Unique Geometrical and Electronic Properties of TM₂B₂ Quadruple Active Sites Supported on C₂N Monolayer Toward Effective Electrochemical Urea Production

Abstract Developing high‐performance electrocatalysts for urea production using CO 2 and N 2 holds great potential to mitigate environmental pollution and energy crisis. In this study, 26 kinds of quadruple TM 2 B 2 ensembles supported on porous C 2 N monolayer are designed as the potential electrocatalysts, with the expectation to provide sufficient space for the co‐adsorption of CO 2 and N 2 and fulfill a synergistic effect of transition metal (TM) and boron atoms. Cr 2 B 2 @C 2 N is selected as the promising electrocatalyst with a record‐low limiting potential of −0.37 V (vs RHE) in the neutral environment, by using a three‐step screening strategy, i.e., stability of the catalyst, adsorption pattern of N 2 ,…