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<p>Efficient electrocatalysts should provide optimal binding sites for intermediates under operating conditions. Atomic rearrangements in catalysts during electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) alter the original structures of active sites. Here we report a general principle for understanding and predicting the reconstruction of Cu bimetallic catalysts during CO<sub>2</sub>RR in terms of selective dissolution–redeposition. We categorize the reconstruction trends of Cu bound to a secondary metal (X, where X = Ag, Fe, Zn or Pd) according to the oxophilicity and miscibility of Cu and X. Cross-sectional microscopy analysis of gas diffusion electrodes reveals that the surface states of reconstructed Cu–X are determined by atomic miscibility. We find that CO<sub>2</sub>RR intermediates alter elemental preferences for dissolution, shifting them away from oxophilicity-governed behaviour and leading to selective Cu dissolution–redeposition in Cu–X. This reconstruction affects spillover in CO<sub>2</sub>RR, controlling the selectivities of ethylene/ethanol and C<sub>1</sub>/C<sub>2</sub> products. We also develop a methodology for the control of reconstruction dynamics. Our findings provide insights into designing catalysts that undergo reconstruction during electrolysis.</p><p></p>

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Unveiling the reconstruction of copper bimetallic catalysts during CO2 electroreduction

  • 期刊论文

  • 发表日期：

    2025年7月14日

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  • Intae Kim,
  • Gi-Baek Lee,
  • Sungin Kim,
  • Hyun Dong Jung,
  • Ji-Yong Kim,
  • Taemin Lee,
  • Hyesung Choi,
  • Jaeyeon Jo,
  • Geosan Kang,
  • Sang-Ho Oh,
  • Woosuck Kwon,
  • Deokgi Hong,
  • Hyoung Gyun Kim,
  • Yujin Lee,
  • Unggi Kim,
  • Hyeontae Kim,
  • Miyoung Kim,
  • Seoin Back,
  • Jungwon Park,
  • Young-Chang Joo,
  • Dae-Hyun Nam

摘要

Efficient electrocatalysts should provide optimal binding sites for intermediates under operating conditions. Atomic rearrangements in catalysts during electrochemical CO2 reduction reaction (CO2RR) alter the original structures of active sites. Here we report a general principle for understanding and predicting the reconstruction of Cu bimetallic catalysts during CO2RR in terms of selective dissolution–redeposition. We categorize the reconstruction trends of Cu bound to a secondary metal (X, where X = Ag, Fe, Zn or Pd) according to the oxophilicity and miscibility of Cu and X. Cross-sectional microscopy analysis of gas diffusion electrodes reveals that the surface states of reconstructed Cu–X are determined by atomic miscibility. We find that CO2RR intermediates alter elemental preferences for dissolution, shifting them away from oxophilicity-governed behaviour and leading to selective Cu dissolution–redeposition in Cu–X. This reconstruction affects spillover in CO2RR, controlling the selectivities of ethylene/ethanol and C1/C2 products. We also develop a methodology for the control of reconstruction dynamics. Our findings provide insights into designing catalysts that undergo reconstruction during electrolysis.