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

Title: Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts
Authors: Li, X; Li, C; Xu, Y; Liu, Q; Bahri, M; Zhang, L; Browning, ND; Cowan, AJ; Tang, J
Publisher Information: Springer Science and Business Media LLC
Publication Year: 2023
Collection: The University of Liverpool Repository
Description: 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.
Document Type: article in journal/newspaper
Language: English
ISSN: 2058-7546
Relation: Li, X orcid:0000-0002-6657-3456 , Li, C orcid:0000-0003-0455-9146 , Xu, Y, Liu, Q orcid:0000-0002-5172-4864 , Bahri, M orcid:0000-0002-8336-9158 , Zhang, L, Browning, ND orcid:0000-0003-0491-251X , Cowan, AJ orcid:0000-0001-9032-3548 and Tang, J orcid:0000-0002-2323-5510 (2023) Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts Nature Energy, 8 (9). pp. 1013-1022. ISSN 2058-7546, 2058-7546
DOI: 10.1038/s41560-023-01317-5
Availability: https://livrepository.liverpool.ac.uk/3172985/; https://doi.org/10.1038/s41560-023-01317-5
Accession Number: edsbas.39AF324D
Database: BASE