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Intermediates Adsorption Engineering of CO2 Electroreduction Reaction in Highly Selective Heterostructure Cu‐Based Electrocatalysts for CO Production

The challenge in the artificial CO2 reduction to fuel is achieving high selective electrocatalysts. Here, a highly selective Cu2O/CuO heterostructure electrocatalyst is developed for CO2 electroreduction. The Cu2O/CuO nanowires modified by Ni nanoparticles exhibit superior catalytic performance with high faradic efficiency (95% for CO). Theoretical and experimental analyses show that the hybridization of Cu2O/CuO nanowires and Ni nanoparticles can not only adjust the d‐band center of electrocatalysts to enhance the intrinsic catalytic activity but also improve the adsorption of COOH* intermediates and suppress the hydrogen evolution reaction to promote the CO conversion efficiency during CO2 reduction reaction. An in situ Raman spectroscopic study further confirms the existence of COOH* species and the engineering intermediates adsorption. This work offers new insights for facile designing of nonprecious transition metal compound heterostructure for CO2 reduction reaction through adjusting the reaction pathway.