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Selective oxidation of methane to C2+ products over Au-CeO2 by photon-phonon co-driven catalysis.

Wang, Chao; Xu, Youxun; Xiong, Lunqiao; Li, Xiyi; Chen, Enqi; Miao, Tina Jingyan; Zhang, Tianyu; ... Tang, Junwang; + view all (2024) Selective oxidation of methane to C2+ products over Au-CeO2 by photon-phonon co-driven catalysis. Nature Communications , 15 , Article 7535. 10.1038/s41467-024-51690-2. Green open access

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Abstract

Direct methane conversion to high-value chemicals under mild conditions is attractive yet challenging due to the inertness of methane and the high reactivity of valuable products. This work presents an efficient and selective strategy to achieve direct methane conversion through the oxidative coupling of methane over a visible-responsive Au-loaded CeO2 by photon-phonon co-driven catalysis. A record-high ethane yield of 755 μmol h−1 (15,100 μmol g−1 h−1) and selectivity of 93% are achieved under optimised reaction conditions, corresponding to an apparent quantum efficiency of 12% at 365 nm. Moreover, the high activity of the photocatalyst can be maintained for at least 120 h without noticeable decay. The pre-treatment of the catalyst at relatively high temperatures introduces oxygen vacancies, which improves oxygen adsorption and activation. Furthermore, Au, serving as a hole acceptor, facilitates charge separation, inhibits overoxidation and promotes the C-C coupling reaction. All these enhance photon efficiency and product yield.

Type: Article
Title: Selective oxidation of methane to C2+ products over Au-CeO2 by photon-phonon co-driven catalysis.
Location: England
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/s41467-024-51690-2
Publisher version: https://doi.org/10.1038/s41467-024-51690-2
Language: English
Additional information: © The Author(s), 2024. This is an Open Access article distributed under the terms of the Creative Commons Attribution Licence (CC BY 4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. https://creativecommons.org/licenses/by/4.0/
Keywords: Heterogeneous catalysis, Photocatalysis
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10196574
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