The Role of Phase Mixing Degree in Promoting C−C Coupling in Electrochemical CO2 Reduction Reaction on Cu‐based Catalysts

A comprehensive investigation on defect structure-to-activity relationship in electrochemical CO₂ reduction reaction by mixing various phases. The efficiency of C−C coupling increased with phase mixing degree of Cu-based catalysts, with a maximum FE of 81 % toward C2+ products. Mechanistic investigation revealed that the increased phase mixing degree facilitated *CO formation and retention at low and high overpotential, respectively.

Abstract

Cu-based catalysts have been identified as the most promising candidates for generation of C2+ products in electrochemical CO₂ reduction reaction. Defect engineering in catalysts is a widely employed strategy for promoting C−C coupling on Cu. However, comprehensive understanding of defect structure-to-activity relationship has not been obtained. In this study, controllable defects generation is achieved, which leads to a series of Cu-based catalysts with various phase mixing degrees. It is observed that the Faradaic efficiency toward C2+ products increases with the phase mixing degree, reaching 81 % at maximum. In situ infrared absorption spectroscopy reveals that the catalysts with higher phase mixing degree tend to form *CO more easily and possess higher retention of *CO under high overpotential window, thereby promoting C−C coupling. This work sheds new light on the relationship between defects and C−C coupling, and the rational developed of more advanced Cu-base catalysts.

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