Regulating the coordination environment of Co single atoms for achieving efficient electrocatalytic activity in CO2 reduction

被引:262
作者
Geng, Zhigang [1 ]
Cao, Yuanjie [2 ]
Chen, Wenxing [3 ]
Kong, Xiangdong [1 ]
Liu, Yan [1 ]
Yao, Tao [2 ]
Lin, Yue [1 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
[3] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
Co single-atom catalysts; N coordinated environment; CO2 electrochemical reduction; METAL-ORGANIC FRAMEWORKS; ELECTROCHEMICAL REDUCTION; OXYGEN EVOLUTION; CARBON-MONOXIDE; ELECTROREDUCTION; STRATEGY; SELECTIVITY; NANOSHEETS; OXIDATION; CATALYSTS;
D O I
10.1016/j.apcatb.2018.08.075
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Regulating the coordination environment of Co single-atom catalysts represents a powerful strategy to enhance its catalytic performance for CO2 electrochemical reduction. Herein, we adopt metal-organic frameworks (MOFs) to assist the preparation of Co single-atom catalysts with four-coordinated N and four-coordinated N/C on N-doped porous carbon. The atomic dispersion of Co atoms species on the N-doped porous carbon were confirmed using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) analysis. XAFS results revealed that the coordination number of the N binding to the Co single atom was strongly dependent on the pyrolysis temperature. The Co atoms with four-coordinated N on N-doped porous carbon (Co-1 -N-4) exhibited a Faradaic efficiency of 82% and a current density of -15.8 mA cm(-2) for CO production in CO2 electrochemical reduction. Moreover, the Co-1-N-4 catalytic site also held remarkable stability for 10-hour potentiostatic test towards CO2 electrochemical reduction. Mechanistic study further revealed that the Co-1-N-4 active site promotes the binding strength of CO2 and facilitates CO2 activation, which was responsible for its excellent CO2 electrochemical reduction performance.
引用
收藏
页码:234 / 240
页数:7
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