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<p>Selective producing CH<sub>4</sub> by CO<sub>2</sub> electroreduction remains challenging, primarily hindered by the complexity of reduction products, sluggish protonation kinetics, and competitive hydrogen evolution reaction. Herein, we developed a silica-copper composite catalyst (CuO/SiO<sub>2</sub>), where CuO nanoparticles are dispersed on the hydroxyl-functionalized SiO<sub>2</sub> nanosheet. The hydroxyl-functionalized SiO<sub>2</sub> support promotes the formation and transfer of interfacial reactive hydrogen species, lowers the energy barrier for the reduction of CO<sub>2</sub> to CH<sub>4</sub> by stabilizing *COOH, *CO, and *H intermediates. Meanwhile, it favors the hydrogenation of *CHO over C—C coupling between C1 intermediates, thereby shifting product selectivity from multi-carbon products towards CH<sub>4</sub>. As a result, CuO/SiO<sub>2</sub> catalyst delivers high CH<sub>4</sub> selectivity over a broad current density range of 0.2–0.9 A/cm<sup>2</sup>, with a peak Faradaic efficiency of 66.2% at 0.6 A/cm<sup>2</sup>. This work demonstrates an effective interfacial engineering strategy for enhancing the selectivity of CO<sub>2</sub>-to-CH<sub>4</sub> conversion.</p>

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Hydroxyl-functionalized SiO2-supported CuO Composite Catalysts Enabling Highly Selective CO2 Electroreduction to CH4 at Industrial Current Densities

  • 期刊论文

  • 发表日期：

    2026年5月16日

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  • Siheng Yang,
  • Qinyuan Hu,
  • Yuxuan Kong,
  • Yuehan Cao,
  • Weiyao Hu,
  • Lei Ran,
  • Xueli Zheng,
  • Haiyan Fu,
  • Hua Chen,
  • Ruixiang Li,
  • Chong Cheng,
  • Shuang Li,
  • Weichao Xue,
  • Jiaqi Xu

摘要

Selective producing CH4 by CO2 electroreduction remains challenging, primarily hindered by the complexity of reduction products, sluggish protonation kinetics, and competitive hydrogen evolution reaction. Herein, we developed a silica-copper composite catalyst (CuO/SiO2), where CuO nanoparticles are dispersed on the hydroxyl-functionalized SiO2 nanosheet. The hydroxyl-functionalized SiO2 support promotes the formation and transfer of interfacial reactive hydrogen species, lowers the energy barrier for the reduction of CO2 to CH4 by stabilizing *COOH, *CO, and *H intermediates. Meanwhile, it favors the hydrogenation of *CHO over C—C coupling between C1 intermediates, thereby shifting product selectivity from multi-carbon products towards CH4. As a result, CuO/SiO2 catalyst delivers high CH4 selectivity over a broad current density range of 0.2–0.9 A/cm2, with a peak Faradaic efficiency of 66.2% at 0.6 A/cm2. This work demonstrates an effective interfacial engineering strategy for enhancing the selectivity of CO2-to-CH4 conversion.