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Expérimentation et modélisation dynamiques de réacteurs catalytiques : vers une meilleure description du processus catalytique

Abstract : Kinetic experiments performed under stationary conditions mainly give information on the rate determining step. Numerous experiments must be done to estimate a limited number of parameters. Unsteady-state experiments, on the other hand, give more detailed information about the kinetics of the different elementary steps with a small number of experiments. In order to work under dynamic conditions, a perturbation of a process variable (concentration, pressure, temperature, etc.) is introduced at the reactor entrance (pulse, step, oscillation ...). This study explores periodic sinusoidal variations of the flow to obtain kinetics for heterogeneous catalytic processes. The kinetic information is contained in the phase lag and the gain change of the oscillations. The oscillations can be kept small and can be performed around steady-state operation, thus studying the kinetics under relevant conditions. First a model able to directly estimate the gain and phase lag has been created. Secondly, simple cases of adsorption have been performed in order to validate the model and to test the experimental set up. To finish, the approach has been applied to the selective hydrogenation of acetylene. Kinetic modeling was carried out in both stationary and dynamic conditions in order to compared the two methodologies
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Caroline Urmès. Expérimentation et modélisation dynamiques de réacteurs catalytiques : vers une meilleure description du processus catalytique. Génie chimique. Université de Lyon, 2018. Français. ⟨NNT : 2018LYSE1226⟩. ⟨tel-02342597⟩

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