Fluorine Doping-Assisted Reconstruction of Isolated Cu Sites for CO Electroreduction Toward Multicarbon Products

The electrocatalytic synthesis of multicarbon compounds from CO is a promising method for storing renewable electricity and addressing global CO issues. Single-atom catalysts are promising candidates for CO reduction, but producing high-value multicarbon (C) products using a single-atom structure remains a significant challenge. In this study, a fluorine doping strategy is proposed to facilitate the reconstruction of isolated Cu atoms, promoting multicarbon generation. The in situ formed Cu nanocrystals contain a substantial amount of stable Cu species, demonstrating remarkable activity for CO-to-multicarbon conversion. Notably, they achieve the highest Cu utilization, with a C partial current density of -2.01 A mg and a C formation rate of 7.03 mmol h mg at ≈-1 V versus RHE. In situ Raman spectroscopy and density functional theory calculations confirm the crucial role of fluorine atoms in structural evolution and electrolysis.