Chen Fei, Bai Chang-Wei, Duan Pi-Jun, Zhang Zhi-Quan, Sun Yi-Jiao, Chen Xin-Jia, Yang Qi, Yu Han-Qing
Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University, Chongqing, 400045, China.
Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, College of Environmental Science and Engineering, Hunan University, Changsha, 410082, China.
Nat Commun. 2024 Sep 6;15(1):7783. doi: 10.1038/s41467-024-52158-z.
The artificial photocatalytic synthesis based on graphitic carbon nitride (g-CN) for HO production is evolving rapidly. However, the simultaneous production of high-value products at electron and hole sites remains a great challenge. Here, we use transformable potassium iodide to obtain semi-crystalline g-CN integrated with the I/I redox shuttle mediators for efficient generation of HO and benzaldehyde. The system demonstrates a prominent catalytic efficiency, with a benzaldehyde yield of 0.78 mol g h and an HO yield of 62.52 mmol g h. Such a constructed system can achieve an impressive 96.25% catalytic selectivity for 2e oxygen reduction, surpassing previously reported systems. The mechanism study reveals that the strong crystal electric field from iodized salt enhances photo-generated charge carrier separation. The I/I redox mediators significantly boost charge migration and continuous electron and proton supply for dual-channel catalytic synthesis. This groundbreaking work in photocatalytic co-production opens neoteric avenues for high-value synthesis.
基于石墨相氮化碳（g-CN）的用于生成羟基自由基（HO）的人工光催化合成技术正在迅速发展。然而，在电子和空穴位点同时生产高价值产品仍然是一个巨大的挑战。在此，我们使用可转化的碘化钾来获得与I/I氧化还原穿梭介质集成的半结晶g-CN，以高效生成HO和苯甲醛。该系统表现出显著的催化效率，苯甲醛产率为0.78 mol g h，HO产率为62.52 mmol g h。这样构建的系统对于2e氧还原可实现高达96.25%的催化选择性，超过了先前报道的系统。机理研究表明，碘盐产生的强晶体电场增强了光生电荷载流子的分离。I/I氧化还原介质显著促进了电荷迁移以及为双通道催化合成持续供应电子和质子。这项光催化联产方面的开创性工作为高价值合成开辟了新途径。
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