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Efficient and selective photocatalytic CH4 conversion to CH3OH with O2 by controlling overoxidation on TiO2

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  • Ningdong Feng

    (Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences
    National Institute for Materials Science (NIMS))

  • Huiwen Lin

    (National Institute for Materials Science (NIMS)
    Nanjing University of Aeronautics and Astronautics)

  • Hui Song

    (National Institute for Materials Science (NIMS))

  • Longxiao Yang

    (Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences)

  • Daiming Tang

    (National Institute for Materials Science (NIMS))

  • Feng Deng

    (Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences)

  • Jinhua Ye

    (National Institute for Materials Science (NIMS)
    Tianjin University)

Abstract

The conversion of photocatalytic methane into methanol in high yield with selectivity remains a huge challenge due to unavoidable overoxidation. Here, the photocatalytic oxidation of CH4 into CH3OH by O2 is carried out on Ag-decorated facet-dominated TiO2. The {001}-dominated TiO2 shows a durable CH3OH yield of 4.8 mmol g−1 h−1 and a selectivity of approximately 80%, which represent much higher values than those reported in recent studies and are better than those obtained for {101}-dominated TiO2. Operando Fourier transform infrared spectroscopy, electron spin resonance, and nuclear magnetic resonance techniques are used to comprehensively clarify the underlying mechanism. The straightforward generation of oxygen vacancies on {001} by photoinduced holes plays a key role in avoiding the formation of •CH3 and •OH, which are the main factors leading to overoxidation and are generally formed on the {101} facet. The generation of oxygen vacancies on {001} results in distinct intermediates and reaction pathways (oxygen vacancy → Ti–O2• → Ti–OO–Ti and Ti–(OO) → Ti–O• pairs), thus achieving high selectivity and yield for CH4 photooxidation into CH3OH.

Suggested Citation

  • Ningdong Feng & Huiwen Lin & Hui Song & Longxiao Yang & Daiming Tang & Feng Deng & Jinhua Ye, 2021. "Efficient and selective photocatalytic CH4 conversion to CH3OH with O2 by controlling overoxidation on TiO2," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24912-0
    DOI: 10.1038/s41467-021-24912-0
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    Cited by:

    1. Chengyang Feng & Shouwei Zuo & Miao Hu & Yuanfu Ren & Liwei Xia & Jun Luo & Chen Zou & Sibo Wang & Yihan Zhu & Magnus Rueping & Yu Han & Huabin Zhang, 2024. "Optimizing the reaction pathway of methane photo-oxidation over single copper sites," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Huizhen Zhang & Pengfei Sun & Xiaozhen Fei & Xuejiao Wu & Zongyi Huang & Wanfu Zhong & Qiaobin Gong & Yanping Zheng & Qinghong Zhang & Shunji Xie & Gang Fu & Ye Wang, 2024. "Unusual facet and co-catalyst effects in TiO2-based photocatalytic coupling of methane," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Yingying Fan & Yuheng Jiang & Haiting Lin & Jianan Li & Yuanjiang Xie & Anyi Chen & Siyang Li & Dongxue Han & Li Niu & Zhiyong Tang, 2024. "Insight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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