Membrane electrode assemblies (MEAs) have been developed for electrochemical conversion of CO₂ to high-value multi-carbon (C₂₊) products at industrial current densities (j > 200 mA cm⁻²). However, the effective and simultaneous modulation of CO₂ and H₂O mass transfer within MEA remains a critical issue, particularly at the three-phase interface. Herein, CO₂ and H₂O channels are incorporated into the catalyst layer network to benefit the micro-environment. The balance of local CO₂ and H₂O at the reaction interface is attained by regulating the catalyst-coated ionomer. In situ DEMS further confirms that the rational routes are successfully established for mass transfer management. The interfacial distribution of CO₂ and H₂O is in-depth investigated via in situ ATR-SEIRAS and molecular dynamics (MD) simulation. Through reasonable catalyst layer design, CO₂-to-C₂₊ performance is substantially enhanced, exhibiting remarkable selectivity to C₂₊ products with a faradaic efficiency (FE) of 89.4 ± 0.69% and a partial current density of 536 ± 4.14 mA cm⁻². The optimized Cu-GDE also exhibits excellent stability of >10 h at a total current of 2 A.

中文翻译：

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合理的催化剂层设计可实现量身定制的传输通道，以实现高效的 CO2 电化学还原为多碳产品


膜电极组件 （MEA） 已被开发用于在工业电流密度 （j > 200 mA ^cm-2） 下将 CO₂ 电化学转化为高价值多碳 （C₂₊） 产品。然而，MEA 中 CO₂ 和 H₂O 传质的有效和同步调制仍然是一个关键问题，尤其是在三相界面处。在此，CO₂ 和 H₂O 通道被整合到催化剂层网络中，以有利于微环境。通过调节催化剂包被的离聚物，可以在反应界面上实现局部 CO₂ 和 H₂O 的平衡。原位DEMS 进一步确认已成功建立合理的路由以进行质量传递管理。通过原位 ATR-SEIRAS 和分子动力学 （MD） 模拟深入研究了 CO₂ 和 H₂O 的界面分布。通过合理的催化剂层设计，CO₂ 对 C₂₊ 性能得到显著提高，对 C₂₊ 产物表现出显着的选择性，法拉第效率 （FE） 为 89.4 ± 0.69%，部分电流密度为 536 ± 4.14 mA ^cm-2。优化的 Cu-GDE 在 2 A 的总电流下还表现出出色的 >10 h 稳定性。