文献类型：期刊文献

英文题名：Cation-Exchange Induced Precise Regulation of Single Copper Site Triggers Room-Temperature Oxidation of Benzene

作者：Zhou, Huang[1,2];Zhao, Yafei[1,2];Gan, Jie[5];Xu, Jie[6,7];Wang, Ying[3,4];Lv, Hongwei[1,2];Fang, Shi[2];Wang, Zhiyuan[1,2];Deng, Ziliang[6,7];Wang, Xiaoqian[1,2];Liu, Peigen[1,2];Guo, Wenxin[1,2];Mao, Boyang[8];Wang, Huijuan[9];Yao, Tao[2];Hong, Xun[1,2];Wei, Shiqiang[2];Duan, Xuezhi[5];Luo, Jun[6,7];Wu, Yuen[1,2]

机构：[1]Univ Sci & Technol China, Collaborat Innovat Ctr Chem Energy Mat iChEM, Sch Chem & Mat Sci, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China;[2]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China;[3]Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China;[4]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[5]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[6]Tianjin Univ Technol, Ctr Electron Microscopy, Tianjin 300384, Peoples R China;[7]Tianjin Univ Technol, Tianjin Key Lab Adv Funct Porous Mat, Inst New Energy Mat & Low Carbon Technol, Tianjin 300384, Peoples R China;[8]Univ Manchester, Natl Graphene Inst, Manchester M13 9PL, Lancs, England;[9]Univ Sci & Technol China, Ctr Micro & Nanoscale Res & Fabricat, Hefei 230026, Peoples R China

年份：2020

卷号：142

期号：29

起止页码：12643

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20203409077752);WOS:【SCI-EXPANDED(收录号:WOS:000555420600014)】；

基金：This work was supported by National Key R&D Program of China 2017YFA (0208300 and 0700104), the National Natural Science Foundation of China (21522107, 21671180, 21521091, U1463202, 21873050, 51971157, and 51761165012), the Tianjin Science Fund for Distinguished Young Scholars, and the National Program for Support of Top-Notch Young Professionals, Shanghai Rising-Star Program (18QA1404300). We thank the photoemission endstations BL1W1B in Beijing Synchrotron Radiation Facility (BSRF), BL14W1 in Shanghai Synchrotron Radiation Facility (SSRF), and BL10B and BL11U in National Synchrotron Radiation Laboratory (NSRL) for the help in characterizations.

语种：英文

外文关键词：Positive ions - Catalyst activity - Coordination reactions - Copper - Sulfur compounds - Catalyst selectivity - High resolution transmission electron microscopy

摘要：The controllable synthesis of stable single-metal site catalysts with an expected coordination environment for high catalytic activity and selectivity is still challenging. Here, we propose a cation-exchange strategy for precise production of an edge-rich sulfur (S) and nitrogen (N) dual-decorated single-metal (M) site catalysts (M = Cu, Pt, Pd, etc.) library. Our strategy relies on the anionic frameworks of sulfides and N-rich polymer shell to generate abundant S and N defects during high-temperature annealing, further facilitating the stabilization of exchanged metal species with atomic dispersion and excellent accessibility. This process was traced by in situ transmission electron microscopy, during which no metal aggregates were observed. Both experiments and theoretical results reveal the precisely obtained S, N dual-decorated Cu sites exhibit a high activity and low reaction energy barrier in catalytic hydroxylation of benzene at room temperature. These findings provide a route to controllably produce stable single-metal site catalysts and an engineering approach for regulating the central metal to improve catalytic performance.