Surface Modification of Nano‐Cu2O for Controlling CO2 Electrochemical Reduction to Ethylene and Syngas

Abstract In the surroundings of carbon neutrality, nano‐Cu 2 O is considered a promising catalyst for the electrochemical CO 2 reduction reaction (ECO 2 RR), whose improvements in product selectivity still require considerable efforts. Here, we present an efficient strategy for controlling the ECO 2 RR product by modifying the surface of nano‐Cu 2 O, i.e., by controlling the exposed facets via a reductant‐controlled method to achieve the highest C 2 H 4 selectivity (Faradic efficiency=74.1 %) for Cu 2 O‐based catalysts in neutral electrolytes, and introducing a well‐suited metal–organic framework (MOF) coating on the surface of nano‐Cu 2 O to obtain syngas completely with an appropriate H 2 :CO ratio. Detailed mechanism and key intermediate have been illustrated by DFT calculations. Our systematic strategy is expected to control the ECO 2 RR product, improve the selectivity, and provide a reliable method for CO 2 management and the green production of important carbon resources.