Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O-2 under mild conditions

作者：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.^*

来源：Science, 2017, 358(6360): 223-226.

DOI：10.1126/science.aan6515

• LOW-TEMPERATURE OXIDATION
• HYDROGEN-PEROXIDE
• ALLOY NANOPARTICLES
• SOL IMMOBILIZATION
• METHANE
• CONVERSION
• ALKANES
• SURFACE
• ETHANE
• SYSTEM

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.

• 出版日期2017-10-13