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. Titre-en-français, Étude expérimentale et modélisation de l'oxydation partielle du méthane en gaz de synthèse sur réacteur catalytique monolithique à temps court __________________________________________________________________________ RESUME en français

_. Titre, Experimental study and mathematical modeling of catalytic partial oxidation of methane to synthesis gas over monolith catalyst at short contact times ____________________________________________________________________________ RESUME en anglais : Main objective of the thesis was to develop a structured reactor for the efficient catalytic partial oxidation of methane (CPOM) to synthesis gas. The investigated catalysts comprised Pt as noble or Ni as base metal supported on CeO 2 -ZrO 2 mixed oxides introduced as wall coatings of corundum monolith substrates. It was possible to elucidate the effect of different dopants modifying the mixed oxide and to establish the impact of process parameters on the CPOM performance of single monolith channels at short contact times. A mechanistic study revealed important factors, e.g. surface (species) or bulk (storage) effects, in the interaction between the CeO 2 -ZrO 2 mixed oxide and Pt, playing a key role as the most active sites. Kinetic experiments lead to the insight that Pt is required for reforming reactions and showed a significant reactivity of the doped CeO 2 -ZrO 2 support in the oxidative methane activation. A mathematical description of the experimental data was achieved with a model accounting mainly for the activity of Pt. The activity of Pt sites was found significantly higher than that of the support although TAP investigations indicated that a more oxidized catalyst shows lower methane activation rates. ____________________________________________________________________________ DISCIPLINE : Chimie ? Génie des procédés ____________________________________________________________________________ MOTS-CLES : Catalytic partial oxidation of methane, synthesis gas, CeZrO x support, structured catalyst, short contact times, reaction mechanism, kinetic study ____________________________________________________________________________ INTITULE ET ADRESSE DE L'U.F.R. OU DU LABORATOIRE : Institut de Recherche sur la Catalyse et l'Environnement de Lyon