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 coupling of methane over a visible-responsive Au-loaded CeO<sub>2</sub> by photon-phonon co-driven catalysis. A record-high ethane yield of 755 μmol h<sup>-1</sup> (15,100 μmol g<sup>-1</sup> h<sup>-1</sup>) 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.

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Publication Details

Journal
Nature Communications
Published
2024-08-30
DOI
https://doi.org/10.1038/s41467-024-51690-2
Citations
56
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
6.56

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article

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

Xiyi Li, Junwang Tang, Yang Lan, Enqi Chen et al.
56 citations
Nature Communications
Catalytic Processes in Materials Science
6.56
article

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

Xiyi Li, Junwang Tang, Yang Lan, Enqi Chen, Tina Jingyan Miao, Lunqiao Xiong, Youxun Xu, Chao Wang, Tianyu Zhang
article en
56 citations

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 CeO<sub>2</sub> by photon-phonon co-driven catalysis. A record-high ethane yield of 755 μmol h<sup>-1</sup> (15,100 μmol g<sup>-1</sup> h<sup>-1</sup>) 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.

Nature CommunicationsVol. 15(1)
Beijing Forestry University (CN), University College London (GB), Tsinghua University (CN)
National Natural Science Foundation of China, China Scholarship Council, Engineering and Physical Sciences Research Council, National Natural Science Foundation of China-Yunnan Joint Fund
Openalex Percentile: Top 1%
Catalytic Processes in Materials Science
6.56
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