The Direct Partial Oxidation of Methane to Dimethyl Ether over Pt/Y₂ O₃ Catalysts Using an NO/O₂ Shuttle

Using a mixture of NO + O₂ as the oxidant enabled the direct selective oxidation of methane to dimethyl ether (DME) over Pt/Y₂ O₃ . The reaction was carried out in a fixed bed reactor at 0.1 MPa over a temperature range of 275-375 °C. During the activity tests, the only carbon-containing products were DME and CO₂ . The DME productivity (μmol g_cat ^-1  h^-1 ) was comparable to oxygenate productivities reported in the literature for strong oxidants (N₂ O, H₂ O₂ , O₃ ). The NO + O₂ mixture formed NO₂ , which acted as the oxygen atom carrier for the ultimate oxidant O₂ . During the methane partial oxidation reaction, NO and NO₂ were not reduced to N₂ . In situ FTIR showed the formation of surface nitrate species, which are considered to be key intermediate species for the selective oxidation.