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MoOx nanoclusters on Mo-doped TiO2 nanosheets with enhanced singlet oxygen generation and sulfide conversion abilities for photocatalytic aerobic oxidative desulfurization

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Abstract

Photocatalytic aerobic oxidation desulfurization (PAODS) is a promising and sustainable alternative to conventional, energy-intensive desulfurization techniques for petroleum products. However, its development is greatly plagued by the low capability in generating highly reactive oxygen species and sluggish kinetics of sulfide oxidation of reported photocatalysts. Here we report a class of MoOx nanocluster decorated on ultrathin Mo-doped TiO2 nanosheet (MoOx/MoTiO) catalyst for efficiently facilitating the photocatalytic aerobic oxidation of sulfides. We demonstrate that MoOx/MoTiO can not only promote the generation of highly reactive singlet oxygen (1O2) but also enhance the aerobic conversion of sulfides, which leads to a record dibenzothiophene oxidation activity of 3.90 mmol g−1 h−1. The multiple experimental characterizations and density functional theory calculations collectively reveal that the doped-Mo sites can interact with the photogenerated excitons, enabling directly energy transfer generation of 1O2 through a new exciton modulation mechanism, and the coordination unsaturated MoOx clusters play the role of co-catalyst to enhance the separation of charge carriers, and effectively catalyze the reaction between sulfides and 1O2 to form sulfones.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21808098, 52261135633, 52025133), the National Key R&D Program of China (2022YFE0128500), the Project of Shandong Province Higher Educational Science (2022KJ122), and Yantai Science and Technology Development Program (2019XDHZ106).

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Authors and Affiliations

  1. College of Chemistry and Materials Science, Ludong University, Yantai, 264025, China

    Suting Xie, Xinyu Zhao, Dongxiao Wang, Huawei Yang, Lixia Yang, Liangjiu Bai, Donglei Wei, Wenxiang Wang, Ying Liang & Hou Chen

  2. College of Materials Science and Engineering, Peking University, Beijing, 100871, China

    Huawei Yang & Shaojun Guo

Authors
  1. Suting Xie
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  2. Xinyu Zhao
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  3. Dongxiao Wang
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  4. Huawei Yang
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  5. Lixia Yang
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  6. Liangjiu Bai
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  7. Donglei Wei
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  11. Shaojun Guo
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Correspondence to Huawei Yang or Shaojun Guo.

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Supporting information The supporting information is available online at https://chem.scichina.com and https://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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11426_2023_1728_MOESM1_ESM.pdf

MoOx nanoclusters on Mo-doped TiO2 nanosheets with enhanced singlet oxygen generation and sulfide conversion abilities for photocatalytic aerobic oxidative desulfurization

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Xie, S., Zhao, X., Wang, D. et al. MoOx nanoclusters on Mo-doped TiO2 nanosheets with enhanced singlet oxygen generation and sulfide conversion abilities for photocatalytic aerobic oxidative desulfurization. Sci. China Chem. 67, 408–414 (2024). https://doi.org/10.1007/s11426-023-1728-6

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  • DOI: https://doi.org/10.1007/s11426-023-1728-6

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