Improving CO2‐to‐C2 Conversion of Atomic CuFONC Electrocatalysts through F, O‐Codrived Optimization of Local Coordination Environment.

Electrocatalytic CO2 to multi‐carbon products is an attractive strategy to achieve a carbon‐neutral energy cycle. Single‐atom catalysts (SACs) that achieve the C2 selectivity always have low metal loading and inevitably undergo in situ reversible/irreversible metallic agglomerations under working conditions. Herein, a high‐density Cu SA anchored F, O, N co‐doped carbon composites (CuFONC) with a stable CuN2O1 configuration is provided, which can reach a remarkable C2 selectivity of ≈80.5% in Faradaic efficiency at −1.3 V versus RHE. In situ/ex situ experimental characterization and density functional theory (DFT) calculations verified that the excellent stability of CuN2O1 during the CO2RR process can be attributed to F/O co‐derived regulation for CuFONC. Remarkably, as confirmed by DFT, it is atomic Cu sites and the adjacent bonded N motifs in CuFONC that act as the adsorption sites for CO* during the C─C coupling process. This work brings a prospective on designing novel but stable atomic Cu coordination for electrolytic CO2‐to‐C2 pathway. [ABSTRACT FROM AUTHOR]