Integrating S-scheme photocatalysis with tandem carbonylation: A green and scalable strategy for CO2 valorization
Feiyan Xu, Feifan Zhao, Xianyu Deng, Jinfeng Zhang, Jianjun Zhang, C.F. Ai, Jiaguo Yu, Hermenegildo Garcı́a
Abstract
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. Tandem photocatalytic CO2 reduction and carbonylation reactions are explored to efficiently create amides from CO, amines, and aryl iodides. This approach offers a green, scalable route for carbon recycling and fine chemical production under mild conditions