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.