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

Yingying Fan,Yuheng Jiang,Haiting Lin,Jianan Li,Yu Xie,Anyi Chen,Siyang Li,Dongxue Han,Li Niu,Zhiyong Tang

Published 2024 in Nature Communications

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. Tungsten trioxide (WO3) is considered the most promising photocatalyst for the highly selective oxidation of methane to formaldehyde, though the origins of its catalytic activity and reaction mechanism are still debated. Here, the authors use WO3 with {001} and {110} facets as model photocatalysts, demonstrating that the photocatalytic oxidation of methane to formaldehyde in WO3 depends on the surface structure, leading to different formaldehyde selectivity.

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