Sulfur‐modulated charge‐asymmetry Cu–Zn bimetallic nanoclusters for efficient CO 2 electroreduction

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CO 2 electroreduction (CO 2 RR) represents a promising negative‐carbon technology, which is in urgent need for efficient and high‐selectivity catalysts. Here, a support control strategy is employed for precise surface engineering of charge‐asymmetry nanocluster catalyst (CuZnSCN), in which zinc and copper atoms together form a metal cluster loaded on sulfur and nitrogen co‐etched carbon matrix. The synergistic promotion mechanism of CO 2 RR by Cu–Zn atom interactions and sulfur–nitrogen atom doping was investigated. A CO partial current density of 74.1 mA cm −2 was achieved in an alkaline electrolyte, as well as a considerable CO Faraday efficiency of 97.7%. In situ XAS (X‐ray absorption spectroscopy) showed that the stabilization of Cu + and Zn 2+ species in the nanoclusters and doped sulfur atoms during the CO 2 RR process contributes to the sustained adsorption of protons and the generation and conversion of the CO. This work verifies the possibility of metal‐support and intermetallic interactions to synergistically enhance electrochemical catalytic performance and provides ideas for further bimetallic cluster catalyst development.