Li, Xiyi, Li, Chao, Xu, Youxun, Liu, Qiong, Bahri, Mounib 
ORCID: 0000-0002-8336-9158, Zhang, Liquan, Browning, Nigel D ORCID: 0000-0003-0491-251X, Cowan, Alexander J ORCID: 0000-0001-9032-3548 and Tang, Junwang
(2023)
Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO<sub>2</sub> photocatalysts.
NATURE ENERGY, 8 (9).
pp. 1013-1022.
Abstract
<jats:title>Abstract</jats:title><jats:p>Photocatalytic oxidative coupling of methane (OCM) produces C<jats:sub>2</jats:sub> molecules that can be used as building blocks for synthesis of fuels and chemicals. However, the yield rate and the selectivity of C<jats:sub>2</jats:sub> products are still moderate due to the stable nature of methane molecules. Here we develop a Au nanocluster-loaded TiO<jats:sub>2</jats:sub> photocatalyst by a sputtering approach, achieving a high methane conversion rate of 1.1 mmol h<jats:sup>−1</jats:sup>, C<jats:sub>2</jats:sub> selectivity of ~90% and apparent quantum efficiency of 10.3 ± 0.6%. The high C<jats:sub>2</jats:sub>/C<jats:sub>2+</jats:sub> 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<jats:sub>2</jats:sub> photoelectron lifetimes by a factor of 66 for O<jats:sub>2</jats:sub> 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.</jats:p>
| Item Type: | Article |
|---|---|
| Divisions: | Faculty of Science and Engineering > School of Engineering Faculty of Science and Engineering > School of Physical Sciences |
| Depositing User: | Symplectic Admin |
| Date Deposited: | 22 Sep 2023 15:54 |
| Last Modified: | 18 Oct 2023 18:27 |
| DOI: | 10.1038/s41560-023-01317-5 |
| Open Access URL: | https://doi.org/10.1038/s41560-023-01317-5 |
| Related URLs: | |
| URI: | https://livrepository.liverpool.ac.uk/id/eprint/3172985 |
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