质子化
催化作用
法拉第效率
动力学
化学
质子
选择性
锌
电子转移
化学动力学
产量(工程)
电化学
结晶学
光化学
材料科学
物理化学
离子
有机化学
电极
物理
量子力学
冶金
作者
Jiayi Chen,Zhongjian Li,Xinyue Wang,Xiahan Sang,Sixing Zheng,Shoujie Liu,Bin Yang,Qinghua Zhang,Lecheng Lei,Liming Dai,Yang Hou
标识
DOI:10.1002/ange.202111683
摘要
Abstract Electrocatalytic reduction of CO 2 (CO 2 RR) to value‐added chemicals is of great significance for CO 2 utilization, however the CO 2 RR process involving multi‐electron and proton transfer is greatly limited by poor selectivity and low yield. Herein, We have developed an atomically dispersed monovalent zinc catalyst anchored on nitrogenated carbon nanosheets (Zn/NC NSs). Benefiting from the unique coordination environment and atomic dispersion, the Zn/NC NSs exhibit a superior CO 2 RR performance, featuring a high current density up to 50 mA cm −2 with an outstanding CO Faradaic efficiency of ≈95 %. The center Zn I atom coordinated with three N atoms and one N atom that bridges over two adjacent graphitic edges (Zn‐N 3+1 ) is identified as the catalytically active site. Experimental results reveal that the twisted Zn‐N 3+1 structure accelerates CO 2 activation and protonation in the rate‐determining step of *CO 2 to *COOH, while theoretical calculations elucidate that atomically dispersed Zn‐N 3+1 moieties decrease the potential barriers for intermediate COOH* formation, promoting the proton‐coupled CO 2 RR kinetics and boosting the overall catalytic performance.
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