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

doi:10.1021/jacs.4c13197

Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles

J Am Chem Soc. 2024 Dec 17. doi: 10.1021/jacs.4c13197. Online ahead of print.

Authors

Libing Zhang^{1

2}, Jiaqi Feng^{1

3}, Ruhan Wang^{1

2}, Limin Wu^{1

2}, Xinning Song^{1

2}, Xiangyuan Jin^{1

2}, Xingxing Tan¹, Shunhan Jia^{1

2}, Xiaodong Ma¹, Lihong Jing¹, Qinggong Zhu^{1

2}, Xinchen Kang^{1

2}, Jianling Zhang^{1

2}, Xiaofu Sun^{1

2}, Buxing Han^{1

2

4}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
² School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
³ State Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), Beijing 102249, China.
⁴ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.

PMID: 39688936
DOI: 10.1021/jacs.4c13197

Abstract

The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of the catalyst. CO₂/CO electroreduction has recently emerged as a potential approach for obtaining C₂₊ products, but it is challenging to achieve high selectivity for a single C₂₊ 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.