Effective Screening Route For Highly Active And Selective Metal-Nitrogen-Doped Carbon Catalysts In Co2 Electrochemical Reduction

To identify high-efficiency metal-nitrogen-doped (M-N-C) electrocatalysts for the electrochemical CO2-to-CO reduction reaction (CO2RR), a method that uses density functional theory calculation is presented to evaluate their selectivity, activity, and structural stability. Twenty-three M-N-4-C catalysts are evaluated, and three of them (M = Fe, Co, or Ni) are identified as promising candidates. They are synthesized and tested as proof-of-concept catalysts for CO2-to-CO conversion. Different key descriptors, including the maximum reaction energy, differences of the *H and *CO binding energy (Delta G(*H)-Delta G(*CO)), and *CO desorption energy (Delta G(*CO -> CO()(g)())), are used to clarify the reaction mechanism. These computational descriptors effectively predict the experimental observations in the entire range of electrochemical potential. The findings provide a guideline for rational design of heterogeneous CO2RR electrocatalysts.