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SmartMat 2021年第2期2卷

作者： Niuwa Yang Dong Chen Penglei Cui Tingyu Lu Hui Liu Chaoquan Hu Lin Xu Jun Yang State Key Laboratory of Multiphase Complex Systems Chinese Academy of Sciences Beijing China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing China Nanjing IPE Institute of Green Manufacturing Industry Nanjing Jiangsu China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials Science Nanjing Normal University Nanjing Jiangsu China Lin Xu School of Chemistry and Materials Science Jiangsu Key Laboratory of New Power Batteries Nanjing Normal University Nanjing 210023 Jiangsu China.

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Nucleation and Growth of Amino Acid and Peptide Supramolecular Polymers through Liquid–Liquid Phase Separation

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Angewandte Chemie 2019年第50期131卷

作者： Chengqian Yuan Aviad Levin Wei Chen Ruirui Xing Qianli Zou Therese W. Herling Pavan Kumar Challa Tuomas P. J. Knowles Xuehai Yan State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China Department of Chemistry University of Cambridge Lensfield Road Cambridge CB2 1EW UK State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China Cavendish Laboratory University of Cambridge CB3 0FE Cambridge UK Center for Mesoscience Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China

The transition of peptides and proteins from the solution phase into fibrillar structures is a general phenomenon encountered in functional and aberrant biology and is increasingly exploited in soft materials science. However, the fundamental molecular events underpinning the early stages of their assembly and subsequent growth have remained challenging to elucidate. Here, we show that liquid–liquid phase separation into solute‐rich and solute‐poor phases is a fundamental step leading to the nucleation of supramolecular nanofibrils from molecular building blocks, including peptides and even amphiphilic amino acids. The solute‐rich liquid droplets act as nucleation sites, allowing the formation of thermodynamically favorable nanofibrils following Ostwald's step rule. The transition from solution to liquid droplets is entropy driven while the transition from liquid droplets to nanofibrils is mediated by enthalpic interactions and characterized by structural reorganization. These findings shed light on how the nucleation barrier toward the formation of solid phases can be lowered through a kinetic mechanism which proceeds through a metastable liquid phase.

关键词： Aminosäuren Flüssig-flüssig-Phasentrennung Nukleation Peptide Supramolekulare Polymere

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Thiolated, Reduced Palladium Nanoclusters with Resolved Structures for the Electrocatalytic Reduction of Oxygen

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Angewandte Chemie 2022年第46期134卷

作者： Dr. Shengli Zhuang Dr. Dong Chen Dr. Qing You Wentao Fan Prof. Jun Yang Prof. Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and Nanotechnology CAS Center for Excellence in Nanoscience Institute of Solid State Physics Chinese Academy of Sciences Hefei 230031 P. R. China Department of Chemistry and Centre for Atomic Engineering of Advanced Materials Anhui University Hefei Anhui 230601 P. R. China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 P.R. China

Although thiolated, reduced Group 11 metal nanoclusters with atomic monodispersity have been repeatedly reported in the past decade, their Pd analogues have not been reported thus far. In this work, we provide a resolution for the challenging synthesis and obtain for the first time an atomically monodisperse thiolated, reduced Pd (q=+0.75) nanocluster with a di-tetrahedron Pd 8 kernel and a +3 charged interstitial B atom, as revealed by ESI-MS, SCXRD, etc. μ-6 B is found for the first time in Group 10 and 11 metal nanoclusters. More importantly, the as-obtained Pd nanoclusters show better catalytic activity compared to 1.4 nm Pd nanoparticles, Pd 2 complexes and even a commercial Pt/C catalyst for the oxygen reduction reaction (ORR), having significant implications for the influence of the metal charge state and space structure on the catalytic activity.

关键词： Electrocatalysis Interstitial B Atom ORR Nanoclusters Palladium

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Molecular Architecture of Cobalt Porphyrin Multilayers on Reduced Graphene Oxide Sheets for High‐Performance Oxygen Reduction Reaction†

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Angewandte Chemie 2013年第21期125卷

作者： Hongjie Tang Huajie Yin Jiangyan Wang Nailiang Yang Dan Wang Zhiyong Tang State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 (P.R. China) National Center for Nanoscience and Technology No.11 Beiyitiao Zhongguancun Beijing 100190 (P. R. China) University of Chinese Academy of Sciences No. 19A Yuquan Road Beijing 100049 (P. R. China)

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Hard‐Sphere Random Close‐Packed Au47Cd2(TBBT)31Nanoclusters with a Faradaic Efficiency of Up to 96 % for Electrocatalytic CO2Reduction to CO

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Angewandte Chemie 2019年第8期132卷

作者： Shengli Zhuang Dong Chen Lingwen Liao Yan Zhao Nan Xia Wenhao Zhang Chengming Wang Jun Yang Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and Nanotechnology CAS Center for Excellence in Nanoscience Institute of Solid State Physics Chinese Academy of Sciences Hefei 230031 P. R. China Institute of Physical Science and Information Technology Anhui University Hefei Anhui 230601 P. R. China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 P. R. China

Metal nanoclusters have recently attracted considerable attention, not only because of their special size range but also because of their well‐defined compositions and structures. However, subtly tailoring the compositions and structures of metal nanoclusters for potential applications remains challenging. Now, a two‐phase anti‐galvanic reduction (AGR) method is presented for precisely tailoring Au 44 (TBBT) 28 to produce Au 47 Cd 2 (TBBT) 31 nanoclusters with a hard‐sphere random close‐packed structure, exhibiting Faradaic efficiencies of up to 96 % at −0.57 V for the electrocatalytic reduction of CO 2 to CO.

关键词： Cadmium CO2-Reduktion Elektrokatalyse Gold-Nanocluster Antigalvanische Reduktion

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Surface Activation by Single Ru Atoms for Enhanced High-Temperature CO2Electrolysis

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Angewandte Chemie 2023年第5期136卷

作者： Dr. Yuefeng Song Junyong Min Yige Guo Rongtan Li Geng Zou Prof. Dr. Mingrun Li Dr. Yipeng Zang Weicheng Feng Dr. Xiaoqian Yao Dr. Tianfu Liu Dr. Xiaomin Zhang Jingcheng Yu Qingxue Liu Dr. Peng Zhang Prof. Dr. Runsheng Yu Prof. Dr. Xingzhong Cao Prof. Dr. Junfa Zhu Prof. Dr. Kun Dong Prof. Dr. Guoxiong Wang Prof. Dr. Xinhe Bao State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China University of Chinese Academy of Sciences Beijing 100039 China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Multi-disciplinary Research Division Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 China

Cathodic CO 2 adsorption and activation is essential for high-temperature CO 2 electrolysis in solid oxide electrolysis cells (SOECs). However, the component of oxygen ionic conductor in the cathode displays limited electrocatalytic activity. Herein, stable single Ruthenium (Ru) atoms are anchored on the surface of oxygen ionic conductor (Ce 0.8 Sm 0.2 O 2-δ , SDC) via the strong covalent metal-support interaction, which evidently modifies the electronic structure of SDC surface for favorable oxygen vacancy formation and enhanced CO 2 adsorption and activation, finally evoking the electrocatalytic activity of SDC for high-temperature CO 2 electrolysis. Experimentally, SOEC with the Ru 1 /SDC-La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ cathode exhibits a current density as high as 2.39 A cm −2 at 1.6 V and 800 °C. This work expands the application of single atom catalyst to the high-temperature electrocatalytic reaction in SOEC and provides an efficient strategy to tailor the electronic structure and electrocatalytic activity of SOEC cathode at the atomic scale.

关键词： CO2 Electroreduction Electronic Structure Oxygen Vacancy Single Atom Catalyst Solid Oxide Electrolysis Cell

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Surface Atomic Architecture: Engineering Surface Atomic Architecture of NiTe Nanocrystals Toward Efficient Electrochemical N2Fixation (Adv. Funct. Mater. 39/2020)

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Advanced Functional Materials 2020年第39期30卷

作者： Menglei Yuan Qiongguang Li Jingxian Zhang Jiawen Wu Tongkun Zhao Zhanjun Liu Le Zhou Hongyan He Bin Li Guangjin Zhang CAS Key Laboratory of Green Process Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Center of Materials Science and Optoeletronics Engineering University of Chinese Academy of Sciences Beijing 100049 China Beijing Engineering Research Center of Printed Electronics Beijing Institute of Graphic Communication Beijing 102600 China CAS Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 China Zhengzhou Tobacco Research Institute of CNTC No 2 Fengyang Street Zhengzhou High‐Tech Development District Zhengzhou 450001 China

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Unveiling Electrochemical Urea Synthesis by Co-Activation of CO2and N2with Mott–Schottky Heterostructure Catalysts

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Angewandte Chemie 2021年第19期133卷

作者： Menglei Yuan Junwu Chen Yiling Bai Prof. Zhanjun Liu Jingxian Zhang Tongkun Zhao Qin Wang Shuwei Li Prof. Hongyan He Prof. Guangjin Zhang CAS Key Laboratory of Green Process Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China Center of Materials Science and Optoeletronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China CAS Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 P. R. China Engineering Design Department Hebei Enco Petrochemical Engineering Co. Ltd. Henan Branch Henan 450000 P. R. China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031 P. R. China

Electrocatalytic C−N bond coupling to convert CO 2 and N 2 molecules into urea under ambient conditions is a promising alternative to harsh industrial processes. However, the adsorption and activation of inert gas molecules and then the driving of the C–N coupling reaction is energetically challenging. Herein, novel Mott–Schottky Bi-BiVO 4 heterostructures are described that realize a remarkable urea yield rate of 5.91 mmol h −1 g −1 and a Faradaic efficiency of 12.55 % at −0.4 V vs. RHE. Comprehensive analysis confirms the emerging space–charge region in the heterostructure interface not only facilitates the targeted adsorption and activation of CO 2 and N 2 molecules on the generated local nucleophilic and electrophilic regions, but also effectively suppresses CO poisoning and the formation of endothermic *NNH intermediates. This guarantees the desired exothermic coupling of *N=N* intermediates and generated CO to form the urea precursor, *NCON*.

关键词： C–N coupling electrocatalysis Mott–Schottky heterostructures urea

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Efficient Capture and Low Energy Release of NH3by Azophenol Decorated Photoresponsive Covalent Organic Frameworks

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Angewandte Chemie 2024年第34期136卷

作者： Xiaoxin Tian Xiao Zhao Zhenzhen Wang Yunlei Shi Zhiyong Li Jikuan Qiu Huiyong Wang Suojiang Zhang Jianji Wang Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Key Laboratory of Green Chemical Media and Reactions Ministry of Education (China) School of Chemistry and Chemical Engineering Henan Normal University Xinxiang Henan 453007 P. R. China School of Chemistry and Materials Engineering Xinxiang University Xinxiang Henan 453003 P. R. China Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China College of Chemistry and Molecular Sciences Longzihu New Energy Laboratory Henan University Zhengzhou Henan 450000 P. R. China

In NH 3 capture technologies, the desorption process is usually driven by high temperature and low pressure (such as 150–200 °C under vacuum), which accounts for intensive energy consumption and CO 2 emission. Developing light responsive adsorbent is promising in this regard but remains a great challenge. Here, we for the first time designed and synthesized a light responsive azophenol-containing covalent organic framework (COF), COF-HNU38, to address this challenge. We found that at 25 °C and 1.0 bar, the cis -COF exhibited a NH 3 uptake capacity of 7.7 mmol g −1 and a NH 3 /N 2 selectivity of 158. In the adsorbed NH 3 , about 29.0 % could be removed by vis-light irradiated cis-trans isomerization at 25 °C, and the remaining NH 3 might be released at 25 °C under vacuum. Almost no decrease in adsorption capacity was observed after eight adsorption-desorption cycles. As such, an efficient NH 3 capture and low energy release strategy was established thanks to the multiple hydrogen bond interactions (which are strong in total but weak in individuals) between NH 3 and the smart COF, as well as the increased polarity and number of hydrogen bond sites after the trans-cis isomerization.

关键词： ammonia capture Covalent Organic Framework (COF) photo switching azophenol

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Catalytic Transformation of PET and CO2into High-Value Chemicals

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Angewandte Chemie 2022年第10期134卷

作者： Yinwen Li Dr. Meng Wang Dr. Xingwu Liu Prof. Dr. Chaoquan Hu Prof. Dr. Dequan Xiao Prof. Dr. Ding Ma Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University Beijing 100871 P. R. China State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan Shanxi 030001 P. R. China Synfuels China Beijing 100195 P. R. China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 People's Republic of China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211135 P. R. China Center for Integrative Materials Discovery Department of Chemistry and Chemical and Biomedical Engineering University of New Haven West Haven CT 06516 USA

Polyethylene terephthalate (PET) and CO 2 , two chemical wastes that urgently need to be transformed in the environment, are converted simultaneously in a one-pot catalytic process through the synergistic coupling of three reactions: CO 2 hydrogenation, PET methanolysis and dimethyl terephthalate (DMT) hydrogenation. More interestingly, the chemical equilibria of both reactions were shifted forward due to a revealed dual-promotion effect, leading to significantly enhanced PET depolymerization. The overall methanol yield from CO 2 hydrogenation exceeded the original thermodynamic equilibrium limit since the methanol was in situ consumed in the PET methanolysis. The degradation of PET by a stoichiometric ratio of methanol was significantly enhanced because the primary product, DMT was hydrogenated to dimethyl cyclohexanedicarboxylate (DMCD) or p-xylene (PX). This synergistic catalytic process provides an effective way to simultaneously recycle two wastes, polyesters and CO 2 , for producing high-value chemicals.

关键词： CO2 Hydrogenation DMT Hydrogenation Dual-Promotion One-Pot Catalysis PET Methanolysis

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