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Engineering the Local Atomic Environments of Indium Single-Atom Catalysts for Efficient Electrochemical Production of Hydrogen Peroxide

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Angewandte Chemie 2022年第12期134卷

作者： Dr. Erhuan Zhang Dr. Lei Tao Dr. Jingkun An Dr. Jiangwei Zhang Lingzhe Meng Dr. Xiaobo Zheng Prof. Yu Wang Prof. Nan Li Prof. Shixuan Du Prof. Jiatao Zhang Prof. Dingsheng Wang Prof. Yadong Li Department of Chemistry Tsinghua University Beijing 100084 P. R. China Institute of Physics & University of Chinese Academy of Sciences Chinese Academy of Sciences Beijing 100190 P. R. China School of Environmental Science and Engineering Academy of Environment and Ecology Tianjin University Tianjin 300072 P. R. China Dalian National Laboratory for Clean Energy & State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced Materials School of Materials Science & Engineering Beijing Institute of Technology Beijing 100081 P. R. China Shanghai Synchrotron Radiation Facilities Shanghai Institute of Applied Physics Chinese Academy of Science Shanghai 201204 P. R. China Beijing National Laboratory for Condensed Matter Physics Beijing 100190 P. R. China

The in-depth understanding of local atomic environment–property relationships of p-block metal single-atom catalysts toward the 2 e − oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first-principles calculations, we develop a heteroatom-modified In-based metal–organic framework-assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored by combined N,S-dual first coordination and B second coordination supported by the hollow carbon rods (In SAs/NSBC). The In SAs/NSBC catalyst exhibits a high H 2 O 2 selectivity of above 95 % in a wide range of pH. Furthermore, the In SAs/NSBC-modified natural air diffusion electrode exhibits an unprecedented production rate of 6.49 mol peroxide g catalyst −1 h −1 in 0.1 M KOH electrolyte and 6.71 mol peroxide g catalyst −1 h −1 in 0.1 M PBS electrolyte. This strategy enables the design of next-generation high-performance single-atom materials, and provides practical guidance for H 2 O 2 electrosynthesis.

关键词： Electrocatalysis Hydrogen Peroxide Indium Single-Atom Catalyst Local Coordination Environments Metal–Organic Frameworks

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Respiration Monitoring: From Molecular Reconstruction of Mesoscopic functional Conductive Silk Fibrous Materials to Remote Respiration Monitoring (Small 26/2020)

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Small 2020年第26期16卷

作者： Liyun Ma Qiang Liu Ronghui Wu Zhaohui Meng Aniruddha Patil Rui Yu Yun Yang Shuihong Zhu Xuwei Fan Chen Hou Yanran Li Wu Qiu Lianfen Huang Jun Wang Naibo Lin Yizao Wan Jian Hu Xiang Yang Liu Research Institution for Biomimetics and Soft Matter College of Physical Science and Technology College of Materials Fujian Provincial Key Laboratory for Soft Functional Materials Research Jiujiang Research Institute Xiamen University Xiamen 361005 P. R. China Key Laboratory of Textile Science & Technology Ministry of Education College of Textiles Donghua University Shanghai 201620 P. R. China College of Textile and Clothing Xinjiang University Urumqi 830000 P. R. China Institute of Advanced Materials East China JiaoTong University Nanchang 330013 P. R. China Department of Physics Faculty of Science National University of Singapore Singapore 117542 Singapore Department of Information and Communication Engineering Xiamen University Xiamen 361005 P. R. China

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Perovskite Light-Emitting Diodes: Efficient CsPbBr3Perovskite Light-Emitting Diodes Enabled by Synergetic Morphology Control (advanced Optical Materials 4/2019)

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advanced Optical Materials 2019年第4期7卷

作者： Li-Peng Cheng Jing-Sheng Huang Yang Shen Guo-Peng Li Xiao-Ke Liu Wei Li Yu-Han Wang Yan-Qing Li Yang Jiang Feng Gao Chun-Sing Lee Jian-Xin Tang Institute of Functional Nano & Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Suzhou 215123 P.R. China School of Materials Science and Engineering Hefei University of Technology (HFUT) Hefei Anhui 230009 P.R. China Biomolecular and Organic Electronics Department of Physics Chemistry and Biology (IFM) Linköping University 58183 Linköping Sweden Center of Super-Diamond and Advanced Film (COSADF) and Department of Chemistry City University of Hong Kong Hong Kong S.A.R. P.R. China Institute of Organic Optoelectronics (IOO) Jiangsu Industrial Technology Research Institute (JITRI) Wujiang Suzhou 215215 P.R. China

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Zinc Metal Batteries: Stratified Zinc-Binding Strategy toward Prolonged Cycling and Flexibility of Aqueous Fibrous Zinc Metal Batteries (Adv. Energy Mater. 16/2021)

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advanced Energy Materials 2021年第16期11卷

作者： Zhaoxi Shen Lei Luo Chaowei Li Jun Pu Junpeng Xie Litong Wang Zhe Huai Ziyi Dai Yagang Yao Guo Hong Institute of Applied Physics and Materials Engineering University of Macau Avenida da Universidade Taipa Macau SAR 999078 China State Key Laboratory of Precision Spectroscopy School of Physics and Electronic Science East China Normal University Shanghai 200062 China National Laboratory of Solid State Microstructures College of Engineering and Applied Sciences Jiangsu Key Laboratory of Artificial Functional Materials Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China Division of Nanomaterials and Jiangxi Key Lab of Carbonene Materials Suzhou Institute of Nano-Tech and Nano-Bionics Nanchang Chinese Academy of Sciences Nanchang 330200 China Department of Physics and Chemistry Faculty of Science and Technology University of Macau Avenida da Universidade Taipa Macau SAR 999078 China

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A Fused Helicene Dimer with a Figure-Eight Topology: Synthesis, Chiral Resolution, and Electronic Properties

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Angewandte Chemie 2023年第23期135卷

作者： Qifeng Zhou Xudong Hou Dr. Jinyi Wang Dr. Yong Ni Dr. Wei Fan Dr. Zhengtao Li Xiao Wei Ke Li Dr. Wei Yuan Zhuofan Xu Prof. Manzhou Zhu Prof. Yanli Zhao Prof. Zhe Sun Prof. Jishan Wu Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Binhai New City Fuzhou 350507 China Department of Chemistry National University of Singapore 3 Science Drive 3 Singapore 117543 Singapore Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Institutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials Anhui University Hefei Anhui 230601 China Institute of Molecular Plus Department of Chemistry and Haihe Laboratory of Sustainable Chemical Transformations Tianjin University Tianjin 300072 China School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singapore Singapore 637371 Singapore

Chiral shape-persistent molecular nanocarbons are promising chiroptical materials; their synthesis, however, remains a big challenge. Herein, we report the facile synthesis and chiral resolution of a double-stranded figure-eight carbon nanobelt 1 in which two [5]helicene units are fused together. Two synthetic routes were developed, and, in particular, a strategy involving Suzuki coupling-mediated macrocyclization followed by Bi(OTf) 3 -catalyzed cyclization of vinyl ether turned out to be the most efficient. The structure of 1 was confirmed by X-ray crystallographic analysis. The isolated ( P , P )- and ( M , M )- enantiomers show persistent chiroptical properties with relatively large dissymmetric factors (| g abs |=5.4×10 −3 and | g lum |=1.0×10 −2 ), which can be explained by the effective electron delocalization along the fully conjugated belt and the unique D 2 symmetry. 1 exhibits local aromatic character with a dominant structure containing eight Clar's aromatic sextet rings.

关键词： Carbon Nanobelt Chirality Circular Dichroism Circularly Polarized Luminescence Figure-Eight

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Fluorinated Rocksalt Cathode with Ultra-high Active Li Content for Lithium-ion Batteries

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Angewandte Chemie 2022年第47期134卷

作者： Dr. Yi Pei Dr. Qing Chen Dr. Yang Ha Prof. Dong Su Prof. Hua Zhou Dr. Shuang Li Dr. Zhenpeng Yao Dr. Lu Ma Dr. Kevin J. Sanders Dr. Chuanchao Sheng Prof. Gillian R. Goward Prof. Lin Gu Prof. Aiping Yu Prof. Wanli Yang Prof. Zhongwei Chen Department of Chemical Engineering Waterloo Institute for Nanotechnology University of Waterloo Waterloo Ontario N2 L 3G1 Canada Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA Department of Chemistry and Department of Computer Science University of Toronto Toronto Ontario M5S 3H6 Canada National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA Department of Chemistry McMaster University Hamilton ON L8S 4 L8 Canada Center of Energy Storage Materials & Technology College of Engineering and Applied Sciences National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing 210093 China

The key to increasing the energy density of lithium-ion batteries is to incorporate high contents of extractable Li into the cathode. Unfortunately, this triggers formidable challenges including structural instability and irreversible chemistry under operation. Here, we report a new kind of ultra-high Li compound: Li 4+ x MoO 5 F x (1≤ x ≤3) for cathode with an unprecedented level of electrochemically active Li (>3 Li + per formula), delivering a reversible capacity up to 438 mAh g −1 . Unlike other reported Li-rich cathodes, Li 4+ x MoO 5 F x presents distinguished structure stability to immunize against irreversible behaviors. Through spectroscopic and electrochemical techniques, we find an anionic redox-dominated charge compensation with negligible oxygen release and voltage decay. Our theoretical analysis reveals a “reductive effect” of high-level fluorination stabilizes the anionic redox by reducing the oxygen ions in pure-Li conditions, enabling a facile, reversible, and high Li-portion cycling.

关键词： Anionic Redox High Fluorination Level Reductive Effect Ultra-High Li Cathode

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High-Performance Electrochemical NO Reduction into NH3by MoS2Nanosheet

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Angewandte Chemie 2021年第48期133卷

作者： Longcheng Zhang Jie Liang Yuanyuan Wang Ting Mou Yiting Lin Luchao Yue Prof. Tingshuai Li Dr. Qian Liu Yonglan Luo Prof. Na Li Prof. Bo Tang Dr. Yang Liu Prof. Shuyan Gao Prof. Abdulmohsen Ali Alshehri Prof. Xiaodong Guo Prof. Dongwei Ma Prof. Xuping Sun Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 610054 Sichuan China School of Chemical Engineering Sichuan University Chengdu 610065 Sichuan China Key Laboratory for Special Functional Materials of Ministry of Education and School of Materials Science and Engineering Henan University Kaifeng 475004 Henan China Institute for Advanced Study Chengdu University Chengdu 610106 Sichuan China College of Chemistry Chemical Engineering and Materials Science Shandong Normal University Jinan 250014 Shandong China School of Materials Science and Engineering Henan Normal University Xinxiang 453007 Henan China Chemistry Department Faculty of Science King Abdulaziz University P.O. Box 80203 Jeddah 21589 Saudi Arabia

Electrochemical reduction of NO not only offers an attractive alternative to the Haber–Bosch process for ambient NH 3 production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS 2 nanosheet on graphite felt (MoS 2 /GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH 3 conversion. In acidic electrolyte, such MoS 2 /GF attains a maximal Faradaic efficiency of 76.6 % and a large NH 3 yield of up to 99.6 μmol cm −2 h −1 . Using MoS 2 nanosheet-loaded carbon paper as the cathode, a proof-of-concept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm −2 and an NH 3 yield of 411.8 μg h −1 mg cat. −1 . Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance–donation mechanism and disfavor the binding of protons and the coupling of N−N bond.

关键词： density functional theory electrocatalysis MoS2 NH3 synthesis NO reduction reaction

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sp2to sp3Hybridization Transformation in Ionic Crystals under Unprecedentedly Low Pressure

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Angewandte Chemie 2022年第44期134卷

作者： Dr. Xingxing Jiang Dr. Maxim S. Molokeev Naizheng Wang Prof. Yonggang Wang Dr. Ting Wen Dr. Zhichao Dong Youquan Liu Prof. Wei Li Prof. Zheshuai Lin Functional Crystals Lab Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China Laboratory of Crystal Physics Kirensky Institute of Physics SB RAS Krasnoyarsk 660036 Russia Department of Physics Far Eastern State Transport University Khabarovsk 680021 Russia Siberian Federal University Krasnoyarsk 660041 Russia University of Chinese Academy of Sciences Beijing 100049 China School of Materials Science and Engineering Peking University Beijing 100871 China Center for High Pressure Science & Technology Advanced Research Beijing 100094 China Laboratory of Space Astronomy and Technology National Astronomical Observatories Chinese Academy of Sciences Beijing 100101 China School of Materials Science and Engineering TKL of Metal and Molecule-Based Material Chemistry Nankai University Tianjin 300350 China

Under cold pressure sp 1 /sp 2 -to-sp 3 hybridization transformation has been exclusively observed in covalent or molecular crystals overwhelmingly above ≈10 GPa, and the approaches to lower the transition pressure are limited on external heat-treatment and/or catalyzers. Herein we demonstrate that, by internal-lattice stress-transfer from ionic to covalent groups, the transformation can be significantly prompted, as shown in a crystal of LiBO 2 under 2.85 GPa for the first case in ionic crystals. This unprecedentedly low transformation pressure is ascribed to the enhanced localized stress on covalent B−O frames transferred from ionic Li−O bonds in LiBO 2 , and accordingly the corresponding structural feature is summarized. This work provides an internal structural regulation strategy for pressure-reduction of the s-p orbital hybridization transformation and extends the sp 1 /sp 2 -to-sp 3 transformation landscape from molecular and covalent compounds to ionic systems.

关键词： Borates Hybridization Transformation Ionic Crystal Stress Transfer

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Erratum: “Using highly accelerated life test to study insulation reliability of multi-layer ceramic capacitors sintered at different temperatures” [J. Appl. Phys. 134, 194101 (2023)]

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Journal of Applied Physics 2024年第1期135卷

作者： Zhifei Wang Shiguang Yan Fei Cao Zhichao Hong Yuelong Xiong Benxia Chen Chenhong Xu Genshui Wang Key Laboratory of Inorganic Functional Materials and Devices Shanghai Institute of Ceramics Chinese Academy of Sciences 1295 Dingxi Road Shanghai 200050 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences 19 Yuquan Road Shijingshan District Beijing 100049 China Fujian Torch Electron Technology Company Ltd. Quanzhou Fujian 362000 China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences 1295 Dingxi Road Shanghai 200050 China School of Chemistry and Materials Science Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences Hangzhou 310024 China

We noticed an error in combining figures in Fig. 6.1 The correct sub-figure Fig. 6(i) should show survival curves of H-MLCC under 75 V 150 °C. However, the curr

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Publisher’s Note: “Using highly accelerated life test to study insulation reliability of multi-layer ceramic capacitors sintered at different temperatures” [J. Appl. Phys. 134, 194101 (2023)]

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Journal of Applied Physics 2024年第2期135卷

This article was originally published online on 15 November 2023 missing an affiliation. All affiliations and identifiers are correct as they appear above. All

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