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Formulating the Electrolyte Towards High-Energy and Safe Rechargeable Lithium–Metal Batteries

Angewandte Chemie 2021年第30期133卷

作者： Qiang Ma Dr. Junpei Yue Min Fan Shuang-Jie Tan Dr. Juan Zhang Dr. Wen-Peng Wang Dr. Yuan Liu Yi-Fan Tian Dr. Quan Xu Prof. Ya-Xia Yin Prof. Ya You Prof. An Luo Prof. Sen Xin Prof. Xiong-Wei Wu Prof. Yu-Guo Guo College of Electrical and Information Engineering Hunan University Changsha Hunan 410082 P. R. China School of Chemistry and Materials Science College of Agronomy Hunan Agricultural University Changsha Hunan 410128 P. R. China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences (CAS) Beijing 100190 P. R. China Nanozyme Medical Center School of Basic Medical Sciences Zhengzhou University Zhengzhou 450001 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei P. R. China

Rechargeable lithium–metal batteries with a cell-level specific energy of >400 Wh kg −1 are highly desired for next-generation storage applications, yet the research has been retarded by poor electrolyte–electrode compatibility and rigorous safety concerns. We demonstrate that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the nickel-rich layered oxide cathodes. By employing the new electrolyte, Li∥LiNi 0.6 Co 0.2 Mn 0.2 O 2 cells show favorable cycling and rate performance, and a 10 Ah Li∥LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell demonstrates a practical specific energy of >450 Wh kg −1 . Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces toward practical realization of high-energy rechargeable batteries.

关键词： hybrid electrolytes in situ polymerization interfacial chemistry rechargeable lithium–metal batteries

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[email protected] 2 hybrid microcapsules with high in vivo biocompatibility and stability for cell therapy

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Colloids and Surfaces B: Biointerfaces 2021年 203卷

作者： Grégory Leroux Myriam Neumann Christophe F. Meunier Virginie Voisin Isabelle Habsch Nathalie Caron Carine Michiels Li Wang Bao-Lian Su Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Molecular Physiology Research Unit (URPhyM) Namur Research Institute for Life Sciences (NARILIS) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Laboratory of Biochemistry and Cell Biology (URBC) Namur Research Institute for Life Sciences (NARILIS) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Luoshi Road 122 Wuhan 430070 China

Designing new materials to encapsulate living therapeutic cells for the treatment of the diseases caused by protein or hormone deficiencies is a great challenge. The desired materials need to be biocompatible towards both entrapped cells and host organisms, have long-term in vivo stability after implantation, allow the diffusion of nutrients and metabolites, and ensure perfect immune-isolation. The current work investigates the in vivo biocompatibility and stability of [email protected] 2 hybrid microcapsules and the immune-isolation of entrapped HepG2 cells, to assess their potential for cell therapy. A comparison was made with alginate-silica hybrid microcapsules (ASA). These two hybrid microcapsules are implanted subcutaneously in female Wistar rats. The inflammatory responses of the rats are monitored by the histological examination of the implants and the surrounding tissues, to indicate their in vivo biocompatibility towards the hosts. The in vivo stability of the microcapsules is evaluated by the recovery rate of the intact microcapsules after implantation. The immune-isolation of the entrapped cells is assessed by their morphology, membrane integrity and intracellular enzymatic activity. The results show high viability of the entrapped cells and insignificant inflammation of the hosts, suggesting the excellent biocompatibility of [email protected] 2 and ASA microcapsules towards both host organisms and entrapped cells. Compared to the ASA microcapsules, more intact [email protected] 2 hybrid microcapsules are recovered 2-day and 2-month post-implantation and more cells remain alive, proving their better in vivo biocompability, stability, and immune-isolation. The present study demonstrates that the [email protected] 2 hybrid microcapsule is a highly promising implantation material for cell therapy.

关键词： Hybrid hydrogels Cell encapsulation In vivo biocompatibility In vivo stability Immune isolation

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Solid Electrolytes: A New Lithium‐Ion Conductor LiTaSiO5: Theoretical Prediction, materials synthesis, and Ionic Conductivity (Adv. Funct. Mater. 37/2019)

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advanced Functional materials 2019年第37期29卷

作者： Qi Wang Jian‐Fang Wu Ziheng Lu Francesco Ciucci Wei Kong Pang Xin Guo State Key Laboratory of Material Processing and Die & Mould Technology Laboratory of Solid State Ionics School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 P. R. China School of Optical and Electronic Information Huazhong University of Science and Technology Wuhan 430074 P. R. China Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and Technology Clear Water Bay Hong Kong P. R. China Center for Information Photonics and Energy Materials Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 P. R. China Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology Clear Water Bay Hong Kong P. R. China Institute for Superconducting & Electronic Materials University of Wollongong Wollongong New South Wales 2522 Australia

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Front Cover: Molecular Engineering of Zinc-Porphyrin Sensitisers for p-Type Dye-Sensitised Solar Cells (ChemPlusChem 7/2018)

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ChemPlusChem 2018年第7期83卷 542-542页

作者： Dr. Jianfeng Lu Dr. Zonghao Liu Narendra Pai Liangcong Jiang Prof. Dr. Udo Bach Dr. Alexandr N. Simonov Prof. Dr. Yi-Bing Cheng Prof. Dr. Leone Spiccia School of Chemistry Monash University Clayton Victoria 3800 Australia School of Optical and Electronic Information Huazhong University of Science and Technology Wuhan 430074 China Department of Materials Science and Engineering Monash University Clayton Victoria 3800 Australia Department of Chemical Engineering Monash University Clayton Victoria 3800 Australia CSIRO Clayton Victoria 3168 Australia ARC Centre of Excellence for Exciton Science Monash University Clayton Victoria 3800 Australia ARC Centre of Excellence for Electromaterials Science Monash University Clayton Victoria 3800 Australia State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Deceased December 2016

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3D Ferroconcrete‐Like Aminated Carbon Nanotubes Network Anchoring Sulfur for advanced Lithium–Sulfur Battery

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advanced Energy materials 2018年第25期8卷

作者： Min Yan Hao Chen Yong Yu Heng Zhao Chao‐Fan Li Zhi‐Yi Hu Pan Wu Lihua Chen Hongen Wang Dongliang Peng Huanxin Gao Tawfique Hasan Yu Li Bao‐Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Department of Materials Science and Engineering College of Materials Xiamen University 422 Siming South Road Xiamen 361005 China Fundamental Research Department SINOPEC Shanghai Research Institute of Petrochemical Technology 165 Pudong Bei Road Shanghai 201208 China Cambridge Graphene Centre University of Cambridge 9 JJ Thomson Avenue Cambridge CB3 0FA UK Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B‐5000 Namur Belgium Clare Hall University of Cambridge Herschel Road Cambridge CB3 9AL UK

To address the serious capacity fading in lithium–sulfur batteries, a 3D ferroconcrete‐like aminated carbon nanotubes network with polyaniline coating as an effective sulfur host to contain polysulfide dissolution is presented here. In this composite, the cross‐linked aminated carbon nanotubes framework provides a fast charge transport pathway and enhancement in the reaction kinetics of the active material to greatly improve the rate capability and sulfur utilization. The ethylenediamine moieties provide strong adhesion of polar discharge products to nonpolar carbon surfaces and thus efficiently prevent polysulfide dissolution to improve the cycle stability, confirmed by density functional theory calculations. The outside polyaniline layers structurally restrain polysulfides to prevent the shuttle effect and active material loss. Benefiting from these advantages, the synthesized composite exhibits a high initial capacity of 1215 mAh g −1 and a capacity of 975 mAh g −1 after 200 cycles at 0.2 C. Even after 200 cycles at 0.5 C, a capacity of 735 mAh g −1 can be maintained, among the best performance reported. The strategy in this work can shed some light on modifying nonpolar carbon surfaces via the amination process to chemically attach sulfur species for high‐performance lithium–sulfur batteries.

关键词： carbon nanotubes density functional theory ethylenediamine modification Li–S battery polyaniline

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Rapid Charge Transfer Endowed by Interfacial Ni-O Bonding in S-scheme Heterojunction for Efficient Photocatalytic H2and Imine Production

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Bowen He Dr. Peng Xiao Dr. Sijie Wan Dr. Jianjun Zhang Prof. Tao Chen Prof. Liuyang Zhang Prof. Jiaguo Yu Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street Wuhan 430078 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Methodology (lead) Writing - original draft (equal) Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China Hefei Anhui 230026 China Contribution: Data curation (equal) Formal analysis (equal) State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Contribution: Formal analysis (supporting) Methodology (supporting) Software (lead) Contribution: Methodology (supporting) Validation (supporting) Contribution: Methodology (supporting) Resources (supporting) Contribution: Formal analysis (equal) Funding acquisition (equal) Supervision (supporting) Writing - review & editing (lead)

Cooperative coupling of H 2 evolution with oxidative organic synthesis is promising in avoiding the use of sacrificial agents and producing hydrogen energy with value-added chemicals simultaneously. Nonetheless, the photocatalytic activity is obstructed by sluggish electron-hole separation and limited redox potentials. Herein, Ni-doped Zn 0.2 Cd 0.8 S quantum dots are chosen after screening by DFT simulation to couple with TiO 2 microspheres, forming a step-scheme heterojunction. The Ni-doped configuration tunes the highly active S site for augmented H 2 evolution, and the interfacial Ni−O bonds provide fast channels at the atomic level to lower the energy barrier for charge transfer. Also, DFT calculations reveal an enhanced built-in electric field in the heterojunction for superior charge migration and separation. Kinetic analysis by femtosecond transient absorption spectra demonstrates that expedited charge migration with electrons first transfer to Ni 2+ and then to S sites. Therefore, the designed catalyst delivers drastically elevated H 2 yield (4.55 mmol g −1 h −1 ) and N-benzylidenebenzylamine production rate (3.35 mmol g −1 h −1 ). This work provides atomic-scale insights into the coordinated modulation of active sites and built-in electric fields in step-scheme heterojunction for ameliorative photocatalytic performance.

关键词： Benzylamine Coupling Oxidation Hydrogen Production Interfacial Charge Transfer S-Scheme Photocatalyst

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Regulating Non-Equilibrium Solvation Structure in Locally Concentrated Ionic Liquid Electrolytes for Wide-Temperature and High-Voltage Lithium Metal Batteries

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Angewandte Chemie 2024年第1期137卷

作者： Haifeng Tu Zhicheng Wang Jiangyan Xue Zhiyong Tang Yang Liu Xiaofang Liu Lingwang Liu Suwan Lu Shixiao Weng Yiwen Gao Guochao Sun Zheng Liu keyang Peng Xin Zhang Dejun Li Guangye Wu Meinan Liu Jianchen Hu Hong Li Jingjing Xu Xiaodong Wu School of Nano-Tech and Nano-Bionics University of Science and Technology of China Hefei Anhui 230026 China i-lab Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Suzhou Jiangsu 215123 China These authors contributed equally to this work: Haifeng Tu Zhicheng Wang Institute of Physics Chinese Academy of Sciences Beijing 100190 China Tianmu Lake Institute of Advanced Energy Storage Technologies Liyang 213300 China Jiangxi Key Laboratory of Flexible Electronics Jiangxi Science & Technology Normal University Nanchang 330013 Jiangxi China 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 Materials School of Resources Environment and Materials Guangxi University Nanning 530004 China National Engineering Laboratory for Modern Silk College of Textile and Clothing Engineering Research Center of Cooperative Innovation for Functional Organic/Polymer Material Micro/Nanofabrication Soochow University Suzhou 215123 China College of Material Science and Engineering Hohai University Nanjing Jiangsu 210024 China

The development of high-voltage lithium metal batteries (LMBs) encounters significant challenges due to aggressive electrode chemistry. Recently, locally concentrated ionic liquid electrolytes (LCILEs) have garnered attention for their exceptional stability with both Li anodes and high-voltage cathodes. However, there remains a limited understanding of how diluents in LCILEs affect the thermodynamic stability of the solvation structure and transportation dynamics of Li + ions. Herein, we propose a wide-temperature LCILEs with 1,3-dichloropropane (DCP13) diluent to construct a non-equilibrium solvation structure under external electric field, wherein the DCP13 diluent enters the Li + ion solvation sheath to enhance Li + ion transport and suppress oxidative side reactions at high-nickel cathode (LiNi 0.9 Co 0.05 Mn 0.05 O 2 , NCM90). Consequently, a Li/NCM90 cell utilizing this LCILE achieves a high capacity retention of 94 % after 240 cycles at 4.3 V, also operates stably at high cut-off voltages from 4.4 V to 4.6 V and over a wide temperature range from −20 °C to 60 °C. Additionally, an Ah-level pouch cell with this LCILE simultaneously achieves high-energy-density and stable cycling, manifesting the practical feasibility. This work redefines the role of diluents in LCILEs, providing inspiration for electrolyte design in developing high-energy-density batteries.

关键词： Lithium metal batteries locally concentrated ionic liquid electrolyte chloroalkane diluent non-equilibrium solvation structure external electric field

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In Situ X-ray Absorption Spectroscopy of Metal/Nitrogen-doped Carbons in Oxygen Electrocatalysis

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Angewandte Chemie 2023年第27期135卷

作者： Bin Wu Tianxiao Sun Ya You Haibing Meng Dulce M. Morales Mailis Lounasvuori Abbas Beheshti Askari Li Jiang Feng Zeng Baoshan Hu Xiangzhi Zhang Renzhong Tai Zhichuan J. Xu Tristan Petit Liqiang Mai Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Straße 15 12489 Berlin Germany Institute of Physics Humboldt University Berlin Newton-Straße 15 12489 Berlin Germany State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Luoshi Road 122 Wuhan 430070 China College of Chemistry Taiyuan University of Technology Taiyuan 030024 China Chemical Engineering group Engineering and Technology institute Groningen (ENTEG) Faculty of Science and Engineering University of Groningen Nijenborgh 4 9747 AG Groningen The Netherlands CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences (CAS) Beijing 100190 China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Nanjing 211816 China College of Chemistry and Chemical Engineering Chongqing University Chongqing 401331 (China) Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore

Metal/nitrogen-doped carbons (M−N−C) are promising candidates as oxygen electrocatalysts due to their low cost, tunable catalytic activity and selectivity, and well-dispersed morphologies. To improve the electrocatalytic performance of such systems, it is critical to gain a detailed understanding of their structure and properties through advanced characterization. In situ X-ray absorption spectroscopy (XAS) serves as a powerful tool to probe both the active sites and structural evolution of catalytic materials under reaction conditions. In this review, we firstly provide an overview of the fundamental concepts of XAS and then comprehensively review the setup and application of in situ XAS, introducing electrochemical XAS cells, experimental methods, as well as primary functions on catalytic applications. The active sites and the structural evolution of M−N−C catalysts caused by the interplay with electric fields, electrolytes and reactants/intermediates during the oxygen evolution reaction and the oxygen reduction reaction are subsequently discussed in detail. Finally, major challenges and future opportunities in this exciting field are highlighted.

关键词： Active Sites In Situ XAS M−N−C Catalysts Oxygen Electrocatalysis Structural Evolution

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Ferromagnetic materials: Strong Ferromagnetism Achieved via Breathing Lattices in Atomically Thin Cobaltites (Adv. Mater. 4/2021)

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advanced materials 2021年第4期33卷

作者： Sisi Li Qinghua Zhang Shan Lin Xiahan Sang Ryan F. Need Manuel A. Roldan Wenjun Cui Zhiyi Hu Qiao Jin Shuang Chen Jiali Zhao Jia-Ou Wang Jiesu Wang Meng He Chen Ge Can Wang Hui-Bin Lu Zhenping Wu Haizhong Guo Xin Tong Tao Zhu Brian Kirby Lin Gu Kui-juan Jin Er-Jia Guo Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences Beijing 100190 China State Key Laboratory of Information Photonics and Optical Communications and Laboratory of Optoelectronics Materials and Devices School of Science Beijing University of Posts and Telecommunications Beijing 100876 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & Nanostructure research center Wuhan University of Technology 122 Luoshi Rd. Wuhan 430070 China NIST Center for Neutron Research National Institute of Standards and Technology (NIST) Gaithersburg MD 20899 USA Department of Materials Science and Engineering University of Florida Gainesville FL 32611 USA Eyring Materials Center Arizona State University Tempe AZ 85287 USA School of Physics and Microelectronics Zhengzhou University Zhengzhou 450052 China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Songshan Lake Materials Laboratory Dongguan Guangdong 523808 China China Spallation Neutron Source Institute of High Energy Physics Chinese Academy of Sciences Beijing 10049 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China

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Three-dimensionally ordered macroporous materials for photo/electrocatalytic sustainable energy conversion, solar cell and energy storage

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EnergyChem 2022年第4期4卷

作者： Yang Ding Chunhua Wang Runtian Zheng Soumyajit Maitra Genwei Zhang Tarek Barakat Subhasis Roy Bao-Lian Su Li-Hua Chen Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Department of Chemistry KU Leuven Celestijnenlaan 200F B-3001 Leuven Belgium Department of Chemical Engineering University of Calcutta 92 APC Road Kolkata West Bengal 700009 India Department of Chemistry Fudan University 2005 Songhu Road 200438 Shanghai China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Clare Hall University of Cambridge Cambridge CB2 1EW UK

Three-dimensionally ordered macroporous (3DOM) materials have aroused tremendous interest in solar light to energy conversion, sustainable and renewable products generation, and energy storage fields owing to their convenient mass transfer channels, high surface area, enhanced interaction between matter and light, plentiful reactive sites as well as tunable composition. In this review, the state-of-the-art 3DOM materials as well as their preparation methods and the relevant applications including photo/electrocatalytic sustainable energy conversion, solar cells, Li ion batteries and supercapacitor are thoroughly outlined. Meanwhile, the unique merits and mechanisms for 3DOM materials in various applications are revealed and discussed in depth. Moreover, the strategies for designing 3DOM materials and the enhanced performance for applications are correlated, which can be significantly valuable to help readers to promptly acquire the comprehensive knowledge and to inspire some new ideas in developing 3DOM materials for further improved performances. Finally, the challenges and perspectives of 3DOM materials for sustainable energy conversion/production, solar cells and energy storage fields are outlooked. We sincerely look forward to that this critical review can facilitate the fast developments in designing highly efficient 3DOM materials and the relevant applications.

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