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<p>The efficient electrochemical CO<sub>2</sub> reduction to C<sub>2+</sub> products at high current densities remains a significant challenge. Here we show inherently hydrophobic and hierarchically porous Cu supraparticles comprising sub-10 nm Cu constituent particles for ampere-level CO<sub>2</sub>-to-C<sub>2+</sub> electrosynthesis. These supraparticles feature abundant grain boundaries for high C<sub>2+</sub> selectivity, coupled with interconnected mesopores and interparticle macropore cavities to enhance the accessibility of the active sites and mass transfer, breaking the trade-off between activity and mass transfer in Cu-based catalysts. Moreover, the intrinsic hydrophobicity of the supraparticles mitigates the water-flooding issue of catalytic layer in flow cells, improving the stability at high current densities. Consequently, the Cu supraparticles achieve ampere-level CO<sub>2</sub> electrolysis up to 3.2 A cm<sup>-2</sup> with a C<sub>2+</sub> Faradaic efficiency of 74.9% (compared to 1.21 A cm<sup>-2</sup> and 55.4% for Cu nanoparticles) and maintain stability at 1 A cm<sup>-2</sup> for over 100 h. This work provides profound insights into the effect of the coupling of mass transfer and catalytic reaction under a high current and presents a corresponding solution by superstructure design.</p>

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Cu supraparticles with enhanced mass transfer and abundant C-C coupling sites achieving ampere-level CO2-to-C2+ electrosynthesis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月10日

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  • Lushan Ma,
  • Hong Liu,
  • Bingbao Mei,
  • Jing Chen,
  • Qingqing Cheng,
  • Jingyuan Ma,
  • Bo Yang,
  • Qiang Li,
  • Hui Yang

摘要

The efficient electrochemical CO2 reduction to C2+ products at high current densities remains a significant challenge. Here we show inherently hydrophobic and hierarchically porous Cu supraparticles comprising sub-10 nm Cu constituent particles for ampere-level CO2-to-C2+ electrosynthesis. These supraparticles feature abundant grain boundaries for high C2+ selectivity, coupled with interconnected mesopores and interparticle macropore cavities to enhance the accessibility of the active sites and mass transfer, breaking the trade-off between activity and mass transfer in Cu-based catalysts. Moreover, the intrinsic hydrophobicity of the supraparticles mitigates the water-flooding issue of catalytic layer in flow cells, improving the stability at high current densities. Consequently, the Cu supraparticles achieve ampere-level CO2 electrolysis up to 3.2 A cm-2 with a C2+ Faradaic efficiency of 74.9% (compared to 1.21 A cm-2 and 55.4% for Cu nanoparticles) and maintain stability at 1 A cm-2 for over 100 h. This work provides profound insights into the effect of the coupling of mass transfer and catalytic reaction under a high current and presents a corresponding solution by superstructure design.