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.

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. - ISSN 0036-8075. - STAMPA. - 358:6360(2017), pp. 223-227. [10.1126/science.aan6515]

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

Dimitratos, Nikolaos;
2017

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.
2017
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. - ISSN 0036-8075. - STAMPA. - 358:6360(2017), pp. 223-227. [10.1126/science.aan6515]
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.*
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11585/666500
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