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

نویسندگان

  • 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
چکیده

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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عنوان ژورنال:
  • Science

دوره 358 6360  شماره 

صفحات  -

تاریخ انتشار 2017