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Front Cover: Titanium Vacancies in TiO2Nanofibers Enable Highly Efficient Photodriven Seawater Splitting (Chem. Eur. J. 57/2021)

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Chemistry – A European Journal 2021年第57期27卷

作者： Yan-Xiang Zhang Dr. Si-Ming Wu Dr. Ge Tian Xiao-Fang Zhao Dr. Li-Ying Wang Dr. Yi-Xia Yin Lu Wu Qian-Ni Li Prof. Dr. Yue-Xing Zhang Prof. Dr. Jin-Song Wu Prof. Dr. Christoph Janiak Prof. Dr. Kenneth I. Ozoemena Prof. Dr. Menny Shalom Prof. Dr. Xiao-Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Materials Science and Engineering & NRC (Nanostructure Research Centre) Wuhan University of Technology Wuhan 430070 P. R. China School of Chemical Engineering and Technology Sun Yat-sen University (Zhuhai) Zhuhai 519000 P. R. China School of Engineering and Applied Sciences Harvard University Cambridge MA 02138 USA State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Wuhan Institute of Physics and Mathematics The Chinese Academy of Sciences Wuhan 430071 P. R. China 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 Institut für Anorganische Chemie und Strukturchemie Heinrich-Heine-Universität Düsseldorf Düsseldorf 40204 Germany Molecular Sciences Institute School of Chemistry University of the Witwatersrand Johannesburg 2050 South Africa Department of Chemistry and Ilse Katz Institute for Nanoscale Science and Technology Ben-Gurion University of the Negev Beer-Sheva 8410501 Israel

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Tandem Catalysis for Selective Oxidation of Methane to Oxygenates Using Oxygen over PdCu/Zeolite

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Angewandte Chemie 2022年第24期134卷

作者： Bo Wu Tiejun Lin Min Huang Shenggang Li Ji Li Xing Yu Ruoou Yang Fanfei Sun Zheng Jiang Yuhan Sun Liangshu Zhong CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China School of Physical Science and Technology ShanghaiTech University Shanghai 201210 P. R. China Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China 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

Selective oxidation of methane to oxygenates with O 2 under mild conditions remains a great challenge. Here we report a ZSM-5 (Z-5) supported PdCu bimetallic catalyst (PdCu/Z-5) for methane conversion to oxygenates by reacting with O 2 in the presence of H 2 at low temperature (120 °C). Benefiting from the co-existence of PdO nanoparticles and Cu single atoms via tandem catalysis, the PdCu/Z-5 catalyst exhibited a high oxygenates yield of 1178 mmol g −1 Pd h −1 (mmol of oxygenates per gram Pd per hour) and at the same time high oxygenates selectivity of up to 95 %. Control experiments and mechanistic studies revealed that PdO nanoparticles promoted the in situ generation of H 2 O 2 from O 2 and H 2 , while Cu single atoms not only accelerated the activation of H 2 O 2 for the generation of abundant hydroxyl radicals (⋅OH) from H 2 O 2 decomposition, but also enabled the homolytic cleavage of CH 4 by ⋅OH to methyl radicals (⋅CH 3 ). Subsequently, the ⋅OH reacted quickly with the ⋅CH 3 to form CH 3 OH with high selectivity.

关键词： Methane Oxygenates Reaction Mechanisms Selective Oxidation Tandem Catalysis

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Two-Second-Annealed 2D/3D Perovskite Films with Graded Energy Funnels and Toughened Heterointerfaces for Efficient and Durable Solar Cells

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Angewandte Chemie 2023年第38期135卷

作者： Dr. Xueqing Chang Dr. Jun-Xing Zhong Sibo Li Dr. Qin Yao Yuxuan Fang Guo Yang Ying Tan Prof. Qifan Xue Prof. Longbin Qiu Dr. Qingqian Wang Prof. Yong Peng Prof. Wu-Qiang Wu MOE Key Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional Materials School of Chemistry Sun Yat-sen University Guangzhou 510006 P. R. China School of chemistry and Materials Science Guangdong University of Education Guangzhou 510303 P.R. China SUSTech Energy Institute for Carbon Neutrality Department of Mechanical and Energy Engineering Southern University of Science and Technology Shenzhen 518055 P. R. China School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 P. R. China State Key Laboratory of Luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and Devices School of Materials Science and Engineering South China University of Technology 381 Wushan Road Guangzhou 510640 P. R. China Institute of Physics Henan Academy of Sciences Mingli Road 266-38 Zhengzhou 450046 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei P. R. China Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

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Ferromagnetic materials: Strong Ferromagnetism Achieved via Breathing Lattices in Atomically Thin Cobaltites (Adv. Mater. 4/2021)

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advanced materials 2021年第4期33卷

作者： Sisi Li Qinghua Zhang Shan Lin Xiahan Sang Ryan F. Need Manuel A. Roldan Wenjun Cui Zhiyi Hu Qiao Jin Shuang Chen Jiali Zhao Jia-Ou Wang Jiesu Wang Meng He Chen Ge Can Wang Hui-Bin Lu Zhenping Wu Haizhong Guo Xin Tong Tao Zhu Brian Kirby Lin Gu Kui-juan Jin Er-Jia Guo Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences Beijing 100190 China State Key Laboratory of Information Photonics and Optical Communications and Laboratory of Optoelectronics Materials and Devices School of Science Beijing University of Posts and Telecommunications Beijing 100876 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & Nanostructure research center Wuhan University of Technology 122 Luoshi Rd. Wuhan 430070 China NIST Center for Neutron Research National Institute of Standards and Technology (NIST) Gaithersburg MD 20899 USA Department of Materials Science and Engineering University of Florida Gainesville FL 32611 USA Eyring Materials Center Arizona State University Tempe AZ 85287 USA School of Physics and Microelectronics Zhengzhou University Zhengzhou 450052 China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Songshan Lake Materials Laboratory Dongguan Guangdong 523808 China China Spallation Neutron Source Institute of High Energy Physics Chinese Academy of Sciences Beijing 10049 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 China

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In Situ X-ray Absorption Spectroscopy of Metal/Nitrogen-doped Carbons in Oxygen Electrocatalysis

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Angewandte Chemie 2023年第27期135卷

作者： Bin Wu Tianxiao Sun Ya You Haibing Meng Dulce M. Morales Mailis Lounasvuori Abbas Beheshti Askari Li Jiang Feng Zeng Baoshan Hu Xiangzhi Zhang Renzhong Tai Zhichuan J. Xu Tristan Petit Liqiang Mai Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Straße 15 12489 Berlin Germany Institute of Physics Humboldt University Berlin Newton-Straße 15 12489 Berlin Germany State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Luoshi Road 122 Wuhan 430070 China College of Chemistry Taiyuan University of Technology Taiyuan 030024 China Chemical Engineering group Engineering and Technology institute Groningen (ENTEG) Faculty of Science and Engineering University of Groningen Nijenborgh 4 9747 AG Groningen The Netherlands 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) Beijing 100190 China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Nanjing 211816 China College of Chemistry and Chemical Engineering Chongqing University Chongqing 401331 (China) Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore

Metal/nitrogen-doped carbons (M−N−C) are promising candidates as oxygen electrocatalysts due to their low cost, tunable catalytic activity and selectivity, and well-dispersed morphologies. To improve the electrocatalytic performance of such systems, it is critical to gain a detailed understanding of their structure and properties through advanced characterization. In situ X-ray absorption spectroscopy (XAS) serves as a powerful tool to probe both the active sites and structural evolution of catalytic materials under reaction conditions. In this review, we firstly provide an overview of the fundamental concepts of XAS and then comprehensively review the setup and application of in situ XAS, introducing electrochemical XAS cells, experimental methods, as well as primary functions on catalytic applications. The active sites and the structural evolution of M−N−C catalysts caused by the interplay with electric fields, electrolytes and reactants/intermediates during the oxygen evolution reaction and the oxygen reduction reaction are subsequently discussed in detail. Finally, major challenges and future opportunities in this exciting field are highlighted.

关键词： Active Sites In Situ XAS M−N−C Catalysts Oxygen Electrocatalysis Structural Evolution

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Design and upgrade of mesoporous perovskite solar cells

Chemistry of Inorganic Materials

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Chemistry of Inorganic materials 2024年 3卷

作者： Yue Ming Youwei Jiang Jinghao Li Jie Huang Peng Xiang Cheng Qiu Yaoguang Rong Electronic and Communication Engineering Shenzhen Polytechnic University Shenzhen 518055 Guangdong PR China School of Chemistry Chemical Engineering and Life Sciences State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei PR China International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 Hubei PR China School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 Hubei PR China Solar Energy High Value Utilization and Green Conversion Hubei Provincial Engineering Research Center College of Electrical Engineering & New Energy China Three Gorges University Yichang 443002 Hubei PR China Hebei Provincial Collaborative Innovation Center of Transportation Power Grid Intelligent Integration Technology and Equipment School of Electrical and Electronic Engineering Shijiazhuang Tiedao University 050043 Shijiazhuang PR China

In recent years, there has been notable progress in the development of perovskite solar cells (PSCs), marked by significant advancements in efficiency, stability, and scalability. Among different device architectures and technical routes, mesoporous perovskite solar cells (MPSCs) based on TiO 2 /ZrO 2 /carbon scaffold and screen-printing fabrication process have shown unique advantages for mass production and commercialization due to the low material cost and scalable fabrication process. Through efforts on material optimization, interface engineering, and device design, the power conversion efficiency of MPSCs has steadily increased from the initial 6.64 % in 2013 to current 22.22 %. Attributing to the screen-printing-based fabrication process, printable mesoscopic PSCs have enabled large-area devices, from mini-modules to modules, and solar panels. In this review, we discuss the development and latest advances of MPSCs, and provide outlooks for further improving the performance of this promising photovoltaic technology.

关键词： Mesoporous perovskite solar cells Printable Mesoscopic structure Stability Upscaling

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Rapid Charge Transfer Endowed by Interfacial Ni-O Bonding in S-scheme Heterojunction for Efficient Photocatalytic H2and Imine Production

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Bowen He Dr. Peng Xiao Dr. Sijie Wan Dr. Jianjun Zhang Prof. Tao Chen Prof. Liuyang Zhang Prof. Jiaguo Yu Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street Wuhan 430078 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Methodology (lead) Writing - original draft (equal) Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China Hefei Anhui 230026 China Contribution: Data curation (equal) Formal analysis (equal) State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Contribution: Formal analysis (supporting) Methodology (supporting) Software (lead) Contribution: Methodology (supporting) Validation (supporting) Contribution: Methodology (supporting) Resources (supporting) Contribution: Formal analysis (equal) Funding acquisition (equal) Supervision (supporting) Writing - review & editing (lead)

Cooperative coupling of H 2 evolution with oxidative organic synthesis is promising in avoiding the use of sacrificial agents and producing hydrogen energy with value-added chemicals simultaneously. Nonetheless, the photocatalytic activity is obstructed by sluggish electron-hole separation and limited redox potentials. Herein, Ni-doped Zn 0.2 Cd 0.8 S quantum dots are chosen after screening by DFT simulation to couple with TiO 2 microspheres, forming a step-scheme heterojunction. The Ni-doped configuration tunes the highly active S site for augmented H 2 evolution, and the interfacial Ni−O bonds provide fast channels at the atomic level to lower the energy barrier for charge transfer. Also, DFT calculations reveal an enhanced built-in electric field in the heterojunction for superior charge migration and separation. Kinetic analysis by femtosecond transient absorption spectra demonstrates that expedited charge migration with electrons first transfer to Ni 2+ and then to S sites. Therefore, the designed catalyst delivers drastically elevated H 2 yield (4.55 mmol g −1 h −1 ) and N-benzylidenebenzylamine production rate (3.35 mmol g −1 h −1 ). This work provides atomic-scale insights into the coordinated modulation of active sites and built-in electric fields in step-scheme heterojunction for ameliorative photocatalytic performance.

关键词： Benzylamine Coupling Oxidation Hydrogen Production Interfacial Charge Transfer S-Scheme Photocatalyst

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Lithium/Sodium-Ion Batteries: In Situ, Atomic-Resolution Observation of Lithiation and Sodiation of WS2Nanoflakes: Implications for Lithium-Ion and Sodium-Ion Batteries (Small 24/2021)

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Small 2021年第24期17卷

作者： Yaobin Xu Ke Wang Zhenpeng Yao Joohoon Kang David Lam Dan Yang Wei Ai Chris Wolverton Mark C. Hersam Ying Huang Wei Huang Vinayak P. Dravid Jinsong Wu Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA NUANCE Center Northwestern University Evanston IL 60208 USA Frontiers Science Center for Flexible Electronics (FSCFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) 127 West Youyi Road Xi'an 710072 China Department of Chemistry and Chemical Biology Harvard University 12 Oxford Street Cambridge MA 02138 USA Department of Chemistry and Computer Science University of Toronto Toronto Ontario Canada School of Advanced Materials Science and Engineering Sungkyunkwan University (SKKU) Suwon 16419 Republic of Korea MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an 710072 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research Centre Wuhan University of Technology 122 Luoshi Road Wuhan Hubei 430070 China

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Ethylenedioxythiophene-Based Small Molecular Donor with Multiple Conformation Locks for Organic Solar Cells with Efficiency of 19.3 %

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Angewandte Chemie 2024年第25期136卷

作者： Dr. Qian Xie Xiangmeng Deng Prof. Chaowei Zhao Dr. Jie Fang Dr. Dongdong Xia Yuefeng Zhang Feng Ding Jiali Wang Mengdi Li Zhou Zhang Dr. Chengyi Xiao Prof. Xunfan Liao Prof. Lang Jiang Dr. Bin Huang Dr. Runying Dai Prof. Weiwei Li Institute of Applied Chemistry Jiangxi Academy of Sciences Nanchang 330096 P. R. China Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry School of Chemistry and Chemical Engineering Jiangxi University of Science and Technology Ganzhou 341000 P. R. China National Engineering Research Center for Carbohydrate Synthesis/Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education Jiangxi Normal University Nanchang 330022 P. R. China Beijing Advanced Innovation Center for Soft Matter Science and Engineering & State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 P. R. China Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

Ternary organic solar cells (T-OSCs) represent an efficient strategy for enhancing the performance of OSCs. Presently, the majority of high-performance T-OSCs incorporates well-established Y-acceptors or donor polymers as the third component. In this study, a novel class of conjugated small molecules has been introduced as the third component, demonstrating exceptional photovoltaic performance in T-OSCs. This innovative molecule comprises ethylenedioxythiophene (EDOT) bridge and 3-ethylrhodanine as the end group, with the EDOT unit facilitating the creation of multiple conformation locks. Consequently, the EDOT-based molecule exhibits two-dimensional charge transport, distinguishing it from the thiophene-bridged small molecule, which displays fewer conformation locks and provides one-dimensional charge transport. Furthermore, the robust electron-donating nature of EDOT imparts the small molecule with cascade energy levels relative to the electron donor and acceptor. As a result, OSCs incorporating the EDOT-based small molecule as the third component demonstrate enhanced mobilities, yielding a remarkable efficiency of 19.3 %, surpassing the efficiency of 18.7 % observed for OSCs incorporating thiophene-based small molecule as the third component. The investigations in this study underscore the excellence of EDOT as a building block for constructing conjugated materials with multiple conformation locks and high charge carrier mobilities, thereby contributing to elevated photovoltaic performance in OSCs.

关键词： Organic solar cells ethylenedioxythiophene conformation locks power conversion efficiency

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Formulating the Electrolyte Towards High-Energy and Safe Rechargeable Lithium–Metal Batteries

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Angewandte Chemie 2021年第30期133卷

作者： Qiang Ma Dr. Junpei Yue Min Fan Shuang-Jie Tan Dr. Juan Zhang Dr. Wen-Peng Wang Dr. Yuan Liu Yi-Fan Tian Dr. Quan Xu Prof. Ya-Xia Yin Prof. Ya You Prof. An Luo Prof. Sen Xin Prof. Xiong-Wei Wu Prof. Yu-Guo Guo College of Electrical and Information Engineering Hunan University Changsha Hunan 410082 P. R. China School of Chemistry and Materials Science College of Agronomy Hunan Agricultural University Changsha Hunan 410128 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 Nanozyme Medical Center School of Basic Medical Sciences Zhengzhou University Zhengzhou 450001 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei P. R. China

Rechargeable lithium–metal batteries with a cell-level specific energy of >400 Wh kg −1 are highly desired for next-generation storage applications, yet the research has been retarded by poor electrolyte–electrode compatibility and rigorous safety concerns. We demonstrate that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the nickel-rich layered oxide cathodes. By employing the new electrolyte, Li∥LiNi 0.6 Co 0.2 Mn 0.2 O 2 cells show favorable cycling and rate performance, and a 10 Ah Li∥LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell demonstrates a practical specific energy of >450 Wh kg −1 . Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces toward practical realization of high-energy rechargeable batteries.

关键词： hybrid electrolytes in situ polymerization interfacial chemistry rechargeable lithium–metal batteries

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