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<p>Dual sites, positioned through atomically precise proximity coordination for C–C coupling, serve as an exemplary platform for CO<sub>2</sub>-to-C<sub>2</sub>H<sub>4</sub> conversion. Nonetheless, their surface-only distribution results in inefficient photogenerated electron injection via long-range migration from the bulk phase, leading to inadequate site charge to drive the consecutive electron transfers for C<sub>2</sub>H<sub>4</sub> synthesis. Here we demonstrate a reticular dual-site photocatalyst design by embedding semiconductor units (TiO<sub>2</sub>, polymeric carbon nitride or WO<sub>3</sub>·H<sub>2</sub>O) within ligand-defective copper-based metal–organic frameworks (CuBTC-D/PC). This system demonstrates a 75.5% selectivity in converting CO<sub>2</sub> to C<sub>2</sub>H<sub>4</sub> with H<sub>2</sub>O as the electron donor. The reticular copper dual sites facilitate short-range photogenerated electron transfer from the photocatalyst to active sites, ensuring a sufficient electron concentration for all elementary steps in C<sub>2</sub>H<sub>4</sub> conversion. Enhanced electron injection allows for high C<sub>2</sub>H<sub>4</sub> selectivity even under low-intensity irradiation (~0.4 Sun), demonstrating suitability for solar-driven applications. This work establishes the feasibility of CO<sub>2</sub> photoreduction to C<sub>2</sub>H<sub>4</sub> as a primary product, providing insights into multi-electron CO<sub>2</sub> photoreduction.</p><p></p>

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Reticular copper dual sites embedded with semiconductor particles for selective CO2-to-C2H4 photoreduction

  • 期刊论文

  • 发表日期：

    2025年7月11日

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  • Qixin Zhou,
  • Yan Guo,
  • Yongfa Zhu

摘要

Dual sites, positioned through atomically precise proximity coordination for C–C coupling, serve as an exemplary platform for CO2-to-C2H4 conversion. Nonetheless, their surface-only distribution results in inefficient photogenerated electron injection via long-range migration from the bulk phase, leading to inadequate site charge to drive the consecutive electron transfers for C2H4 synthesis. Here we demonstrate a reticular dual-site photocatalyst design by embedding semiconductor units (TiO2, polymeric carbon nitride or WO3·H2O) within ligand-defective copper-based metal–organic frameworks (CuBTC-D/PC). This system demonstrates a 75.5% selectivity in converting CO2 to C2H4 with H2O as the electron donor. The reticular copper dual sites facilitate short-range photogenerated electron transfer from the photocatalyst to active sites, ensuring a sufficient electron concentration for all elementary steps in C2H4 conversion. Enhanced electron injection allows for high C2H4 selectivity even under low-intensity irradiation (~0.4 Sun), demonstrating suitability for solar-driven applications. This work establishes the feasibility of CO2 photoreduction to C2H4 as a primary product, providing insights into multi-electron CO2 photoreduction.