Shaanxi 710127 P. R. China Shanghai Synchrotron Radiation Facility Zhangjiang Laboratory Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 China Division of Physical Biology CAS Key Laboratory of Interfacial Physics and Technology Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201800 China University of Chinese Academy of Sciences Beijing 100049 China School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200127 China Instrumental Analysis Center Shanghai Jiao Tong University Shanghai China

Fluorescent copper nanoclusters (CuNCs) have been widely used in chemical sensors, biological imaging, and light‐emitting devices. However, individual fluorescent CuNCs have limitations in their capabilities arising from poor photostability and weak emission intensities. As one kind of aggregation‐induced emission luminogen (AIEgen), the formation of aggregates with high compactness and good order can efficiently improve the emission intensity, stability, and tunability of CuNCs. Here, DNA nanoribbons, containing multiple specific binding sites, serve as a template for in situ synthesis and assembly of ultrasmall CuNCs (0.6 nm). These CuNC self‐assemblies exhibit enhanced luminescence and excellent fluorescence stability because of tight and ordered arrangement through DNA nanoribbons templating. Furthermore, the stable and bright CuNC assemblies are demonstrated in the high‐sensitivity detection and intracellular fluorescence imaging of biothiols.

关键词： cluster compounds copper fluorescence nanostructures self-assembly

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Tandem Synergistic Effect of Cu-In Dual Sites Confined on the Edge of Monolayer CuInP2S6toward Selective Photoreduction of CO2into Multi-Carbon Solar Fuels

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Angewandte Chemie 2023年第9期136卷

作者： Wa Gao Dr. Li Shi Wentao Hou Cheng Ding Prof. Qi Liu Prof. Ran Long Haoqiang Chi Prof. Yongcai Zhang Xiaoyong Xu Xueying Ma Zheng Tang Prof. Yong Yang Prof. Xiaoyong Wang Prof. Qing Shen Prof. Yujie Xiong Prof. Jinlan Wang Prof. Zhigang Zou Yong Zhou School of Physical Science and Technology Tiangong University Tianjin 300387 P. R. China School of Physics Jiangsu Key Laboratory of Nanotechnology Eco-materials and Renewable Energy Research Center (ERERC) National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 P. R. China State Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM) Nanjing University of Posts and Telecommunications Nanjing 210023 P. R. China School of Chemical and Environmental Engineering School of Materials and Engineering Anhui Polytechnic University Wuhu 241000 P. R. China School of Chemistry and Materials Science University of Science and Technology of China Hefei 230036 Anhui P. R. China Chemistry Interdisciplinary Research Center School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225009 P. R. China Key Laboratory of Soft Chemistry and Functional Materials (MOE) Nanjing University of Science and Technology Nanjing 210094 P. R. China Graduate School of Informatics and Engineering University of Electrocommunication 1-5-1 Chofugaoka Chofu Tokyo 1828585 Japan School of Physics Southeast University Nanjing 211189 Jiangsu P. R. China School of Science and Engineering The Chinese University of Hongkong (Shenzhen) Shenzhen Guangdong 518172 P. R. China

One-unit-cell, single-crystal, hexagonal CuInP 2 S 6 atomically thin sheets of≈0.81 nm in thickness was successfully synthesized for photocatalytic reduction of CO 2 . Exciting ethene (C 2 H 4 ) as the main product was dominantly generated with the yield-based selectivity reaching ≈56.4 %, and the electron-based selectivity as high as ≈74.6 %. The tandem synergistic effect of charge-enriched Cu−In dual sites confined on the lateral edge of the CuInP 2 S 6 monolayer (ML) is mainly responsible for efficient conversion and high selectivity of the C 2 H 4 product as the basal surface site of the ML, exposing S atoms, can not derive the CO 2 photoreduction due to the high energy barrier for the proton-coupled electron transfer of CO 2 into *COOH. The marginal In site of the ML preeminently targets CO 2 conversion to *CO under light illumination, and the *CO then migrates to the neighbor Cu sites for the subsequent C−C coupling reaction into C 2 H 4 with thermodynamic and kinetic feasibility. Moreover, ultrathin structure of the ML also allows to shorten the transfer distance of charge carriers from the interior onto the surface, thus inhibiting electron-hole recombination and enabling more electrons to survive and accumulate on the exposed active sites for CO 2 reduction.

关键词： Atomic Layer CO2 Edge Ethylene Photoreduction

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Cover Picture: (ChemistrySelect 25/2024)

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ChemistrySelect 2024年第25期9卷

作者： Dr. Dmitry S. Muratov Lev O. Luchnikov Dr. Danila S. Saranin Artur R. Ishteev Vladislav Kurichenko Evgeniy A. Kolesnikov Dr. Denis V. Kuznetsov Dr. Aldo Di Carlo Department of Chemistry University of Turin via Pietro Giuria 5 Turin 10125 Italy Laboratory of Advanced Solar Energy (LASE) National University of Science and Technology “MISiS” Leninsky prospekt 6 Moscow 119049 Russia N.N. Semenov Federal Research Center for Chemical Physics Russian Academy of Sciences Kosygina st. 4 Moscow 119991 Russia Department of Functional NanoSystems and High-Temperature Materials Materials National University of Science and Technology “MISiS” Leninsky prospekt 4 Moscow 119049 Russia CHOSE – Centre for Hybrid and Organic Solar Energy Department of Electronic Engineering University of Rome Tor Vergata via del Politecnico 1 Rome 00133 Italy

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In-situ spectroscopic probe of the intrinsic structure feature of single-atom center in electrochemical CO/CO2 reduction to methanol

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Nature Communications 2023年第1期14卷 1-10页

作者： Xinyi Ren Jian Zhao Xuning Li Shifu Wang Xiong Zhang Yanqiang Huang Junming Shao Aude Salamé Etienne Boutin Thomas Groizard Chengyu Liu Marc Robert Binbin Pan Yanguang Li Jie Ding Bin Liu Wen-Yang Huang Wen-Jing Zeng Sung-Fu Hung CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China University of Chinese Academy of Sciences Beijing 100049 China Department of Chemical Physics University of Science and Technology of China Hefei 230026 China Université Paris Cité Laboratoire d’Electrochimie Moléculaire CNRS F-75006 Paris France Institut Universitaire de France (IUF) F-75005 Paris France Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou 215123 China Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China Department of Materials Science and Engineering City University of Hong Kong Hong Kong SAR 999077 China Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 300 Taiwan

While exploring the process of CO/CO2electroreduction (COxRR) is of great significance to achieve carbon recycling, deciphering reaction mechanisms so as to further design catalytic systems able to overcome sluggish kinetics remains challenging. In this work, a model single-Co-atom catalyst with well-defined coordination structure is developed and employed as a platform to unravel the underlying reaction mechanism of COxRR. The as-prepared single-Co-atom catalyst exhibits a maximum methanol Faradaic efficiency as high as 65% at 30 mA/cm2in a membrane electrode assembly electrolyzer, while on the contrary, the reduction pathway of CO2to methanol is strongly decreased in CO2RR. In-situ X-ray absorption and Fourier-transform infrared spectroscopies point to a different adsorption configuration of *CO intermediate in CORR as compared to that in CO2RR, with a weaker stretching vibration of the C–O bond in the former case. Theoretical calculations further evidence the low energy barrier for the formation of a H-CoPc-CO–species, which is a critical factor in promoting the electrochemical reduction of CO to methanol.

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