Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles
Libing Zhang, Jiaqi Feng, Ruhan Wang, Limin Wu, Xinning Song, Xiangyuan Jin, Xingxing Tan, Shunhan Jia, Xiaodong Ma, Lihong Jing, Qinggong Zhu, Xinchen Kang, Jianling Zhang, Xiaofu Sun, Buxing Han
Abstract
The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of the catalyst. CO 2 /CO electroreduction has recently emerged as a potential approach for obtaining C 2+ products, but it is challenging to achieve high selectivity for a single C 2+ 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 –2 and a formation rate of 2.1 mmol h –1 cm –2 . 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.