Transient Behavior of Methane Oxidation over Pt/SiO_2

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The transient behavior of methane oxidation over Pt/SiO_2 with wide exposing dispersion such as Dh＝7, 16, 27, 40 and 81％ was studied by using the transient response method at the temperature range 250〜335℃. For the five catalysts used a common rate equation was derived : γ=(4.2×10^<－3>〜2.5×10^<－2>)exp(-80〜－89/RT)P_<CH_4>^<0.49-0.96>P0^0_<0_2> The turnover frequency of the reaction was steeply reduced with increasing Dh suggesting a structure sensitive reaction. The mode of the transient response curves of CO_2 formed caused by the concentration change in methane at the inlet of the reactor was sensitively changed by the value of Dh, and they were characterized by two modes, either an instantaneous or overshoot types. To explain the drastic change in the mode, the reaction mechanism shifting the rate controlling steps from the surface reaction to the oxidation of the intermediates formed is proposed.
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