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<p>Electroreduction of CO<sub>2</sub> or CO can produce renewable ethanol—a valuable industrial chemical. However, the limited energy and carbon efficiencies of reported systems present practical challenges. Here we introduce p-block elements into copper catalysts, enabling electrosynthesis of ethanol from CO for 200 h and delivering a full-cell energy efficiency of 22% and a carbon efficiency of 50%, seven-fold better than state-of-the-art. Density functional theory calculations indicate that the lead-doped copper catalyst enhances the cleavage of C–O bonds in *OCH<sub><i>x</i></sub> molecules formed during CO hydrogenation. This enhances the cross-coupling reaction between *CO and *CH<sub><i>x</i></sub> species favouring ethanol production, as opposed to the conventional *CO dimerization pathway that primarily yields ethylene. Using a set of in situ spectroscopic techniques, we show that the addition of lead to copper catalysts expedites the generation of *OCH<sub><i>x</i></sub> species and increases the coverage of *CH<sub><i>x</i></sub> species, thereby enhancing their coupling with *CO and improving ethanol production, in agreement with our theoretical predictions.</p><p></p>

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Electrosynthesis of ethanol via CO–CHx cross-coupling on copper alloy catalysts with engineered oxygen affinity

  • 期刊论文

  • 发表日期：

    2025年9月1日

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  • Pengyu Liu,
  • Ning Sun,
  • Jie Su,
  • Yiyan Wang,
  • Zheng Peng,
  • Shoushun Chen,
  • Panagiotis Papangelakis,
  • Adnan Ozden,
  • Rui Kai Miao,
  • Xiu Wang,
  • Yi Xu,
  • Jianrong Zeng,
  • Haibin Wang,
  • Hanqi Liu,
  • Yanan Zhao,
  • Shucheng Shi,
  • Mohsen Shakouri,
  • Hongyan Liang,
  • Ziyun Wang,
  • Hui Zhang,
  • Yongfeng Hu,
  • Zhenpeng Yao,
  • David Sinton,
  • Jun Li

摘要

Electroreduction of CO2 or CO can produce renewable ethanol—a valuable industrial chemical. However, the limited energy and carbon efficiencies of reported systems present practical challenges. Here we introduce p-block elements into copper catalysts, enabling electrosynthesis of ethanol from CO for 200 h and delivering a full-cell energy efficiency of 22% and a carbon efficiency of 50%, seven-fold better than state-of-the-art. Density functional theory calculations indicate that the lead-doped copper catalyst enhances the cleavage of C–O bonds in *OCHx molecules formed during CO hydrogenation. This enhances the cross-coupling reaction between *CO and *CHx species favouring ethanol production, as opposed to the conventional *CO dimerization pathway that primarily yields ethylene. Using a set of in situ spectroscopic techniques, we show that the addition of lead to copper catalysts expedites the generation of *OCHx species and increases the coverage of *CHx species, thereby enhancing their coupling with *CO and improving ethanol production, in agreement with our theoretical predictions.