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Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates

Author

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  • Xiao Sun

    (University of Science and Technology of China)

  • Xuanye Chen

    (University of Science and Technology of China)

  • Cong Fu

    (University of Science and Technology of China)

  • Qingbo Yu

    (Anhui University of Science and Technology)

  • Xu-Sheng Zheng

    (University of Science and Technology of China)

  • Fei Fang

    (University of Science and Technology of China)

  • Yuanxu Liu

    (Anhui University of Chinese Medicine, Anhui Academy of Chinese Medicine)

  • Junfa Zhu

    (University of Science and Technology of China)

  • Wenhua Zhang

    (University of Science and Technology of China)

  • Weixin Huang

    (University of Science and Technology of China
    Chinese Academy of Sciences)

Abstract

H2O2 is widely used as an oxidant for photocatalytic methane conversion to value-added chemicals over oxide-based photocatalysts under mild conditions, but suffers from low utilization efficiencies. Herein, we report that O2 is an efficient molecular additive to enhance the utilization efficiency of H2O2 by suppressing H2O2 adsorption on oxides and consequent photogenerated holes-mediated H2O2 dissociation into O2. In photocatalytic methane conversion over an anatase TiO2 nanocrystals predominantly enclosed by the {001} facets (denoted as TiO2{001})-C3N4 composite photocatalyst at room temperature and ambient pressure, O2 additive significantly enhances the utilization efficiency of H2O2 up to 93.3%, giving formic acid and liquid-phase oxygenates selectivities respectively of 69.8% and 97% and a formic acid yield of 486 μmolHCOOH·gcatalyst−1·h−1. Efficient charge separation within TiO2{001}-C3N4 heterojunctions, photogenerated holes-mediated activation of CH4 into ·CH3 radicals on TiO2{001} and photogenerated electrons-mediated activation of H2O2 into ·OOH radicals on C3N4, and preferential dissociative adsorption of methanol on TiO2{001} are responsible for the active and selective photocatalytic conversion of methane to formic acid over TiO2{001}-C3N4 composite photocatalyst.

Suggested Citation

  • Xiao Sun & Xuanye Chen & Cong Fu & Qingbo Yu & Xu-Sheng Zheng & Fei Fang & Yuanxu Liu & Junfa Zhu & Wenhua Zhang & Weixin Huang, 2022. "Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34563-4
    DOI: 10.1038/s41467-022-34563-4
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    2. Xiyi Li & Chao Wang & Jianlong Yang & Youxun Xu & Yi Yang & Jiaguo Yu & Juan J. Delgado & Natalia Martsinovich & Xiao Sun & Xu-Sheng Zheng & Weixin Huang & Junwang Tang, 2023. "PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    3. Xiangcheng Zhang & Silian Cheng & Chao Chen & Xue Wen & Jie Miao & Baoxue Zhou & Mingce Long & Lizhi Zhang, 2024. "Keto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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