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<p>Elucidating the fundamental mechanisms underlying Cu reconstruction is paramount for the rational design of catalysts that meet the stringent activity, selectivity, and durability requirements for industrial-scale CO<sub>2</sub>/CO electroreduction (CO<sub>2</sub>RR/CORR). While both dissolution-redeposition and atomic migration pathways have been proposed, the operational conditions dictating their relative dominance remain poorly understood. Through quasi <i>in situ</i> Cu<sup>+</sup> detection and <i>in situ</i> atomic force microscopy (AFM), we reveal a striking mechanistic dichotomy: Cu reconstruction during CO<sub>2</sub>RR occurs strictly in the presence of Cu<sup>+</sup>, whereas CORR-induced reconstruction proceeds independently of Cu<sup>+</sup> species. These findings suggest that Cu reconstruction in CO<sub>2</sub>RR follows a dissolution-redeposition mechanism induced by oxidative radicals, while atomic migration emerges as the dominant pathway in CORR. Density functional theory calculations further demonstrate that adsorbed *CO intermediates reduce Cu–Cu bond strength, creating metastable surface configurations that promote Cu atomic migration. These insights provide a foundation for leveraging reconstruction to design high-performance Cu-based catalysts.</p>

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Identifying Cu reconstruction mechanism in CO2 and CO electroreduction via Cu+ detection and in situ atomic force microscopy

  • 期刊论文

  • 发表日期：

    2025年6月3日

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  • Yunpei Yue,
  • Zhitan Wu,
  • Zilin Ye,
  • Zhiguo Li,
  • Xinyu Wang,
  • Kai Xie,
  • Daliang Han,
  • Quan-Hong Yang,
  • Zhe Weng

摘要

Elucidating the fundamental mechanisms underlying Cu reconstruction is paramount for the rational design of catalysts that meet the stringent activity, selectivity, and durability requirements for industrial-scale CO2/CO electroreduction (CO2RR/CORR). While both dissolution-redeposition and atomic migration pathways have been proposed, the operational conditions dictating their relative dominance remain poorly understood. Through quasi in situ Cu+ detection and in situ atomic force microscopy (AFM), we reveal a striking mechanistic dichotomy: Cu reconstruction during CO2RR occurs strictly in the presence of Cu+, whereas CORR-induced reconstruction proceeds independently of Cu+ species. These findings suggest that Cu reconstruction in CO2RR follows a dissolution-redeposition mechanism induced by oxidative radicals, while atomic migration emerges as the dominant pathway in CORR. Density functional theory calculations further demonstrate that adsorbed *CO intermediates reduce Cu–Cu bond strength, creating metastable surface configurations that promote Cu atomic migration. These insights provide a foundation for leveraging reconstruction to design high-performance Cu-based catalysts.