Merging semi-crystallization and multispecies iodine intercalation at photo-redox interfaces for dual high-value synthesis

Fei Chen (), Chang-Wei Bai, Pi-Jun Duan, Zhi-Quan Zhang, Yi-Jiao Sun, Xin-Jia Chen, Qi Yang and Han-Qing Yu ()
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Fei Chen: Chongqing University
Chang-Wei Bai: Chongqing University
Pi-Jun Duan: Chongqing University
Zhi-Quan Zhang: Chongqing University
Yi-Jiao Sun: Chongqing University
Xin-Jia Chen: Chongqing University
Qi Yang: Hunan University
Han-Qing Yu: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-17

Abstract: Abstract The artificial photocatalytic synthesis based on graphitic carbon nitride (g-C3N4) for H2O2 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-C3N4 integrated with the I-/I3- redox shuttle mediators for efficient generation of H2O2 and benzaldehyde. The system demonstrates a prominent catalytic efficiency, with a benzaldehyde yield of 0.78 mol g−1 h−1 and an H2O2 yield of 62.52 mmol g−1 h−1. 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-/I3- 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.

Date: 2024
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DOI: 10.1038/s41467-024-52158-z

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