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<p>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<sup>+</sup> ion hydrated water (K·H<sub>2</sub>O) and thereby decreasing the H<sup>*</sup> coverage on the catalyst surface. Meanwhile, the electron transfer from dual-phase Cu to Ce SAs yields Cu<sup>+</sup> species, which boost the formation of active atop-adsorbed <sup>*</sup>CO (CO<sub>atop</sub>), improving CO<sub>atop</sub>-CO<sub>atop</sub> coupling kinetics. These together lead to the preferential pathway of ketene intermediate (<sup>*</sup>CH<sub>2</sub>-C=O) formation, which then reacts with OH<sup>-</sup> 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<sup>−2</sup> 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%.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月21日

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  • 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,
  • Min-Rui Gao

摘要

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%.