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Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions

Agarwal, Nishtha, Freakley, Simon J., McVicker, Rebecca U., Althahban, Sultan M., Dimitratos, Nikolaos, He, Qian, Morgan, David J., Jenkins, Robert L., Willock, David J., Taylor, Stuart H., Kiely, Christopher J. and Hutchings, Graham J. 2017. Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions. Science 358 (6360) , pp. 223-227. 10.1126/science.aan6515

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Abstract

The selective oxidation of methane, the primary component of natural gas, remains an important challenge in catalysis. We used colloidal gold-palladium nanoparticles, rather than the same nanoparticles supported on titanium oxide, to oxidize methane to methanol with high selectivity (92%) in aqueous solution at mild temperatures. Then, using isotopically labeled oxygen (O2) as an oxidant in the presence of hydrogen peroxide (H2O2), we demonstrated that the resulting methanol incorporated a substantial fraction (70%) of gas-phase O2. More oxygenated products were formed than the amount of H2O2 consumed, suggesting that the controlled breakdown of H2O2 activates methane, which subsequently incorporates molecular oxygen through a radical process. If a source of methyl radicals can be established, then the selective oxidation of methane to methanol using molecular oxygen is possible.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Cardiff Catalysis Institute (CCI)
Chemistry
Publisher: American Association for the Advancement of Science
ISSN: 0036-8075
Date of First Compliant Deposit: 19 September 2017
Date of Acceptance: 25 August 2017
Last Modified: 28 Mar 2019 22:27
URI: http://orca.cf.ac.uk/id/eprint/104762

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