Selective oxidation of methane to C<sub>2+</sub> products over Au-CeO<sub>2</sub> by photon-phonon co-driven catalysis.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 39214973.
- Also identified by DOI 10.1038/s41467-024-51690-2 and PMC identifier 11364766.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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.