Improving CO<sub>2</sub>‐to‐C<sub>2</sub> Conversion of Atomic CuFONC Electrocatalysts through F, O‐Codrived Optimization of Local Coordination Environment
Zunhang Lv, Changli Wang, Yarong Liu, Rui Liu, Fang Zhang, Xiao Feng, Wenxiu Yang, Bo Wang
Abstract
Abstract Electrocatalytic CO 2 to multi‐carbon products is an attractive strategy to achieve a carbon‐neutral energy cycle. Single‐atom catalysts (SACs) that achieve the C 2 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 CuN 2 O 1 configuration is provided, which can reach a remarkable C 2 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 CuN 2 O 1 during the CO 2 RR 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 CO 2 ‐to‐C 2 pathway.