Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts

Xiyi Li, Chao Li, Youxun Xu, Qiong Liu, Mounib Bahri, Liquan Zhang, Nigel D. Browning, Alexander J. Cowan () and Junwang Tang ()
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Xiyi Li: University College London
Chao Li: University of Liverpool
Youxun Xu: University College London
Qiong Liu: Guangdong Academy of Sciences (China National Analytical Center, Guangzhou)
Mounib Bahri: University of Liverpool
Liquan Zhang: University College London
Nigel D. Browning: University of Liverpool
Alexander J. Cowan: University of Liverpool
Junwang Tang: University College London

Nature Energy, 2023, vol. 8, issue 9, 1013-1022

Abstract: Abstract Photocatalytic oxidative coupling of methane (OCM) produces C2 molecules that can be used as building blocks for synthesis of fuels and chemicals. However, the yield rate and the selectivity of C2 products are still moderate due to the stable nature of methane molecules. Here we develop a Au nanocluster-loaded TiO2 photocatalyst by a sputtering approach, achieving a high methane conversion rate of 1.1 mmol h−1, C2 selectivity of ~90% and apparent quantum efficiency of 10.3 ± 0.6%. The high C2/C2+ yield rate is on the same order of magnitude as the benchmark thermal catalysts in OCM processes operated at high temperature (>680 °C). Au nanoparticles are shown to prolong TiO2 photoelectron lifetimes by a factor of 66 for O2 reduction, together with Au acting as a hole acceptor and catalytic centre to promote methane adsorption, C–H activation and C–C coupling. This work underscores the importance of multifunctional co-catalysts and mechanistic understanding to improve photocatalytic OCM.

Date: 2023
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DOI: 10.1038/s41560-023-01317-5

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