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Selective oxidation of methane to methanol and methyl hydroperoxide over palladium modified MoO3 photocatalyst under ambient conditions

Sun, Songmei, Dummer, Nicholas F., Bere, Takudzwa, Barnes, Alexandra J., Shaw, Greg, Douthwaite, Mark, Pattisson, Samuel, Lewis, Richard J., Richards, Nia, Morgan, David J. and Hutchings, Graham J. 2022. Selective oxidation of methane to methanol and methyl hydroperoxide over palladium modified MoO3 photocatalyst under ambient conditions. Catalysis Science & Technology 12 (11) , pp. 3727-3736. 10.1039/D2CY00240J

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Abstract

Selective partial oxidation of methane to valuable oxygenated products remains a great challenge, as typically over oxidation of oxygenated products to COx is observed. Weak oxidative species on the catalyst surface have a great potential to overcome this limitation. However, weak oxidative species usually have low concentrations and are easily decomposed. Here we report a Pd/MoO3 photocatalyst which can realize excellent methane oxidation to methanol and methyl hydroperoxide in pure water, under simulated solar light by in situ generated H2O2 at room temperature and pressure. The combined selectivity for methanol and methyl hydroperoxide is up to 98.6%, representing a productivity rate of 42.5 μmol gcat−1 h−1. Further studies on the reaction mechanism indicate that PdO species on the Pd loaded MoO3 catalyst play an essential role in the suppression of over oxidation. In this case PdO traps the photo-generated electrons, leaving photo-generated holes for decomposition of H2O2 into weak oxidative hydroperoxyl radicals which are not involved in the formation of over oxidation products.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Additional Information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Publisher: Royal Society of Chemistry
ISSN: 2044-4753
Funders: The Shanghai Science and Technology Commission, the National Natural Science Foundation of China and the European Union's Horizon 2020 research and innovation program under the Marie Sk�odowska-Curie Actions
Date of First Compliant Deposit: 1 July 2022
Date of Acceptance: 1 May 2022
Last Modified: 31 Aug 2022 07:58
URI: https://orca.cardiff.ac.uk/id/eprint/150943

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