4.8 Article

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

Journal

SCIENCE
Volume 358, Issue 6360, Pages 223-226

Publisher

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aan6515

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Funding

  1. MAXNET Energy Consortium
  2. NSF Major Research Instrumentation program [MRI/DMR-1040229]
  3. Saudi Arabian government

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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 (O-2) as an oxidant in the presence of hydrogen peroxide (H2O2), we demonstrated that the resulting methanol incorporated a substantial fraction (70%) of gas-phase O-2. 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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