Asymmetrically Coordinated Cu Dual‐Atom‐Sites Enables Selective CO 2 Electroreduction to Ethanol

作者：Changli Chen, Zhiyi Sun, Gangzhi Qin, Bingchao Wang, Minggang Liu, Qingru Liang, Xinyu Li, Runzhuo Pang, Yingshu Guo, Yujing Li, Wenxing Chen · 发表于：Advanced Materials · 年份：2024 · DOI：10.1002/adma.202409797 · 被引用次数：74 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Advanced battery technologies research

Abstract Electrochemical reduction of CO 2 (CO 2 RR) to value‐added liquid fuels is a highly attractive solution for carbon‐neutral recycling, especially for C 2+ products. However, the selectivity control to preferable products is a great challenge due to the complex multi‐electron proton transfer process. In this work, a series of Cu atomic dispersed catalysts are synthesized by regulating the coordination structures to optimize the CO 2 RR selectivity. Cu 2 ‐SNC catalyst with a uniquely asymmetrical coordinated CuN 2 ‐CuNS site shows high ethanol selective with the FE of 62.6% at −0.8 V versus RHE and 60.2% at 0.9 V versus RHE in H‐Cell and Flow‐Cell test, respectively. Besides, the nest‐like structure of Cu 2 ‐SNC is beneficial to the mass transfer process and the selection of catalytic products. In situ experiments and theory calculations reveal the reaction mechanisms of such high selectivity of ethanol. The S atoms weaken the bonding ability of the adjacent Cu to the carbon atom, which accelerates the selection from *CHCOH to generate *CHCHOH, resulting in the high selectivity of ethanol. This work indicates a promising strategy in the rational design of asymmetrically coordinated single, dual, or tri‐atom catalysts and provides a candidate material for CO 2 RR to produce ethanol.