Unusual facet and co-catalyst effects in TiO2-based photocatalytic coupling of methane

Huizhen Zhang, Pengfei Sun, Xiaozhen Fei, Xuejiao Wu, Zongyi Huang, Wanfu Zhong, Qiaobin Gong, Yanping Zheng, Qinghong Zhang, Shunji Xie (), Gang Fu () and Ye Wang ()
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Huizhen Zhang: Xiamen University
Pengfei Sun: Xiamen University
Xiaozhen Fei: Xiamen University
Xuejiao Wu: Xiamen University
Zongyi Huang: Xiamen University
Wanfu Zhong: Xiamen University
Qiaobin Gong: Xiamen University
Yanping Zheng: Xiamen University
Qinghong Zhang: Xiamen University
Shunji Xie: Xiamen University
Gang Fu: Xiamen University
Ye Wang: Xiamen University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Photocatalytic coupling of methane to ethane and ethylene (C2 compounds) offers a promising approach to utilizing the abundant methane resource. However, the state-of-the-art photocatalysts usually suffer from very limited C2 formation rates. Here, we report our discovery that the anatase TiO2 nanocrystals mainly exposing {101} facets, which are generally considered less active in photocatalysis, demonstrate surprisingly better performances than those exposing the high-energy {001} facet. The palladium co-catalyst plays a pivotal role and the Pd2+ site on co-catalyst accounts for the selective C2 formation. We unveil that the anatase {101} facet favors the formation of hydroxyl radicals in aqueous phase near the surface, where they activate methane molecules into methyl radicals, and the Pd2+ site participates in facilitating the adsorption and coupling of methyl radicals. This work provides a strategy to design efficient nanocatalysts for selective photocatalytic methane coupling by reaction-space separation to optimize heterogeneous-homogeneous reactions at solid-liquid interfaces.

Date: 2024
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DOI: 10.1038/s41467-024-48866-1

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