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Single Pt atom decorated graphitic carbon nitride as an efficient photocatalyst for the hydrogenation of nitrobenzene into aniline

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Abstract

The hydrogenation of nitrobenzene into aniline is one of industrially important reactions, but still remains great challenge due to the lack of highly active, chemo-selective and eco-friendly catalyst. By using extensive density functional theory (DFT) calculations, herein we predict that single Pt atom decorated g-C3N4 (Pt@g-C3N4) exhibits excellent catalytic activity and selectivity for the conversion of nitrobenzene into aniline under visible light. The overall activation energy barrier for the hydrogenation of nitrobenzene on single atom Pt@g-C3N4 catalyst is even lower than that of the bare Pt(111) surface. The dissociation of N–O bonds on single Pt atom is triggered by single hydrogen atom rather than double hydrogen atoms on the Pt(111) surface. Moreover, the Pt@g-C3N4 catalyst exhibits outstanding chemoselectivity towards the common reducible substituents, such as phenyl,–C=C,–C≡C and–CHO groups during the hydrogenation. In addition, the doped single Pt atom can significantly enhance the photoconversion efficiency by broadening the light absorption of the pristine g-C3N4 to visible light region. Our results highlight an interesting and experimentally synthesized single-atom photocatalyst (Pt@g-C3N4) for efficient hydrogenation of nitrobenzene to aniline under a sustainable and green approach.

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Acknowledgements

We acknowledge generous grants of high-performance computing resources provided by NCI National Facility and The Pawsey Supercomputing Centre through the National Computational Merit Allocation Scheme supported by the Australian Government and the Government of Western Australia. A. D. also greatly appreciates the financial support of the Australian Research Council under Discovery Project (No. DP170103598).

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  1. School of Chemistry, Physics and Mechanical Engineering, Science and Engineering Faculty, Queensland University of Technology, Gardens Point Campus, Brisbane, QLD, 4001, Australia

    Tianwei He, Chunmei Zhang, Lei Zhang & Aijun Du

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  1. Tianwei He
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He, T., Zhang, C., Zhang, L. et al. Single Pt atom decorated graphitic carbon nitride as an efficient photocatalyst for the hydrogenation of nitrobenzene into aniline. Nano Res. 12, 1817–1823 (2019). https://doi.org/10.1007/s12274-019-2439-z

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