Chem. J. Chinese Universities ›› 2022, Vol. 43 ›› Issue (2): 20210640.doi: 10.7503/cjcu20210640

• Physical Chemistry • Previous Articles     Next Articles

Optimal Distribution of Active Sites of CO2 Reduction Reaction Catalyzed by Diatomic Site M-N-C

ZHOU Ying, HE Peinan, FENG Haisong, ZHANG Xin()   

  1. State Key Laboratory of Chemical Resource Engineering,College of Chemistry,Beijing University of Chemical Technology,Beijing 100029,China
  • Received:2021-09-06 Online:2022-02-10 Published:2021-11-11
  • Contact: ZHANG Xin E-mail:zhangxin@mail.buct.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(22173003);the National Key Research and Development Program of China(2021YFC2103501)

Abstract:

The diatomic site M-N-C catalysts are one of the best catalysts for CO2 reduction reaction(CO2RR). However, the current researches mainly focus on the regulation of the atom type of the active center of M-N-C, and underestimate the effect of the coordination environment and distribution of the active sites on their catalytic performance. A typical diatomic site M-N-C catalyst(NiFe-N-C) was selected as the research object, and the electrocatalytic CO2RR reaction mechanism of nine types of NiFe-N-C catalysts with different coordination environments at active sites were systematically investigated by the density functional theory(DFT) method. The results show that with the increase of the coordination number of metal atoms and the distance between diatomic sites, the stability of M-N-C catalysts, the catalytic activity of CO2 reduction to CO, and the selectivity of inhibiting hydrogen evolution reaction all show a trend of increasing first and then decreasing. Among them, the NiFe-N-C-model 3 catalyst with four-coordinated and symmetrically distributed metal atoms exhibits the best catalytic performance due to the strong interaction of the diatomic sites. This study provides theoretical support for the precise regulation of active sites in diatomic site M-N-C catalysts and the rational design of CO2RR catalysts.

Key words: M-N-C Catalyst, CO2 Reduction reaction, Active site distribution, Theoretical calculation

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