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<p>The rapid increase in atmospheric CO<sub>2</sub> levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO<sub>2</sub> reduction presents a sustainable solution; however, conventional systems suffer from inefficient charge separation and limited product applicability. Herein, a green and scalable tandem strategy is developed by integrating S-scheme photocatalysis with palladium-catalyzed carbonylation. A rationally designed CeO<sub>2</sub>/Bi<sub>2</sub>S<sub>3</sub> heterojunction leverages its hierarchical structure, broad visible-light absorption, oxygen-vacancy-mediated charge dynamics, and the S-scheme charge transfer mechanism to achieve highly efficient photocatalytic CO<sub>2</sub>-to-CO conversion (14.05 mmol g<sup>−1</sup>, 98% selectivity). The generated CO is directly utilized in a subsequent carbonylation reaction under mild conditions, yielding high-value amides with near-quantitative CO utilization. This integrated approach eliminates the risks of CO handling and enhances economic viability, providing a direct and effective route for converting CO<sub>2</sub> into fine chemicals. By bridging photocatalysis with industrial catalysis, this work advances sustainable carbon recycling technologies and opens avenues for the development of efficient CO<sub>2</sub> conversion systems.</p>

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Integrating S-scheme photocatalysis with tandem carbonylation: A green and scalable strategy for CO2 valorization

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月25日

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  • Feiyan Xu,
  • Feifan Zhao,
  • Xianyu Deng,
  • Jinfeng Zhang,
  • Jianjun Zhang,
  • Chenbin Ai,
  • Jiaguo Yu,
  • Hermenegildo García

摘要

The rapid increase in atmospheric CO2 levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO2 reduction presents a sustainable solution; however, conventional systems suffer from inefficient charge separation and limited product applicability. Herein, a green and scalable tandem strategy is developed by integrating S-scheme photocatalysis with palladium-catalyzed carbonylation. A rationally designed CeO2/Bi2S3 heterojunction leverages its hierarchical structure, broad visible-light absorption, oxygen-vacancy-mediated charge dynamics, and the S-scheme charge transfer mechanism to achieve highly efficient photocatalytic CO2-to-CO conversion (14.05 mmol g−1, 98% selectivity). The generated CO is directly utilized in a subsequent carbonylation reaction under mild conditions, yielding high-value amides with near-quantitative CO utilization. This integrated approach eliminates the risks of CO handling and enhances economic viability, providing a direct and effective route for converting CO2 into fine chemicals. By bridging photocatalysis with industrial catalysis, this work advances sustainable carbon recycling technologies and opens avenues for the development of efficient CO2 conversion systems.