Xu Feiyan, Zhao Feifan, Deng Xianyu, Zhang Jinfeng, Zhang Jianjun, Ai Chenbin, Yu Jiaguo, García Hermenegildo
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan, P. R. China.
Instituto Universitario de Tecnología Química, CSIC-UPV, Universitat Politècnica de València, Valencia, Spain.
Nat Commun. 2025 Jul 25;16(1):6882. doi: 10.1038/s41467-025-60961-5.
The rapid increase in atmospheric CO levels due to industrialization underscores the urgent need for innovative carbon valorization strategies. Photocatalytic CO 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/BiS 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-to-CO conversion (14.05 mmol g, 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 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 conversion systems.
工业化导致大气中一氧化碳（CO）水平迅速上升，这凸显了对创新碳 valorization 策略的迫切需求。光催化 CO 还原提供了一种可持续的解决方案；然而，传统系统存在电荷分离效率低下和产品适用性有限的问题。在此，通过将 S 型光催化与钯催化的羰基化反应相结合，开发了一种绿色且可扩展的串联策略。合理设计的 CeO/BiS 异质结利用其分级结构、广泛的可见光吸收、氧空位介导的电荷动力学以及 S 型电荷转移机制，实现了高效的光催化 CO 到 CO 的转化（14.05 mmol g，98% 选择性）。生成的 CO 在温和条件下直接用于后续的羰基化反应，以近乎定量的 CO 利用率生成高价值的酰胺。这种集成方法消除了 CO 处理的风险并提高了经济可行性，为将 CO 转化为精细化学品提供了一条直接有效的途径。通过将光催化与工业催化相结合，这项工作推动了可持续碳循环技术的发展，并为高效 CO 转化系统的开发开辟了道路。
