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Experimental study and mathematical modeling of catalytic partial oxidation of methane to synthesis gas over monolith catalyst at short contact times

Abstract : The main objective of the thesis was to develop a monolith-type structured reactor for the efficient catalytic partial oxidation of methane to synthesis gas. The investigated catalysts comprised Pt as noble or Ni as base metal supported on CeO2-ZrO2 mixed oxides introduced as wall coatings of corundum monolith substrates. It was possible to elucidate the effect of different dopants modifying the mixed oxide on oxygen storage properties 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, like surface and bulk adspecies nature and dynamics, the interaction between Pt and CeO2-ZrO2 playing a key role for catalyst activity. Kinetic experiments demonstrated that Pt is required for reforming reactions and showed a significant reactivity of the doped CeO2-ZrO2 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 later was found significantly higher than that of the support although TAP investigations indicated that a more oxidized catalyst shows higher methane activation rates.
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Submitted on : Tuesday, October 19, 2010 - 12:12:05 PM
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  • HAL Id : tel-00527446, version 1

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Elena Leonidovna Gubanova. Experimental study and mathematical modeling of catalytic partial oxidation of methane to synthesis gas over monolith catalyst at short contact times. Other. Université Claude Bernard - Lyon I, 2008. English. ⟨NNT : 2008LYO10204⟩. ⟨tel-00527446⟩

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