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Engineering a Local Free Water Enriched Microenvironment for Surpassing Platinum Hydrogen Evolution Activity

Angewandte Chemie 2022年第35期134卷

作者： Qunlei Wen Junyuan Duan Wenbin Wang Dr. Danji Huang Dr. Youwen Liu Dr. Yongliang Shi Prof. JiaKun Fang Prof. Anmin Nie Prof. Huiqiao Li Prof. Tianyou Zhai State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Conceptualization (equal) Investigation (lead) Writing - original draft (lead) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Investigation (supporting) Writing - original draft (supporting) State Key Lab of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Conceptualization (lead) Formal analysis (lead) Writing - review & editing (lead) Center for Spintronics and Quantum Systems State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and Engineering Xi'an Jiaotong University Xi'an Shanxi 710049 P. R. China Contribution: Investigation (lead) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Formal analysis (equal) Investigation (equal) Writing - review & editing (equal) Center for High Pressure Science State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao Hebei 066004 P. R. China Contribution: Formal analysis (equal) Contribution: Writing - review & editing (equal) Contribution: Conceptualization (supporting) Project administration (lead) Supervision (equal) Writing - review & editing (equal)

Manipulating the catalyst–electrolyte interface to push reactants into the inner Helmholtz plane (IHP) is highly desirable for efficient electrocatalysts, however, it has rarely been implemented due to the elusive electrochemical IHP and inherent inert catalyst surface. Here, we propose the introduction of local force fields by the surface hydroxyl group to engineer the electrochemical microenvironment and enhance alkaline hydrogen evolution activity. Taking a hydroxyl group immobilized Ni/Ni 3 C heterostructure as a prototype, we reveal that the local hydrogen bond induced by the surface hydroxyl group drags 4-coordinated hydrogen-bonded H 2 O molecules across the IHP to become free H 2 O and thus continuously supply reactants forcatalytic sites catalytic sites. In addition, the hydroxyl group coupled with the Ni/Ni 3 C heterostructure further lowers the water dissociation energy by polarization effects. As a direct outcome, hydroxyl-rich catalysts surpass Pt/C activity at high current density (500 mA cm −2 @ ≈276 mV) in alkaline medium.

关键词： Electrochemical Double Layer High Current Densities Hydrogen Evolution Local Hydrogen Bond Surface Hydroxyl

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Structural Modulation of Nanographenes Enabled by Defects, Size and Doping for Oxygen Reduction Reaction

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Angewandte Chemie 2024年第2期137卷

作者： Dr. Bin Wu Dr. Haibing Meng Xingbao Chen Ying Guo Li Jiang Xiaofeng Shi Dr. Jiexin Zhu Juncai Long Wenliang Gao Feng Zeng Dr. Wen-Jie Jiang Yongfa Zhu Dingsheng Wang Prof. Liqiang Mai Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Straße 15 12489 Berlin Germany Present address School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue 639798 Singapore Singapore Institute of Physics Humboldt University Berlin Newton-Straße 15 12489 Berlin Germany These authors contributed equally to this work College of Chemistry and Chemical Engineering Taiyuan University of Technology 030024 Taiyuan State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Luoshi Road 122 430070 Wuhan China 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) 100190 Beijing China School of Environment and Safety Engineering North University of China 030051 Taiyuan China College of Chemistry and Chemical Engineering Chongqing University Chongqing 400044 China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University 211816 Nanjing China Department of Chemical Engineering The University of Melbourne 3010 Melbourne Victoria Department of Chemistry Tsinghua University 100084 Beijing China

Nanographenes are among the fastest-growing materials used for the oxygen reduction reaction (ORR) thanks to their low cost, environmental friendliness, excellent electrical conductivity, and scalab.e synthesis. The perspective of replacing precious metal-based electrocatalysts with functionalized graphene is highly desirable for reducing costs in energy conversion and storage systems. Generally, the enhanced ORR activity of the nanographenes is typically deemed to originate from the heteroatom doping effect, size effect, defects effect, and/or their synergistic effect. All these factors can efficiently modify the charge distribution on the sp 2 -conjugated carbon framework, bringing about optimized intermediate adsorption and accelerated electron transfer steps during ORR. In this review, the fundamental chemical and physical properties of nanographenes are first discussed about ORR applications. Afterward, the role of doping, size, defects, and their combined influence in boosting nanographenes’ ORR performance is introduced. Finally, significant challenges and essential perspectives of nanographenes as advanced ORR electrocatalysts are highlighted.

关键词： Dopants Size Defects Graphene ORR

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An Anomalous Electron Configuration Among 3dTransition Metal Atoms

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Angewandte Chemie 2022年第7期135卷

作者： Zhexin Tang Tongtong Shang Han Xu Ting Lin Ang Gao Weiguang Lin Xinyan Li Shiyu Wang Botao Yu Fanqi Meng Qinghua Zhang Xuefeng Wang Dong Su Qingbo Meng Lijun Wu Lin Gu Ce-Wen Nan Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences 100190 Beijing P. R. China School of Physical Sciences University of Chinese Academy of Sciences 100049 Beijing P. R. China State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University 100084 Beijing P. R. China Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials Department of Materials Science and Engineering Tsinghua University 100084 Beijing P. R. China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of Sciences 100049 Beijing P. R. China Condensed Matter Physics and Materials Science Division Brookhaven National Laboratory 11973 Upton NY USA

Physical properties of materials are mainly determined by valence electron configurations, where different valence shells would induce divergent phenomena. In compounds containing Sc 2+ , 3 d electron occupancy is expected, the same as other transition metal atoms like Ti 3+ . But this situation still awaits experimental verification in inorganic materials. Here, we selected ScS to measure the valence electron density and orbital population of Sc 2+ through delicate quantitative convergent-beam electron diffraction. With the absence of 3 d orbital features around Sc-atom sites and the nearly bare population of t 2g orbital, the unintuitive occupation of 4 s orbital in Sc 2+ is concluded. It should be the first time to report such a special electron configuration in a transition metal compound, in which 4 s rather than 3 d orbital is preferred. Our findings reveal the distinct behavior of Sc and probable ways to modulate material properties by controlling electron orbitals.

关键词： Electron Configuration Electron Density Distribution Electron Microscopy Quantitative Convergent-Beam Electron Diffraction Scandium

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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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Publisher Correction:Vertical‑Aligned and Ordered‑Active Architecture of Heterostructured Fibers for High Electrochemical Capacitance

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advanced Fiber materials 2024年第6期6卷 1992-1992页

作者： Xiaolin Zhu Hui Qiu Yang Zhang Zengming Man Wangyang Lu Ningzhong Bao Guan Wu National Engineering Lab for Textile Fiber Materials and Processing Technology Zhejiang Sci-Tech UniversityHangzhou 310018People’s Republic of China Zhejiang Provincial Innovation Center of Advanced Textile Technology Shaoxing 312000People’s Republic of China State Key Laboratory of Materials‑Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009People’s Republic of China

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Author Correction: Real-space measurement of orbital electron populations for Li1-xCoO2

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Nature Communications 2022年第1期13卷 1页

作者： Tongtong Shang Dongdong Xiao Xiaohui Rong Ang Gao Ting Lin Zhexin Tang Xiaozhi Liu Xinyan Li Qinghua Zhang Ruijuan Xiao Xuefeng Wang Dong Su Yong-Sheng Hu Hong Li Lin Gu Fanqi Meng Ce-Wen Nan Yuren Wen Qian Yu Ze Zhang Vaclav Petricek Lijun Wu Yimei Zhu Jian-Min Zuo Jing Zhu Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 P. R. China School of Physical Sciences University of Chinese Academy of Sciences Beijing 100049 China Songshan Lake Materials Laboratory Dongguan 523808 P. R. China State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 P. R. China School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 P. R. China Department of Materials Science and Engineering Center of Electron Microscopy and State Key Laboratory of Silicon Materials Zhejiang University Hangzhou 310027 P. R. China Institute of Physics Academy of Sciences of the Czech Republic Praha 180 40 Czech Republic Condensed Matter Physics and Materials Science Division Brookhaven National Laboratory Upton New York 11973 USA Department of Materials Science and Engineering University of Illinois at Urbana Champaign 1304 W Green St Urbana 61801 USA Beijing National Center for Electron Microscopy Laboratory of Advanced Materials Department of Materials Science and Engineering Tsinghua University Beijing 100084 P. R. China

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Regio-Regular Polymer Acceptors Enabled by Determined Fluorination on End Groups for All-Polymer Solar Cells with 15.2 % Efficiency

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Angewandte Chemie 2021年第18期133卷

作者： Han Yu Mingao Pan Rui Sun Indunil Agunawela Dr. Jianquan Zhang Yuhao Li Zhenyu Qi Han Han Xinhui Zou Wentao Zhou Dr. Shangshang Chen Dr. Joshua Yuk Lin Lai Siwei Luo Dr. Zhenghui Luo Prof. Dahui Zhao Prof. Xinhui Lu Prof. Harald Ade Prof. Fei Huang Prof. Jie Min Prof. He Yan The Institute for Advanced Studies Wuhan University Wuhan 430072 China Hong Kong University of Science and Technology–Shenzhen Research Institute No. 9 Yuexing 1st RD Hi-tech Park Nanshan Shenzhen 518057 China Department of Chemistry Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials Energy Institute and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration & Reconstruction Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China Department of Physics and Organic and Carbon Electronics Laboratories (ORaCEL) North Carolina State University Raleigh NC 27695 USA Department of Physics Chinese University of Hong Kong New Territories Hong Kong 999077 China Beijing National Laboratory for Molecular Sciences Centre for Soft Matter Science and Engineering Key Lab of Polymer Chemistry & Physics of the Ministry of Education College of Chemistry Peking University Beijing 100871 China Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 China Key Laboratory of Materials Processing and Mold Zhengzhou University Ministry of Education 450002 Zhengzhou China

Polymerization sites of small molecule acceptors (SMAs) play vital roles in determining device performance of all-polymer solar cells (all-PSCs). Different from our recent work about fluoro- and bromo- co-modified end group of IC-FBr (a mixture of IC-FBr1 and IC-FBr2), in this paper, we synthesized and purified two regiospecific fluoro- and bromo- substituted end groups (IC-FBr- o & IC-FBr- m ), which were then employed to construct two regio-regular polymer acceptors named PYF-T- o and PYF-T- m , respectively . In comparison with its isomeric counterparts named PYF-T- m with different conjugated coupling sites, PYF-T- o exhibits stronger and bathochromic absorption to achieve better photon harvesting. Meanwhile, PYF-T- o adopts more ordered inter-chain packing and suitable phase separation after blending with the donor polymer PM6, which resulted in suppressed charge recombination and efficient charge transport. Strikingly, we observed a dramatic performance difference between the two isomeric polymer acceptors PYF-T- o and PYF-T- m . While devices based on PM6:PYF-T- o can yield power conversion efficiency (PCE) of 15.2 %, devices based on PM6:PYF-T- m only show poor efficiencies of 1.4 %. This work demonstrates the success of configuration-unique fluorinated end groups in designing high-performance regular polymer acceptors, which provides guidelines towards developing all-PSCs with better efficiencies.

关键词： all-polymer solar cells fluorinated end group isomeric effect organic solar cells polymer acceptors

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

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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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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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