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

Ningdong Feng (), Huiwen Lin, Hui Song, Longxiao Yang, Daiming Tang, Feng Deng and Jinhua Ye ()
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Ningdong Feng: Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences
Huiwen Lin: National Institute for Materials Science (NIMS)
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)

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-24912-0

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