Asymmetric C–C Coupling to Drive CO Conversion to Acetate

作者：Jia Liu, Ouwen Peng, Derong Chen, Xiaocang Han, Shibo Xi, Qikun Hu, Zixuan Gao, Yijia Yuan, Kun Zhang, Kian Ping Loh · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c07400 · 被引用次数：11 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Electrocatalysts for Energy Conversion

Electrochemical reduction of carbon monoxide (CORR) provides pathways for decarbonizing chemical manufacturing by producing high-value multicarbon (C 2+ ) products, though achieving high activity and selectivity toward a single principal C 2+ product remains challenging. Acetate, a critical liquid product, can be metabolized by bacteria to synthesize long-chain carbon compounds. Here, we design a core–shell Cu 2 O/Cu-2-methylimidazole (CuIM) catalyst with dual Cu sites (Cu + and Cu 0 ) during the CORR, which shifts the reaction pathway from symmetric *CO–*CO coupling to asymmetric *CH 2 –*CO coupling, thereby enhancing acetate formation. Ex situ X-ray diffraction spectroscopy (XRD) and in situ attenuated total reflection Fourier transform infrared (ATR-FTIR) analyses reveal that Cu + remains stable and acts as an active site for generating *CH 2 intermediates on the CuIM catalyst. The CuIM electrocatalyst achieves a Faradaic efficiency (FE) of 77.8% for acetate production from CO and a partial current density of 541.3 mA cm –2 . These advancements enable high energy efficiency in membrane electrode assemblies and reduced downstream separation costs for liquid products in solid-state electrolyte systems.