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Visible-light-driven oxidative coupling of primary amines with high selectivity in air over Ni/Ce-doped defective carbon nitride

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Abstract

Visible-light-driven photocatalysis is a sustainable, low-cost, and stable, method for chemical conversion in organic processes. A novel porous g-C3N4 nanosheet (CN) photocatalytic material co-doped with nickel and cerium has been synthesized using a one-step thermal polymerization method. We used XPS, XRD, EPR, UV–vis DRS, SEM, and PL to disclose the structural, optical, and electrical features of the catalysts. Experiments with EPR radical trapping confirmed the existence of reactive oxygen species and holes in the photocatalytic activity. The charge transfer and separation efficiency of the produced catalysts were evaluated using EIS and photocurrent measurements. Ni/Ce-doped CN nanosheets showed improved photocatalytic activities under visible light irradiation, with NiCe-CN showing the best performance with 98% conversion after 2.5 h, and product selectivity exceeding 99% in light-driven amine-imine oxidation reactions. Radical trapping experiments reveal the importance of generating h+, 1O2, and \(\cdot {\text{O}}_{2}^{ - }\) for photocatalytic conversion of substrates, with relevant catalytic mechanisms presented. This study provides a crucial reference for designing and synthesizing novel bimetallic co-doped g-C3N4 photocatalytic materials to enhance photocatalytic organic synthesis reactions.

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Acknowledgements

We gratefully acknowledge the financial support by the National Natural Science Foundation of China (22278333), the Natural Science Foundation of Shaanxi Province (2020JM-434).

Funding

This study was funded by National Natural Science Foundation of China, 22278333, Yonghui Tian, Natural Science Foundation of Shaanxi Province, 2020JM-434, Yonghui Tian.

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  1. Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, College of Chemistry & Materials Science, Northwest University, Xi’an, 710069, Shaanxi, China

    Xian-De Zhou & Yong-Hui Tian

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Yong-Hui Tian conceived the idea and directed the project. Xian-De Zhou performed the experiments and analyzed the data and provided starting materials and participated in characterization studies. Xian-De Zhou wrote the manuscript, and all authors read and approved the manuscript.

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Zhou, XD., Tian, YH. Visible-light-driven oxidative coupling of primary amines with high selectivity in air over Ni/Ce-doped defective carbon nitride. J Mater Sci: Mater Electron 35, 675 (2024). https://doi.org/10.1007/s10854-024-12416-8

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