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

doi:10.1126/science.aan6515

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

Department of Chemistry

Research output: Contribution to journal › Article

147 Citations (Scopus)

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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 language	English
Pages (from-to)	223-227
Number of pages	5
Journal	Science
Volume	358
Issue number	6360
Early online date	7 Sep 2017
DOIs	https://doi.org/10.1126/science.aan6515
Publication status	Published - 13 Oct 2017

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Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions
This is the author's version of the work. It is posted here by permission of the AAAS for personal use, not for re-distribution. The definitive version was published in Science on 13th October 2017 Volume 358, issue 6360, DOI:10.1126/science.aan6515
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Simon Freakley
- S.Freakley@bath.ac.uk
- Department of Chemistry - Lecturer
- Centre for Sustainable and Circular Technologies (CSCT)
Person: Research & Teaching, Researcher

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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; Hutchings, Graham J.

In: Science, Vol. 358, No. 6360, 13.10.2017, p. 223-227.

Research output: Contribution to journal › Article

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 ; Hutchings, Graham J. / Aqueous Au-Pd colloids catalyze selective CH₄ oxidation to CH₃OH with O₂ under mild conditions. In: Science. 2017 ; Vol. 358, No. 6360. pp. 223-227.

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

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.",

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AU - Dimitratos, Nikolaos

AU - He, Qian

AU - Morgan, David J

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AU - Kiely, Christopher J

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AB - 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.

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

Abstract

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Simon Freakley

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