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Macrocyclic Transformations from Norrole to Isonorrole and an N‐Confused Corrole with a Fused Hexacyclic Ring System Triggered by a Pyrrole Substituent

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Angewandte Chemie 2016年第9期128卷

作者： Miao Li Pingchun Wei Masatoshi Ishida Xin Li Mathew Savage Rui Guo Zhongping Ou Sihai Yang Hiroyuki Furuta Yongshu Xie Key Laboratory for Advanced Materials and Institute of Fine Chemicals Shanghai Key Laboratory of Functional Materials Chemistry East China University of Science and Technology Shanghai 200237 P.R. China Education Center for Global Leaders in Molecular Systems for Devices and Center for Molecular Systems Department of Chemistry and Biochemistry Graduate School of Engineering Kyushu University Fukuoka 819-0395 Japan School of Chemistry University of Manchester Manchester m139pl UK School of Chemistry and Chemical Engineering Jiangsu University Zhenjiang 212013 P.R. China

Three kinds of fused porphyrinoids, L2 – L4 , possessing different types of corrole‐based frameworks were synthesized from a pyrrole‐substituted corrole isomer (norrole L1 ). Oxidation of L1 afforded a unique N‐C meso ‐fused pyrrolyl isonorrole L2 , involving the fusion of an auxiliary pyrrolic NH moiety with a meso‐sp 3 ‐hybridized carbon atom. Subsequently, L2 underwent macrocycle transformations to give singly and doubly N‐C Ar ‐fused N‐confused corroles, L3 and L4 , respectively. L3 and L4 contain fused [5.7.6.5]‐tetra‐ and [5.6.7.7.6.5]‐hexacyclic structures, respectively, prepared through lateral annulation. These skeletal transformation reactions from norrole to its isomer isonorrole and finally to N‐confused corrole indicate that multiply fused porphyrinoids could be readily synthesized from pyrrole‐appended confused porphyrinoids.

关键词： Aromatizität Corrole Kondensierte Ringe N-invertierte Corrole Porphyrinoide

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Corrigendum to “Sputtered and selenized Sb 2 Se 3 thin-film solar cells with open-circuit voltage exceeding 500 mV” [Nano Energy 73 (2020) 104806]

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Nano Energy 2020年 76卷

作者： Guang-Xing Liang Yan-Di Luo Shuo Chen Rong Tang Zhuang-Hao Zheng Xue-Jin Li Xin-Sheng Liu Yi-Ke Liu Ying-Fen Li Xing-Ye Chen Zheng-Hua Su Xiang-Hua Zhang Hong-Li Ma Ping Fan Shenzhen Key Laboratory of Advanced Thin Films and Applications College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen 518060 PR China School of Science and Engineering The Chinese University of Hong Kong (Shenzhen) Shenzhen 518060 PR China Key Laboratory for Special Functional Materials of Ministry of Education Henan University Kaifeng 475004 PR China School of Material and Metallurgical Engineering Guizhou Institute of Technology Guiyang 550003 PR China Univ Rennes CNRS ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226 Rennes F-35000 France

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Frontispiece: Tracking the Process of a Solvothermal Domino Reaction Leading to a Stable Triheteroarylmethyl Radical: A Combined Crystallographic and Mass-Spectrometric Study

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Angewandte Chemie International Edition 2019年第12期58卷

作者： Dr. Bin Liu Fei Yu Min Tu Zhong-Hong Zhu Dr. Yuexing Zhang Dr. Zhong-Wen Ouyang Dr. Zhenxing Wang Dr. Ming-Hua Zeng Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules College of Chemistry and Chemical Engineering Hubei University Wuhan 430062 P. R. China Department Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources School of Chemistry and Pharmaceutical Sciences Guangxi Normal University Guilin 541004 P. R. China Wuhan National High Magnetic Field Center & School of Physics Huazhong University of Science and Technology Wuhan 430074 P. R. China

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Regulating the Inner Helmholtz Plane with a High Donor Additive for Efficient Anode Reversibility in Aqueous Zn-Ion Batteries

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Angewandte Chemie 2023年第21期135卷

作者： Jinrong Luo Liang Xu Yijing Zhou Tianran Yan Yanyan Shao Dongzi Yang Liang Zhang Zhou Xia Tianheng Wang Prof. Liang Zhang Prof. Tao Cheng Prof. Yuanlong Shao College of Energy Soochow Institute for Energy and Materials Innovations (SIEMIS) Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow University Suzhou 215006 P. R. China Institute of Functional Nano and Soft Materials (FUNSOM) Soochow University Suzhou 215123 P. R. China School of Environmental and Biological Engineering Nanjing University of Science and Technology Nanjing 210094 P. R. China School of Materials Science and Engineering Peking University Beijing 100871 P. R. China

The performance of aqueous Zn ion batteries (AZIBs) is highly dependent on inner Helmholtz plane (IHP) chemistry. Notorious parasitic reactions containing hydrogen evolution reactions (HER) and Zn dendrites both originate from abundant free H 2 O and random Zn deposition inside active IHP. Here, we report a universal high donor number (DN) additive pyridine (Py) with only 1 vol. % addition (Py-to-H 2 O volume ratio), for regulating molecule distribution inside IHP. Density functional theory (DFT) calculations and molecular dynamics (MD) simulation verify that incorporated Py additive could tailor Zn 2+ solvation sheath and exclude H 2 O molecules from IHP effectively, which is in favor of preventing H 2 O decomposition. Consequently, even at extreme conditions such as high depth of discharge (DOD) of 80 %, the symmetric cell based on Py additive can sustain approximately 500 h long-term stability. This efficient strategy with high DN additives furnishes a promising direction for designing novel electrolytes and promoting the practical application of AZIBs, despite inevitably introducing trace organic additives.

关键词： Donor Number Inner Helmholtz Plane Solvation Sheath Zn Anode Zn Utilization Rate

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Brain Tumor Therapy: Systemic Delivery of Monoclonal Antibodies to the Central Nervous System for Brain Tumor Therapy (Adv. Mater. 19/2019)

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advanced Materials 2019年第19期31卷

作者： Lei Han Chaoyong Liu Hongzhao Qi Junhu Zhou Jing Wen Di Wu Duo Xu Meng Qin Jie Ren Qixue Wang Lixia Long Yang Liu Irvin Chen Xubo Yuan Yunfeng Lu Chunsheng Kang Department of Neurosurgery Tianjin Medical University General Hospital Key Laboratory of Neurotrauma Variation and Regeneration Ministry of Education and Tianjin Municipal Government Tianjin Neurological Institute Tianjin 300052 China College of Life Science and Technology and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 China School of Materials Science Engineering Tianjin University Tianjin 300350 China Department of Microbiology Immunology and Molecular Genetics David Geffen School of Medicine University of California Los Angeles UCLA AIDS Institute Los Angeles CA 90095 USA Department of Chemical and Biomolecular Engineering University of California Los Angeles CA 90095 USA Key Laboratory of Functional Polymer Materials of Ministry of Education Institute of Polymer Chemistry College of Chemistry State Key Laboratory of Medicinal Chemical Biology Nankai University Tianjin 300071 China

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Processability: Evaluation of Electron Donor Materials for Solution‐Processed Organic Solar Cells via a Novel Figure of Merit (Adv. Energy Mater. 18/2017)

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advanced Energy Materials 2017年第18期7卷

作者： Jie Min Yuriy N. Luponosov Chaohua Cui Bin Kan Haiwei Chen Xiangjian Wan Yongsheng Chen Sergei A. Ponomarenko Yongfang Li Christoph J. Brabec The Institute for Advanced Studies Wuhan University Wuhan 430072 China Institute of Materials for Electronics and Energy Technology (I‐MEET) Friedrich‐Alexander University Erlangen‐Nuremberg Martensstraße 7 91058 Erlangen Germany Enikolopov Institute of Synthetic Polymeric Materials of the Russian Academy of Sciences Profsoyuznaya st. 70 Moscow 117393 Russia Laboratory of Advanced Optoelectronic Materials College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China State Key Laboratory and Institute of Elemento‐Organic Chemistry Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University Tianjin 300071 China Key Laboratory of Functional Polymer Materials and the Centre of Nanoscale Science and Technology Institute of Polymer Chemistry College of Chemistry Nankai University Tianjin 300071 China Chemistry Department Moscow State University Leninskie Gory 1–3 Moscow 119991 Russia Bavarian Center for Applied Energy Research (ZAE Bayern) Haberstraße 2a 91058 Erlangen Germany

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Organic Solar Cells: Sequentially Deposited versus Conventional Nonfullerene Organic Solar Cells: Interfacial Trap States, Vertical Stratification, and Exciton Dissociation (Adv. Energy Mater. 47/2019)

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advanced Energy Materials 2019年第47期9卷

作者： Jiangbin Zhang Moritz H. Futscher Vincent Lami Felix U. Kosasih Changsoon Cho Qinying Gu Aditya Sadhanala Andrew J. Pearson Bin Kan Giorgio Divitini Xiangjian Wan Dan Credgington Neil C. Greenham Yongsheng Chen Caterina Ducati Bruno Ehrler Yana Vaynzof Richard H. Friend Artem A. Bakulin Cavendish Laboratory University of Cambridge JJ Thomson Avenue Cambridge CB3 0HE UK Department of Chemistry Imperial College London London SW7 2AZ UK Center for Nanophotonics AMOLF Science Park 104 1098 XG Amsterdam The Netherlands Kirchhoff Institute for Physics and the Centre for Advanced Materials Heidelberg University Im Neuenheimer Feld 227 69120 Heidelberg Germany Department of Materials Science & Metallurgy University of Cambridge 27 Charles Babbage Road Cambridge CB3 0FS UK School of Electrical Engineering Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 Republic of Korea The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials State Key Laboratory and Institute of Elemento‐Organic Chemistry College of Chemistry Nankai University Tianjin 300071 China Dresden Integrated Centre for Applied Physics and Photonic Materials (IAPP) and Centre for Advancing Electronics Dresden (CFAED) Technical University of Dresden Nöthnitzer Straße 61 01187 Dresden Germany

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Main-Group Metal-Nonmetal Dynamic Proton Bridges Enhance Ammonia Electrosynthesis

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Angewandte Chemie 2024年第45期136卷

作者： Yuntong Sun Liming Dai Kai Dong Nicole L. D. Sui Yinghao Li Prof. Jingwen Sun Prof. Jianrong Zeng Prof. Wenjun Fan Prof. Meng Tian Prof. Junwu Zhu Prof. Jong-Min Lee School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University 62 Nanyang Drive 637459 Singapore Singapore Key Laboratory for Soft Chemistry and Functional Materials School of Chemistry and Chemical Engineering Nanjing University of Science and Technology 210094 Nanjing China School of Chemical Engineering The University of Adelaide 5000 Adelaide South Australia Australia Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences 201204 Shanghai P. R. China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian National Laboratory for Clean Energy 116023 Dalian Liaoning P. R. China Interdisciplinary Center for Fundamental and Frontier Sciences Nanjing University of Science and Technology 214443 Jiangyin Jiangsu China

The electrochemical nitrogen reduction reaction (eNRR) is a crucial process for the sustainable production of ammonia (NH 3 ) for energy and agriculture applications. However, the reaction's efficiency is highly dependent on the activation of the inert N≡N bond, which is hindered by the electron back-donation to the π* orbitals of the N≡N bond, resulting in low eNRR capacity. Herein, we report a main-group metal-nonmetal (O−In−S) eNRR catalyst featuring a dynamic proton bridge, with In−S serving as the polarization pair and O functioning as the dynamic electron pool. In situ spectroscopic analysis and theoretical calculations reveal that the In−S polarization pair acts as asymmetric dual-sites, polarizing the N≡N bond by concurrently back-donating electrons to both the π x * and π y * orbitals of N 2 , thereby overcoming the significant band gap limitations, while inhibiting the competitive hydrogen evolution reaction. Meanwhile, the O dynamic electron pool acts as a “repository” for electron storage and donation to the In−S polarization pair. As a result, the O−In−S dynamic proton bridge exhibits exceptional NH 3 yield rates and Faradaic efficiencies (FEs) across a wide potential window of 0.3 V, with an optimal NH 3 yield rate of 80.07±4.25 μg h −1 mg −1 and an FE of 38.01±2.02 %, outperforming most previously reported catalysts.

关键词： electrocatalysis nitrogen reduction reaction dynamic proton bridge polarization pair asymmetric dual-sites

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In Situ Polymerized 1,3-Dioxolane Electrolyte for Integrated Solid-State Lithium Batteries

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Angewandte Chemie 2023年第12期135卷

作者： Ye Qian Mi Wei Deng Chaohui He Prof. Dr. Osman Eksik Yi Ping Zheng De Kun Yao Dr. Xian Bin Liu Yan Hong Yin Ye Sheng Li Prof. Dr. Bao Yu Xia Prof. Dr. Zi Ping Wu Ganzhou Key Laboratory of Advanced Metals and Functional Materials Faculty of Materials Metallurgy and Chemistry Jiangxi University of Science and Technology Ganzhou 341000 China Contribution: Data curation (lead) Contribution: Formal analysis (lead) Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Wuhan National Laboratory for Optoelectronics School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China Institute of Nanotechnology Gebze Technical University Gebze 41400 Turkey Contribution: Investigation (equal) Contribution: Methodology (lead) Contribution: Supervision (equal) Writing - original draft (lead) Contribution: Resources (lead) Contribution: Conceptualization (lead) Supervision (lead) Visualization (lead) Writing - review & editing (equal) Contribution: Project administration (lead) Supervision (lead) Validation (lead) Writing - original draft (lead)

Solid-state lithium batteries are promising and safe energy storage devices for mobile electronics and electric vehicles. In this work, we report a facile in situ polymerization of 1,3-dioxolane electrolytes to fabricate integrated solid-state lithium batteries. The in situ polymerization and formation of solid-state dioxolane electrolytes on interconnected carbon nanotubes (CNTs) and active materials is the key to realizing a high-performance battery with excellent interfacial contact among CNTs, active materials and electrolytes. Therefore, the electrodes could be tightly integrated into batteries through the CNTs and electrolyte. Electrons/ions enable full access to active materials in the whole electrode. Electrodes with a low resistance of 4.5 Ω □ −1 and high lithium-ion diffusion efficiency of 2.5×10 −11 cm 2 s −1 can significantly improve the electrochemical kinetics. Subsequently, the batteries demonstrated high energy density, amazing charge/discharge rate and long cycle life.

关键词： Interface Lithium Battery Polymerization Solid-State Electrolyte

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Quantification of Charge Transport and Mass Deprivation in Solid Electrolyte Interphase for Kinetically-Stable Low-Temperature Lithium-Ion Batteries

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Angewandte Chemie 2024年第43期136卷

作者： Dr. Liwei Dong Prof. Hui-Juan Yan Qing-Xiang Liu Prof. Jia-Yan Liang Dr. Junpei Yue Min Niu Xingyu Chen Enhui Wang Prof. Sen Xin Prof. Xinghong Zhang Prof. Chunhui Yang Prof. Yu-Guo Guo MOE Engineering Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions School of Chemistry and Chemical Engineering Harbin Institute of Technology (HIT) Harbin 150001 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 School of Chemical Sciences University of Chinese Academy of Sciences (UCAS) Beijing 100049 P. R. China National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and Structures Harbin Institute of Technology (HIT) Harbin 150001 P. R. China

Graphite (Gr)-based lithium-ion batteries with admirable electrochemical performance below −20 °C are desired but are hindered by sluggish interfacial charge transport and desolvation process. Li salt dissociation via Li + -solvent interaction enables mobile Li + liberation and contributes to bulk ion transport, while is contradictory to fast interfacial desolvation. Designing kinetically-stable solid electrolyte interphase (SEI) without compromising strong Li + -solvent interaction is expected to compatibly improve interfacial charge transport and desolvation kinetics. However, the relationship between physicochemical features and temperature-dependent kinetics properties of SEI remains vague. Herein, we propose four key thermodynamics parameters of SEI potentially influencing low-temperature electrochemistry, including electron work function, Li + transfer barrier, surface energy, and desolvation energy. Based on the above parameters, we further define a novel descriptor, separation factor of SEI ( S SEI ), to quantitatively depict charge (Li + /e − ) transport and solvent deprivation processes at Gr/electrolyte interface. A Li 3 PO 4 -based, inorganics-enriched SEI derived by Li difluorophosphate (LiDFP) additive exhibits the highest S SEI (4.89×10 3 ) to enable efficient Li + conduction, e − blocking and rapid desolvation, and as a result, much suppressed Li-metal precipitation, electrolyte decomposition and Gr sheets exfoliation, thus improving low-temperature battery performances. Overall, our work originally provides visualized guides to improve low-temperature reaction kinetics/thermodynamics by constructing desirable SEI chemistry.

关键词： Lithium-ion battery Low temperature Solid electrolyte interphase Transport kinetic Interfacial stability

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