Abstract
The homogeneous gas phase O 2-based oxidation of methane was studied in the temperature range, from 500°C to 750°C at methane partial pressures ranging from 3 bar to 40 bar. At the lower end of the temperature range methanol, formaldehyde, and CO represent the main products, while at temperatures exceeding 650° C/C-coupled products, C 2H 6, C 2H 4, C 3H 6 and C 3H 8 predominate. The change in selectivity as function of the temperature is well explained based on a free radical chain mechanism with degenerate branching, initiated by the gas phase reaction, CH 4+O 2→CH · 3+HO · 2. Bringing in basic catalysts known to catalyze the system at low methane partial pressures, in the reactor e.g. SrCO 3, BaCO 3, and 7% Li/MgO resulted in reduced rates of methane and oxygen conversions, and only minor changes in the selectivity to coupled products were observed.
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