Sustainedly High‐Rate Electroreduction of CO2 to Multi‐Carbon Products on Nickel Oxygenate/Copper Interfacial Catalysts

Abstract Copper (Cu) is the most attractive electrocatalyst for CO 2 reduction to multi‐carbon (C 2+ ) products with high economic value in considerable amounts. However, the rational design of a structurally stable Cu‐based catalyst that can achieve high activity and stability towards C 2+ products remain a grand challenge. Here, a highly stable nickel oxygenate/Cu electrocatalyst is developed with abundant NiOOH/Cu interfaces by in situ electrochemical reconstruction. The nickel oxygenate/Cu electrocatalyst achieves a superior Faradaic efficiency of 86.3 ± 3.0% and a record partial current density of 2085 A g −1 for C 2+ products with long‐term stability. In situ experimental and theoretical studies demonstrates that the exceptional performance in generating C 2+ products is attributed to the presence of the NiOOH/Cu interfaces which increase *CO coverage, lower energy barrier for *CO coupling and stabilize *OCCO simultaneously. This work provides new insights into the rational design of electrocatalysts to achieve stable and efficient electrocatalytic CO 2 reduction capabilities.