Insight into selectivity of photocatalytic methane oxidation to formaldehyde on tungsten trioxide

Yingying Fan, Yuheng Jiang, Haiting Lin, Jianan Li, Yuanjiang Xie, Anyi Chen, Siyang Li, Dongxue Han (), Li Niu () and Zhiyong Tang ()
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Yingying Fan: Guangzhou University
Yuheng Jiang: National Center for Nanoscience and Technology
Haiting Lin: Guangzhou University
Jianan Li: Guangzhou University
Yuanjiang Xie: Guangzhou University
Anyi Chen: Guangzhou University
Siyang Li: National Center for Nanoscience and Technology
Dongxue Han: Guangzhou University
Li Niu: Guangzhou University
Zhiyong Tang: National Center for Nanoscience and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Tungsten trioxide (WO3) has been recognized as the most promising photocatalyst for highly selective oxidation of methane (CH4) to formaldehyde (HCHO), but the origin of catalytic activity and the reaction manner remain controversial. Here, we take {001} and {110} facets dominated WO3 as the model photocatalysts. Distinctly, {001} facet can readily achieve 100% selectivity of HCHO via the active site mechanism whereas {110} facet hardly guarantees a high selectivity of HCHO along with many intermediate products via the radical way. In situ diffuse reflectance infrared Fourier transform spectroscopy, electron paramagnetic resonance and theoretical calculations confirm that the competitive chemical adsorption between CH4 and H2O and the different CH4 activation routes on WO3 surface are responsible for diverse CH4 oxidation pathways. The microscopic mechanism elucidation provides the guidance for designing high performance photocatalysts for selective CH4 oxidation.

Date: 2024
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DOI: 10.1038/s41467-024-49138-8

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