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<p>Understanding the impact of cell architectures on product selectivity and the carbon–carbon coupling mechanism of the CO<sub>2</sub> electrochemical reduction reaction remains a central challenge due to the complex mass transport conditions of reactants and intermediates. Here we demonstrate that introducing a porous protective layer on copper-based gas diffusion electrodes in flow cells can modulate the mass transport of both the reactant and an intermediate, and can bridge the activity gap between flow cell and membrane electrode assembly configurations. Electrokinetic investigations in flow cells with and without a protective layer provide direct evidence of the Eley–Rideal mechanism in the copper-catalysed carbon–carbon coupling step. Coelectrolysis of <sup>12</sup>CO<sub>2</sub>/<sup>13</sup>CO in different reactor configurations reveals that the interfacial microenvironment depends sensitively on the interplay between surface reactions and mass transport from and to the catalyst layer.</p><p></p>

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Evidence of Eley–Rideal mechanism in Cu-catalysed CO2 electroreduction in flow cells with a protective layer

  • 期刊论文

  • 发表日期：

    2026年7月30日

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  • Qiwen Sun,
  • Yao Ye,
  • Zebang Yin,
  • Gong Zhang,
  • Xiaoxia Chang,
  • Jinlong Gong,
  • Bingjun Xu

摘要

Understanding the impact of cell architectures on product selectivity and the carbon–carbon coupling mechanism of the CO2 electrochemical reduction reaction remains a central challenge due to the complex mass transport conditions of reactants and intermediates. Here we demonstrate that introducing a porous protective layer on copper-based gas diffusion electrodes in flow cells can modulate the mass transport of both the reactant and an intermediate, and can bridge the activity gap between flow cell and membrane electrode assembly configurations. Electrokinetic investigations in flow cells with and without a protective layer provide direct evidence of the Eley–Rideal mechanism in the copper-catalysed carbon–carbon coupling step. Coelectrolysis of 12CO2/13CO in different reactor configurations reveals that the interfacial microenvironment depends sensitively on the interplay between surface reactions and mass transport from and to the catalyst layer.