Étude phénoménologique et modélisation des mécanismes d'oxydation et d'adsorption d'impuretés gazeuses en hélium : application à l'optimisation du système de purification d'un réacteur à caloporteur gaz

Abstract : In GEN IV studies on future fission nuclear reactors, two concepts using helium as a coolant have been selected: GFR and VHTR. Among radioactive impurities and dusts, helium can contain H2, CO, CH4, CO2, H2O, O2, as well as nitrogenous species. To optimize the reactor functioning and lifespan, it is necessary to control the coolant chemical composition using a dedicated purification system. A pilot designed at the CEA allows studying this purification system. Its design includes three unit operations: H2 and CO oxidation on CuO, then two adsorption steps. This study aims at providing a detailed analysis of the first and second purification steps, which have both been widely studied experimentally at laboratory scale. A first modelling based on a macroscopic approach was developed to represent the behaviour of the reactor and has shown that the CuO fixed bed conversion is dependent on the chemistry (mass transfer is not an issue) and is complete. The results of the structural analysis of the solids allow considering the CuO as particles made of 200 nm diameter grains. Hence, a new model at grain scale is proposed. It is highlighted that the kinetic constants from these two models are related with a scale factor which depends on geometry. A competition between carbon monoxide and hydrogen oxidation has been shown. Activation energies are around 30 kJ.mol-1. Simulation of the simultaneous oxidations leads to consider CO preferential adsorption. A similar methodology has been applied for CO2 and H2O adsorption. The experimental isotherms showed a Langmuir type adsorption. Using this model, experimental and theoretical results agree
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Fanny Legros. Étude phénoménologique et modélisation des mécanismes d'oxydation et d'adsorption d'impuretés gazeuses en hélium : application à l'optimisation du système de purification d'un réacteur à caloporteur gaz. Autre. Institut National Polytechnique de Lorraine, 2008. Français. ⟨NNT : 2008INPL106N⟩. ⟨tel-01753014⟩

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