A NOx-catalyzed process for the oxidation of methane and ethane to formaldehyde by dioxygen was presented. At 600°C in the presence of a stoichiometric amount of dioxygen (NO: O2 = 2), NOx will catalyze the conversion of both methane and ethane to formaldehyde in relatively good yields. When partial oxidation of methane was carried out at 525°C in an excess of dioxygen, > 2% CH3NO2 was formed. Increasing the temperature to ∼ 600°C prevented CH3NO2 formation. The yield of oxygenates from methane was over 11%. The yield increased to over 16% when 0.7% of ethane was added to the gas mixture. The yield of oxygenates from ethane was over 24%. A catalytic cycle involving NO2 as the C-H activating species was proposed.
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