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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 ORCID: https://orcid.org/0000-0002-6620-4335, He, Qian ORCID: https://orcid.org/0000-0003-4891-3581, Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731, Jenkins, Robert L., Willock, David J. ORCID: https://orcid.org/0000-0002-8893-1090, Taylor, Stuart H. ORCID: https://orcid.org/0000-0002-1933-4874, Kiely, Christopher J. ORCID: https://orcid.org/0000-0001-5412-0970 and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 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: Chemistry
Cardiff Catalysis Institute (CCI)
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: 16 Apr 2024 19:50
URI: https://orca.cardiff.ac.uk/id/eprint/104762

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