Atomically dispersed cerium on copper tailors interfacial water structure for efficient CO-to-acetate electroreduction

Xue-Peng Yang, Zhi-Zheng Wu, Ye-Cheng Li, Shu-Ping Sun, Yu-Cai Zhang, Jing-Wen Duanmu, Pu-Gan Lu, Xiao-Long Zhang, Fei-Yue Gao, Yu Yang, Ye-Hua Wang, Peng-Cheng Yu, Shi-Kuo Li () and Min-Rui Gao ()
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Xue-Peng Yang: Anhui University
Zhi-Zheng Wu: University of Science and Technology of China
Ye-Cheng Li: University of Science and Technology of China
Shu-Ping Sun: University of Science and Technology of China
Yu-Cai Zhang: University of Science and Technology of China
Jing-Wen Duanmu: University of Science and Technology of China
Pu-Gan Lu: University of Science and Technology of China
Xiao-Long Zhang: University of Science and Technology of China
Fei-Yue Gao: University of Science and Technology of China
Yu Yang: University of Science and Technology of China
Ye-Hua Wang: University of Science and Technology of China
Peng-Cheng Yu: University of Science and Technology of China
Shi-Kuo Li: Anhui University
Min-Rui Gao: University of Science and Technology of China

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Electrosynthesis of acetate from carbon monoxide (CO) powered by renewable electricity offers one promising avenue to obtain valuable carbon-based products but undergoes unsatisfied selectivity because of the competing hydrogen evolution reaction. We report here a cerium single atoms (Ce-SAs) modified crystalline-amorphous dual-phase copper (Cu) catalyst, in which Ce SAs reduce the electron density of the dual-phase Cu, lowering the proportion of interfacial K+ ion hydrated water (K·H2O) and thereby decreasing the H* coverage on the catalyst surface. Meanwhile, the electron transfer from dual-phase Cu to Ce SAs yields Cu+ species, which boost the formation of active atop-adsorbed *CO (COatop), improving COatop-COatop coupling kinetics. These together lead to the preferential pathway of ketene intermediate (*CH2-C=O) formation, which then reacts with OH- enriched by pulsed electrolysis to generate acetate. Using this catalyst, we achieve a high Faradaic efficiency of 71.3 ± 2.1% toward acetate and a time-averaged acetate current density of 110.6 ± 2.0 mA cm−2 under a pulsed electrolysis mode. Furthermore, a flow-cell reactor assembled by this catalyst can produce acetate steadily for at least 138 hours with selectivity greater than 60%.

Date: 2025
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DOI: 10.1038/s41467-025-58109-6

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