Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles

• Published in: Journal of the American Chemical Society 2024-12
• Main Authors: Zhang, Libing, Feng, Jiaqi, Wang, Ruhan, Wu, Limin, Song, Xinning, Jin, Xiangyuan, Tan, Xingxing, Jia, Shunhan, Ma, Xiaodong, Jing, Lihong, Zhu, Qinggong, Kang, Xinchen, Zhang, Jianling, Sun, Xiaofu, Han, Buxing
• Format: Article
• Language: English
• ISSN: 1520-5126; 1520-5126
• DOI: 10.1021/jacs.4c13197

The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of the catalyst. CO /CO electroreduction has recently emerged as a potential approach for obtaining C products, but it is challenging to achieve high selectivity for a single C product. Herein, we develop a Cu atomic ensemble that satisfies the appropriate site distance and coordination environment required for electrocatalytic CO-to-acetate conversion, which shows outstanding overall performance with an acetate Faradaic efficiency of 70.2% with a partial current density of 225 mA cm and a formation rate of 2.1 mmol h cm . Moreover, a single-pass CO conversion rate of 91% and remarkable stability can be also obtained. Detailed experimental and theoretical investigations confirm the significant advantages of the Cu atomic ensembles in optimizing C-C coupling, stabilizing key ketene intermediate (*CCO), and inhibiting the *HOCCOH intermediate, which can switch the CO reduction pathway from the ethanol/ethylene on the conventional metallic Cu site to the acetate on the Cu atomic ensembles.