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

Nishtha Agarwal, Simon J Freakley, Rebecca U McVicker, Sultan M Althahban, Nikolaos Dimitratos, Qian He, David J Morgan, Robert L Jenkins, David J Willock, Stuart H Taylor, Christopher J Kiely, Graham J. Hutchings

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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.
Original languageEnglish
Pages (from-to)223-227
Number of pages5
JournalScience
Volume358
Issue number6360
Early online date7 Sep 2017
DOIs
Publication statusPublished - 13 Oct 2017

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