Dual-atom active sites embedded in two-dimensional C2N for efficient CO2 electroreduction: A computational study

Double-atom catalysts (DACs) have emerged as an enhanced platform of single-atom catalyst for promoting electrocatalytic CO2 reduction reaction (CO2RR). Herein, we present a density-functional theory study on CO2RR performance seven C2N-supported homo- and heteronuclear DACs, denoted M2@C2N. Our results demonstrate that there exists substantial synergistic effect dual-metal-atom N2M2N2 active site C2N matrix OCO bond activation. The dual-atom M2 sites are able to drive beyond C1 products with low limiting potential (UL). Specifically, C2H4 formation is preferred [email protected]2N (M = Fe, Co, Ni, Cu) versus CH4 Cu). Furthermore, *CO+*CO co-binding strength can serve descriptor activity making C2 such the moderate binding in lowest UL. Remarkably, C-affinity matters most CC coupling while both C- O-affinity control formation. provide theoretical insight into rational design DACs efficient CO2RR.