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The Nature of Structural Defects in ZIF-8 Revealed with1H and31P MAS NMR and X-Ray Absorption Spectroscopy

Angewandte Chemie 2024年第2期137卷

作者： Dr. Anton A. Gabrienko Dr. Somboon Chaemchuen Dr. Zongkui Kou Prof. Naoki Ogiwara Prof. Hiroshi Kitagawa Dr. Alexander E. Khudozhitkov Prof. Alexander G. Stepanov Dr. Daniil I. Kolokolov Prof. Francis Verpoort Boreskov Institute of Catalysis Novosibirsk Ac. Lavrentiev av. 5 Novosibirsk 630090 Russia Both authors contributed equally State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Department of Chemical Engineering Faculty of Engineering Mahidol University Nakhon Pathom 73170 Thailand Department of Basic Science School of Arts and Sciences The University of Tokyo 3-8-1 Komaba Meguro-ku Tokyo 153-8902 Japan Division of Chemistry Graduate School of Science Kyoto University Kitashirakawa-Oiwakecho Sakyo-ku Kyoto 606-8502 Japan School of Chemistry and Chemical Engineering Shandong University of Technology Zibo 255049 China Joint Institute of Chemical Research (FFMiEN) Peoples Friendship University of Russia (RUDN University) 6 Miklukho-Maklaya Str. 117198 Moscow Russia

The metal–organic frameworks (MOFs) attract interest as potential catalysts whose catalytic properties are driven by defects. Several methods have been proposed for the defects-inducing synthesis of MOFs. However, the active species formed on the defective sites remain elusive and uncharacterized, as the spectroscopic fingerprints of these species are hidden by the regular structure signals. In this work, we have performed the synthesis of ZIF-8 MOF with defect-inducing procedures using fully deuterated 2-methylimidazolate ligands to enhance the defective sites′ visibility. By combining 1 H and 31 P MAS NMR spectroscopy and X-ray absorption spectroscopy, we have found evidence for the presence of different structural hydroxyl Zn−OH groups in the ZIF-8 materials. It is demonstrated that the ZIF-8 defect sites are represented by Zn−OH hydroxyl groups with the signals at 0.3 and −0.7 ppm in the 1 H MAS NMR spectrum. These species are of basic nature and may be responsible for the catalytic activity of the ZIF-8 material.

关键词： metal–organic framework defects solid state NMR XAS catalysis

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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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Regulating the Mechanical and Optical Properties of Polymer-based Nanocomposites by Sub-Nanowires

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Angewandte Chemie 2022年第5期135卷

作者： Feng Yuan Dr. Chen Ouyang Minzheng Yang Prof. Wenxiong Shi Dr. Weibin Ren Prof. Yang Shen Prof. Yan Wei Prof. Xuliang Deng Prof. Xun Wang Institute of Medical Technology Peking University Health Science Center Beijing 100191 China Beijing Laboratory of Biomedical Materials Department of Geriatric Dentistry Peking University School and Hospital of Stomatology Beijing 100081 China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China Contribution: Software (supporting) Contribution: Formal analysis (supporting) Contribution: Formal analysis (supporting) Supervision (supporting) Contribution: Conceptualization (equal) Formal analysis (lead) Supervision (lead) Contribution: Conceptualization (lead) Supervision (lead) Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Methodology (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Sub-nanowires (SNWs) exhibit great potential applications in nanocomposites owing to their high specific surface area, high flexibility, and similarity to polymer chains in dimension, which are a good entry point to bridge inorganic materials and polymer materials. Herein, we synthesized hydroxyapatite sub-nanowires (HAP SNWs) and engineered hydroxyapatite sub-nanowires/polyimide (HSP) gels and films by simple mixing of HAP SNWs and polyimide (PI). Benefiting from the interactions between HAP SNWs and PI, these nanocomposites were a continuous hybrid network. As the increase of HAP SNWs contents, the viscosity and modulus of HSP gels were greatly improved by one or two orders of magnitude compared with PI gel. HSP films not only maintained high transparency but also gained high haze, as well as exhibited enhanced Young's modulus. Thus, both HSP gels and films developed in this work are promising for various applications in coatings and high-performance films.

关键词： Gels Nanocomposites Nanowires Thin Films

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H2-free Semi-hydrogenation of Butadiene by the Atomic Sieving Effect of Pd Membrane with Tree-like Pd Dendrites Array

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Angewandte Chemie 2023年第38期135卷

作者： Yong-Qing Yan Zhao Wei Prof. Zhao Wang Yao Li Wei-Hao Wang Bo Jiang Prof. Bao-Lian Su Laboratory of Living Materials the State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Validation (equal) Writing - original draft (equal) Writing - review & editing (equal) Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Guangdong Laboratory Xianhu Hydrogen Valley Foshan 528200 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Writing - original draft (supporting) Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles 5000 Namur Belgium

H 2 -free semi-hydrogenation at room temperature shows great advantage for replacing the thermocatalytic process in industry owing to the high energy and resource saving, however, remains great challenges. Herein, a tree-like Pd dendrites array decorated Pd membrane was constructed as the core device in an electrochemistry assisted gas-fed membrane reactor for butadiene semi-hydrogenation. It reveals that hydrogen atomic sieving effect of this Pd-based membrane under electrochemical condition was the key for semi-hydrogenation. The configuration study of Pd nanostructured membrane demonstrates that the penetration of hydrogen atoms through Pd membrane from electrochemical side to chemical side is affected by the consumption of hydrogen atom in semi-hydrogenation step. Such atomic sieving property of nanostructured Pd membrane with 5.1 times increase in catalytic active surface area brings above 14 times higher in butadiene conversion than that of bare Pd foil, with ≈90 % of butenes selectivity at butadiene conversion ≈98 % over 300 h of H 2 -free reaction under 15 mA cm −2 .

关键词： 1,3-Butadiene Pd Membrane Semi-Hydrogenation Unsaturated Hydrocarbons Water Electrolysis

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Flux creep relaxation in single crystal Hg-1201

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Journal of Physics: Conference Series 2010年第1期234卷

作者： M Baenitz K Lüders N Barišič Y Cho Y Li G Yu X Zhao M Greven Max-Planck-Institut für Chemische Physik fester Stoffe Nöthnitzer Str. 40 01187 Dresden Germany Freie Universität Berlin Fachbereich Physik Arnimallee 14 14195 Berlin Germany T.H. Geballe Laboratory for Advanced Materials Stanford University Stanford California 94305 USA 1. Physikalisches Institut Universität Stuttgart Pfaffenwaldring 57 70550 Stuttgart Germany BK21 Team of Nano Fusion Technology Pusan National University Miryang 627-706 Republic of Korea Department of Physics Stanford University Stanford California 94305 USA State Key Lab of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University 2699 Qianjin Street Changchun 130012 PR China Department of Applied Physics Stanford University Stanford California USA

Magnetization measurements on a single crystal of the high-Tc cuprate HgBa2CuO4 (Hg-1201) are performed for the two field orientations B||c and B||(a,b). Besides zero-field-cooling (zfc) – field-cooling (fc) and magnetization studies, the flux creep relaxation is determined. The zfc curves exhibit pronounced step-like anomalies in the mixed state above the lower critical field Bc1. They are interpreted as those points in the phase diagram where the penetrating flux fronts meet at the center of the sample. In order to obtain more information about the flux pinning mechanism flux creep relaxation experiments are performed at different temperatures in magnetic fields of 0.15 and 2 T. The resulting supercurrent dependence on the mean activation energy is analysed according to the collective pinning theory which predicts U ∝ ((j/jc)−μ −1). The μ-values for B||c are 0.5 at higher temperatures and 2 at 5 K, and they vary between 1.1 and 1.5 for B||(a,b). The observed behaviour is quite different from that found for powder samples.

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Frontispiece: Subnanometer Bimetallic Platinum–Zinc Clusters in Zeolites for Propane Dehydrogenation

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Angewandte Chemie International Edition 2020年第44期59卷

作者： Dr. Qiming Sun Dr. Ning Wang Qiyuan Fan Lei Zeng Dr. Alvaro Mayoral Dr. Shu Miao Dr. Ruoou Yang Prof. Zheng Jiang Wei Zhou Dr. Jichao Zhang Tianjun Zhang Prof. Jun Xu Prof. Peng Zhang Prof. Jun Cheng Dong-Chun Yang Prof. Ran Jia Dr. Lin Li Prof. Qinghong Zhang Prof. Ye Wang Prof. Osamu Terasaki Prof. Jihong Yu State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P. R. China State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and Esters College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China Center for High-resolution Electron Microscopy (CħEM) School of Physical Science and Technology ShanghaiTech University Shanghai 201210 P. R. China JEOL (Beijing) Co. Ltd. Beijing 100080 P. R. China Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201800 P. R. China Wuhan Center for Magnetic Resonance State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Wuhan Institute of Physics and Mathematics Chinese Academy of Sciences Wuhan 430071 P. R. China Department of Chemistry Dalhousie University Halifax Nova Scotia B3H 4R2 Canada Institute of Theoretical Chemistry Jilin University Changchun 130023 P. R. China Electron Microscopy Center Jilin University Changchun 130012 P. R. China International Center of Future Science Jilin University Qianjin Street 2699 Changchun 130012 P. R. China

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Frontispiz: Subnanometer Bimetallic Platinum–Zinc Clusters in Zeolites for Propane Dehydrogenation

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Angewandte Chemie 2020年第44期132卷

作者： Qiming Sun Ning Wang Qiyuan Fan Lei Zeng Alvaro Mayoral Shu Miao Ruoou Yang Zheng Jiang Wei Zhou Jichao Zhang Tianjun Zhang Jun Xu Peng Zhang Jun Cheng Dong‐Chun Yang Ran Jia Lin Li Qinghong Zhang Ye Wang Osamu Terasaki Jihong Yu State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 P. R. China State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and Esters College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 P. R. China Center for High-resolution Electron Microscopy (CħEM) School of Physical Science and Technology ShanghaiTech University Shanghai 201210 P. R. China JEOL (Beijing) Co. Ltd. Beijing 100080 P. R. China Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201800 P. R. China Wuhan Center for Magnetic Resonance State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Wuhan Institute of Physics and Mathematics Chinese Academy of Sciences Wuhan 430071 P. R. China Department of Chemistry Dalhousie University Halifax Nova Scotia B3H 4R2 Canada Institute of Theoretical Chemistry Jilin University Changchun 130023 P. R. China Electron Microscopy Center Jilin University Changchun 130012 P. R. China International Center of Future Science Jilin University Qianjin Street 2699 Changchun 130012 P. R. China

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26th Annual Computational Neuroscience Meeting (CNS*2017): Part 3 Antwerp, Belgium. 15-20 July 2017 Abstracts

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BMC NEUROSCIENCE 2017年第Sup1期18卷 95-176页

作者： [Anonymous] Department of Neuroscience Yale University New Haven CT 06520 USA Department Physiology & Pharmacology SUNY Downstate Brooklyn NY 11203 USA NYU School of Engineering 6 MetroTech Center Brooklyn NY 11201 USA Kings County Hospital Center Brooklyn NY 11203 USA Departament de Matemàtica Aplicada Universitat Politècnica de Catalunya Barcelona 08028 Spain Institut de Neurobiologie de la Méditerrannée (INMED) INSERM UMR901 Aix-Marseille Univ Marseille France Center of Neural Science New York University New York NY USA Aix-Marseille Univ INSERM INS Inst Neurosci Syst Marseille France Laboratoire de Physique Théorique et Modélisation CNRS UMR 8089 Université de Cergy-Pontoise 95300 Cergy-Pontoise Cedex France Department of Mathematics and Computer Science ENSAT Abdelmalek Essaadi’s University Tangier Morocco Laboratory of Natural Computation Department of Information and Electrical Engineering and Applied Mathematics University of Salerno 84084 Fisciano SA Italy Department of Medicine University of Salerno 84083 Lancusi SA Italy Dipartimento di Fisica Università degli Studi Aldo Moro Bari and INFN Sezione Di Bari Italy Data Analysis Department Ghent University Ghent Belgium Coma Science Group University of Liège Liège Belgium Cruces Hospital and Ikerbasque Research Center Bilbao Spain BIOtech Department of Industrial Engineering University of Trento and IRCS-PAT FBK 38010 Trento Italy Department of Data Analysis Ghent University Ghent 9000 Belgium The Wellcome Trust Centre for Neuroimaging University College London London WC1N 3BG UK Department of Electronic Engineering NED University of Engineering and Technology Karachi Pakistan Blue Brain Project École Polytechnique Fédérale de Lausanne Lausanne Switzerland Departement of Mathematics Swansea University Swansea Wales UK Laboratory for Topology and Neuroscience at the Brain Mind Institute École polytechnique fédérale de Lausanne Lausanne Switzerland Institute of Mathematics

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