Effective Screening Route for Highly Active and Selective Metal-Nitrogen-Doped Carbon Catalysts in CO₂...

To identify high-efficiency metal-nitrogen-doped (M-N-C) electrocatalysts for the electrochemical CO₂ -to-CO reduction reaction (CO₂ RR), a method that uses density functional theory calculation is presented to evaluate their selectivity, activity, and structural stability. Twenty-three M-N₄ -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 (ΔG_*H -ΔG_*CO ), and *CO desorption energy (ΔG_{*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 CO₂ RR electrocatalysts.