Abstract
The oxidation of methane over Pd/Al 2O 3 catalysts in flow systems has been investigated at temperatures in the range 250–600°C and with O 2/CH 4 ratios between 0.5 and 10.0. Oscillatory behaviour in the evolution of heat of reaction was observed for mixtures close to the stoichiometric composition. The frequency of oscillation increased with rising temperature. The amplitude also depended on both temperature and feed gas composition, and was greatest under conditions such that the consumption of oxygen was almost complete. The oscillatory behaviour may be attributed to the periodic or aperiodic changes in a Pd–PdO x active phase, modulated by the specific reaction environment at elevated temperature.
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