Creating interfaces of Cu⁰/Cu⁺ in oxide-derived copper catalysts for electrochemical CO₂ reduction to multi-carbon...

Electrochemical carbon dioxide reduction reaction (CO₂RR) is an effective approach to capture CO₂ and convert it into value-added chemicals and fuels, thereby reducing excess CO₂ emissions. Recent reports have shown that copper-based catalysts exhibit excellent performance in converting CO₂ into multi-carbon compounds and hydrocarbons. However, theselectivityto the couplingproductsispoor. Therefore, tuningCO₂-reductionselectivitytoward C₂₊productsover Cu-based catalyst is one of the most important issues in CO₂RR. Herein, we prepare a nanosheet catalyst with interfaces of Cu⁰/Cu⁺. The catalyst achieves Faraday efficiency (FE) of C₂₊ over 50% in a wide potential window between - 1.2 V to - 1.5 V versus reversible hydrogen electrode (vs. RHE). Moreover, the catalyst exhibits maximum FE of 44.5% and 58.9% towards C₂H₄ and C₂₊, with a partial current density of 10.5 mA cm^-2 at - 1.4 V. Density functional theory (DFT) calculations show that the interface of Cu⁰/Cu⁺ facilitates CC coupling to form C₂₊ products, while inhibits CO₂conversion toC₁products.