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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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Hierarchial Zeolites: Beyond Creation of Mesoporosity: The Advantages of Polymer‐Based Dual‐Function Templates for Fabricating Hierarchical Zeolites (Adv. Funct. Mater. 12/2016)

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advanced Functional materials 2016年第12期26卷

作者： Qiwei Tian Zhaohui Liu Yihan Zhu Xinglong Dong Youssef Saih Jean‐Marie Basset Miao Sun Wei Xu Liangkui Zhu Daliang Zhang Jianfeng Huang Xiangju Meng Feng‐Shou Xiao Yu Han King Abdullah University of Science and Technology (KAUST) Advanced Membranes and Porous Materials Center (AMPMC) Physical Sciences and Engineering Division (PSE) Thuwal 23955‐6900 Saudi Arabia King Abdullah University of Science and Technology (KAUST) KAUST Catalysis Center (KCC) Physical Sciences and Engineering Division (PSE) Thuwal 23955‐6900 Saudi Arabia Cooperate Research and Development Center King Abdullah University of Science and Technology Saudi Aramco Thuwal 23955‐6900 Saudi Arabia Department of Chemistry State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University Changchun 130012 China Imaging and Characterization Core Laboratory King Abdullah University of Science and Technology Thuwal 23955‐6900 Saudi Arabia Key Lab of Applied Chemistry of Zhejiang Province Department of Chemistry Zhejiang University Hangzhou 310028 P. R. China

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Tuning Adsorbate-Mediated Strong Metal-Support Interaction by Oxygen Vacancy: A Case Study in Ru/TiO2

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Angewandte Chemie 2024年第31期136卷

作者： Juan Li Lin Zhang Prof. Xingda An Prof. Kai Feng Dr. Xuchun Wang Jiari He Prof. Yang Huang Prof. Jingjing Liu Prof. Liang Zhang Prof. Binhang Yan Prof. Chaoran Li Prof. Le He Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou 215123 Jiangsu PR China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 Jiangsu PR China Department of Chemistry Soochow University-Western University Centre for Synchrotron Radiation Research University of Western Ontario London N6 A 5B7 Ontario Canada State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics (LICP) Chinese Academy of Sciences Lanzhou 730000 China. Institute of Information Technology Suzhou Institute of Trade and Commerce Suzhou 215009 Jiangsu PR China Department of Chemical Engineering Tsinghua University Beijing 100084 P. R. China Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Suzhou 215123 Jiangsu PR China

The adsorbate-mediated strong metal-support interaction (A-SMSI) offers a reversible means of altering the selectivity of supported metal catalysts, thereby providing a powerful tool for facile modulation of catalytic performance. However, the fundamental understanding of A-SMSI remains inadequate and methods for tuning A-SMSI are still in their nascent stages, impeding its stabilization under reaction conditions. Here, we report that the initial concentration of oxygen vacancy in oxide supports plays a key role in tuning the A-SMSI between Ru nanoparticles and defected titania (TiO 2-x ). Based on this new understanding, we demonstrate the in situ formation of A-SMSI under reaction conditions, obviating the typically required CO 2 -rich pretreatment. The as-formed A-SMSI layer exhibits remarkable stability at various temperatures, enabling excellent activity, selectivity and long-term stability in catalyzing the reverse water gas-shift reaction. This study deepens the understanding of the A-SMSI and the ability to stabilize A-SMSI under reaction conditions represents a key step for practical catalytic applications.

关键词： SMSI oxygen vacancy heterogeneous catalysis CO2 hydrogenation adsorbate mediation

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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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Mg-Pillared LiCoO2: Towards Stable Cycling at 4.6 V

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Angewandte Chemie 2020年第9期133卷

作者： Yangyang Huang Yongcheng Zhu Dr. Haoyu Fu Mingyang Ou Dr. Chenchen Hu Sijie Yu Prof. Zhiwei Hu Prof. Chien-Te Chen Prof. Gang Jiang Hongkai Gu Prof. He Lin Prof. Wei Luo Prof. Yunhui Huang Institute of New Energy for Vehicles School of Materials Science and Engineering Tongji University Shanghai 201804 P. R. China Institute of Atomic and Molecular Physics Sichuan University Chengdu 610065 China State Key Laboratory of Material Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China Max Planck Institute for Chemical Physics of Solids Nöthnitzer Strasse 40 01187 Dresden Germany National Synchrotron Radiation Research Center 101 Hsin-Ann Road Hsinchu 30076 Taiwan Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201804 China

LiCoO 2 is used as a cathode material for lithium-ion batteries, however, cationic/anodic-redox-induced unstable phase transitions, oxygen escape, and side reactions with electrolytes always occur when charging LiCoO 2 to voltages higher than 4.35 V, resulting in severe capacity fade. Reported here is Mg-pillared LiCoO 2 . Dopant Mg ions, serving as pillars in the Li-slab of LiCoO 2 , prevent slab sliding in a delithiated state, thereby suppressing unfavorable phase transitions. Moreover, the resulting Li-Mg mixing structure at the surface of Mg-pillared LiCoO 2 is beneficial for eliminating the cathode-electrolyte interphase overgrowth and phase transformation in the close-to-surface region. Mg-pillared LiCoO 2 exhibits a high capacity of 204 mAh g −1 at 0.2 C and an enhanced capacity retention of 84 % at 1.0 C over 100 cycles within the voltage window of 3.0–4.6 V. In contrast, pristine LiCoO 2 has a capacity retention of 14 % within the same voltage window.

关键词： cathodes doping lithium magnesium materials science

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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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Heterogenised Molecular Catalysts for Sustainable Electrochemical CO2Reduction

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Angewandte Chemie 2022年第38期134卷

作者： Dr. Domenico Grammatico Andrew J. Bagnall Ludovico Riccardi Prof. Marc Fontecave Prof. Bao-Lian Su Prof. Laurent Billon Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles 5000 Namur Belgium Bio-inspired Materials Group: Functionality & Self-assembly Universite de Pau et des Pays de l'Adour E2S UPPA CNRS IPREM UMR 5254 64000 Pau France Present address: Energy Conversion and Hydrogen Center for Energy Austrian Institute of Technology GmbH Giefinggasse 2 1210 Vienna Austria Department of Chemistry Ångström Laboratories Uppsala University Box 523 751 20 Uppsala Sweden Laboratoire de Chimie et Biologie des Métaux Univ. Grenoble Alpes CNRS CEA IRIG 17 Rue des Martyrs 38054 Grenoble Cedex France Molecular Materials and Nanosystems Institute for Complex Molecular Systems Eindhoven University of Technology 5600 MB Eindhoven The Netherlands Laboratoire de Chimie des Processus Biologiques UMR CNRS 8229 Collège de France-CNRS-Sorbonne Université PSL Research University 11 Place Marcelin Berthelot 75005 Paris France State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China

There has been a rapid rise in interest regarding the advantages of support materials to protect and immobilise molecular catalysts for the carbon dioxide reduction reaction (CO 2 RR) in order to overcome the weaknesses of many well-known catalysts in terms of their stability and selectivity. In this Review, the state of the art of different catalyst-support systems for the CO 2 RR is discussed with the intention of leading towards standard benchmarking for comparison of such systems across the most relevant supports and immobilisation strategies, taking into account these multiple pertinent metrics, and also enabling clearer consideration of the necessary steps for further progress. The most promising support systems are described, along with a final note on the need for developing more advanced experimental and computational techniques to aid the rational design principles that are prerequisite to prospective industrial upscaling.

关键词： Carbon Dioxide Reduction Electrochemical Reduction Heterogenization Molecular Catalysts Solar Fuels

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Over 19 % Efficiency Organic Solar Cells Enabled by Manipulating the Intermolecular Interactions through Side Chain Fluorine Functionalization

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Angewandte Chemie 2024年第15期136卷

作者： Prof. Huawei Hu Shuai Liu Jiaoyu Xu Dr. Ruijie Ma Dr. Zhengxing Peng Top Archie Dela Peña Dr. Yongjie Cui Wenting Liang Xiaoli Zhou Dr. Siwei Luo Dr. Han Yu Prof. Mingjie Li Prof. Jiaying Wu Prof. Shangshang Chen Prof. Gang Li Prof. Yiwang Chen State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai 201620 P. R. China Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis Jiangxi Normal University 99 Ziyang Avenue Nanchang 330022 P. R. China Department of Electrical and Electronic Engineering Research Institute for Smart Energy (RISE) Guangdong-Hong Kong-Macao (GHM) Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 999077 P. R. China Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA Function Hub Advanced Materials Thrust The Hong Kong University of Science and Technology Nansha 511400 Guangzhou P. R. China The Hong Kong Polytechnic University Faculty of Science Department of Applied Physics Kowloon Hong Kong 000000 P. R. China Department of Chemistry Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong 999077 P. R. China School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 P. R. China

Fluorine side chain functionalization of non-fullerene acceptors (NFAs) represents an effective strategy for enhancing the performance of organic solar cells (OSCs). However, a knowledge gap persists regarding the relationship between structural changes induced by fluorine functionalization and the resultant impact on device performance. In this work, varying amounts of fluorine atoms were introduced into the outer side chains of Y-series NFAs to construct two acceptors named BTP-F0 and BTP-F5. Theoretical and experimental investigations reveal that side-chain fluorination significantly increase the overall average electrostatic potential (ESP) and charge balance factor, thereby effectively improving the ESP-induced intermolecular electrostatic interaction, and thus precisely tuning the molecular packing and bulk-heterojunction morphology. Therefore, the BTP-F5-based OSC exhibited enhanced crystallinity, domain purity, reduced domain spacing, and optimized phase distribution in the vertical direction. This facilitates exciton diffusion, suppresses charge recombination, and improves charge extraction. Consequently, the promising power conversion efficiency (PCE) of 17.3 % and 19.2 % were achieved in BTP-F5-based binary and ternary devices, respectively, surpassing the PCE of 16.1 % for BTP-F0-based OSCs. This work establishes a structure-performance relationship and demonstrates that fluorine functionalization of the outer side chains of Y-series NFAs is a compelling strategy for achieving ideal phase separation for highly efficient OSCs.

关键词： non-fullerene acceptors fluorine functionalization intermolecular interactions solar cells molecular packing

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

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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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Enhanced exchange bias in all-oxide heterostructures with cation-ordered ferrimagnetic double-perovskite

npj Spintronics

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npj Spintronics 2024年第1期2卷 1-6页

作者： Xiaofu Qiu Hetian Chen Yuhan Liang Xiaoyu Jiang Jing Ma Di Yi Zelin Wang Tianxiang Nan Yujun Zhang Fangyuan Zhu Zhen Chen State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China School of Integrated Circuits Beijing National Research Center for Information Science and Technology Tsinghua University Beijing 100084 China National Center for Electron Microscopy in Beijing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing 100049 China

The realization and control of exchange bias (EB) are highly desirable for spintronic applications. All-oxide heterostructures comprised of ferromagnetic and antiferromagnetic/multiferroic oxides provide an ideal platform to enable the electric-field control of EB, promising for energy-efficient memory and logic devices. However, the low block temperature (TB) and small bias field (HEB) hinder further advances towards room-temperature applications. Here, we report an alternative approach to enhance the interface-induced EB by using ferrimagnetic double-perovskite with B-site cation ordering. In heterostructures comprised of double-perovskite Sr2FeReO6(SFRO) and LaFeO3(LFO), a high TB(about 250 K) and large HEBare observed, which is significantly larger than the counterparts with LFO and ferromagnetic oxides. Further analysis suggests that the cation-ordering and ferrimagnetic spin structure of the double-perovskite could contribute significantly to the enhanced exchanged bias when interfacing with G-type antiferromagnets. Our results open a new avenue for developing all-oxides heterostructures for future magnetic technologies.

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