Evaluation of the First order Kinetic Approximation in Heterogeneous Catalysis*
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概要
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The validity of first order kinetic approximation in heterogeneous catalysis has been evaluated by using the transient response method. As an example of a solid catalysed reaction, the oxidation of carbon monoxide has been studied on four different metal oxides MnO_2, Cr_2O_3, Pb_3O_4, and ZnO. The steady stale rate analysis apparently met first order kinetics with respect to the concentration of CO for all the catalysts. The Arrhenius plots of the apparent first order rate constant obtained clearly gave a good straight line and estimated the apparent activation energy of the reactions on each catalyst. A simple first order kinetic model due to surface reaction controlling is proposed to explain the transient state and the steady stale of reaction. Based on the models proposed, the transient response curves of carbon dioxide caused by the stepwise change in the concentration are simulated by using personal computers The results exhibit a large deviation of the calculated curves from the experimental ones especially at the transient state whereas the steady state values of both are in good agreement. Four different dual path models have separately been proposed for each of the four catalysts. The models consistently explain the characteristic mode of the transient response curves obtained for each catalyst and under wide experimental conditions. The activation energy of the slowest elementary step is evaluated for all the catalysts, and some of the values deviate largely from those estimated from the apparent first order kinetic models.
- 北見工業大学の論文
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