Silver Single-Atom Catalyst for Efficient Electrochemical CO2 Reduction Synthesized from Thermal Transformation and Surface Reconstruction. - 文章详情页

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We　report　an　Ag1　single-atom　catalyst　(Ag1　/MnO2　),　which　was　synthesized　from　thermal　transformation　of　Ag　nanoparticles　(NPs)　and　surface　reconstruction　of　MnO2　.　The　evolution　process　of　Ag　NPs　to　single　atoms　is　firstly　revealed　by　various　techniques,　including　in situ　ETEM,　in situ　XRD　and　DFT　calculations.　The　temperature-induced　surface　reconstruction　process　from　the　MnO2　(211)　to　(310)　lattice　plane　is　critical　to　firmly　confine　the　existing　surface　of　Ag　single　atoms;　that　is,　the　thermal　treatment　and　surface　reconstruction　of　MnO2　is　the　driving　force　for　the　formation　of　single　Ag　atoms.　The　as-obtained　Ag1　/MnO2　achieved　95.7　%　Faradic　efficiency　at　-0.85 V　vs.　RHE,　and　coupled　with　long-term　stability　for　electrochemical　CO2　reduction　reaction　(CO2　RR).　DFT　calculations　indicated　single　Ag　sites　possessed　high　electronic　density　close　to　Fermi　Level　and　could　act　exclusively　as　the　active　sites　in　the　CO2　RR.　As　a　result,　the　Ag1　/MnO2　catalyst　demonstrated　remarkable　performance　for　the　CO2　RR,　far　surpassing　the　conventional　Ag　nanosized　catalyst　(AgNP　/MnO2　)　and　other　reported　Ag-based　catalysts.

关键词：

silver CO2 reduction reaction surface reconstruction anti-Ostwald ripening

作者机构：

[ 1 ] [Zhang Ningqiang]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
[ 2 ] [Zhang Xinxin]Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, P. R. China
[ 3 ] [Tao Lei]Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China
[ 4 ] [Jiang Peng]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
[ 5 ] [Ye Chenliang]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
[ 6 ] [Lin Rui]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
[ 7 ] [Huang Zhiwei]Department of Environmental Science & Engineering, Huaqiao University, Xiamen, 361021, P. R. China
[ 8 ] [Li Ang]Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100124, P. R. China
[ 9 ] [Pang Dawei]Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100124, P. R. China
[ 10 ] [Yan Han]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
[ 11 ] [Wang Yu]Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, P. R. China
[ 12 ] [Xu Peng]CAS Key Laboratory of Standardization and Measurement for Nanotechnology, National Center for Nanoscience and Technology, Beijing, 100190, P. R. China
[ 13 ] [An Sufeng]State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China
[ 14 ] [Zhang Qinghua]Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China
[ 15 ] [Liu Licheng]Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, P. R. China
[ 16 ] [Du Shixuan]Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China
[ 17 ] [Han Xiaodong]Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, 100124, P. R. China
[ 18 ] [Wang Dingsheng]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China
[ 19 ] [Li Yadong]Department of Chemistry, Tsinghua University, Beijing, 100084, P. R. China

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