Li, Xiyi;
Li, Chao;
Xu, Youxun;
Liu, Qiong;
Bahri, Mounib;
Zhang, Liquan;
Browning, Nigel D;
... Tang, Junwang; + view all
(2023)
Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts.
Nature Energy
10.1038/s41560-023-01317-5.
(In press).
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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.
| Type: | Article |
|---|---|
| Title: | Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41560-023-01317-5 |
| Publisher version: | https://doi.org/10.1038/s41560-023-01317-5 |
| Language: | English |
| Additional information: | This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
| Keywords: | Nanoparticles, Photocatalysis, Photochemistry, Solar fuels |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10175656 |
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