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

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 coupli...

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Bibliographic Details
Published in:Nature communications 2024-08, Vol.15 (1), p.7535-12, Article 7535
Main Authors: Wang, Chao, Xu, Youxun, Xiong, Lunqiao, Li, Xiyi, Chen, Enqi, Miao, Tina Jingyan, Zhang, Tianyu, Lan, Yang, Tang, Junwang
Format: Article
Language:English
Subjects:
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Catalysis
Catalysts
Catalytic converters
Cerium oxides
Charge efficiency
Chemical reactions
Coupling
Ethane
High temperature
Humanities and Social Sciences
Methane
multidisciplinary
Oxidation
Oxygen
Phonons
Photons
Quantum efficiency
Science
Science (multidisciplinary)
Selectivity
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Summary: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 CeO 2 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. To achieve high yield and selectivity of C 2+ products from methane conversion, the authors report a photon-phonon co-driven catalytic process using CeO 2 catalysts. Gold, as a co-catalyst, promotes C-C coupling and suppresses overoxidation
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-024-51690-2