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

作者：Xiyi Li, Chao Li, Youxun Xu, Qiong Liu, Mounib Bahri, Liquan Zhang, Nigel D. Browning, Alexander J. Cowan, Junwang Tang · 发表于：Nature Energy · 年份：2023 · DOI：10.1038/s41560-023-01317-5 · 被引用次数：243 · 研究领域：Catalytic Processes in Materials Science、Advanced Photocatalysis Techniques、Catalysis and Oxidation Reactions

Abstract Photocatalytic oxidative coupling of methane (OCM) produces C 2 molecules that can be used as building blocks for synthesis of fuels and chemicals. However, the yield rate and the selectivity of C 2 products are still moderate due to the stable nature of methane molecules. Here we develop a Au nanocluster-loaded TiO 2 photocatalyst by a sputtering approach, achieving a high methane conversion rate of 1.1 mmol h −1 , C 2 selectivity of ~90% and apparent quantum efficiency of 10.3 ± 0.6%. The high C 2 /C 2+ 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 TiO 2 photoelectron lifetimes by a factor of 66 for O 2 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.