Le LPTI/CEA (Laboratoire des Procédés Thermiques Innovants) développe un procédé d’incinération-vitrification de déchets radioactifs. La première étape du dispositif consiste en l’élimination de la charge organique (polymère) par incinération du déchet suspendu dans un four. L’objectif du travail présenté dans ce document est d’étudier les paramètres opératoires susceptibles de modifier la vitesse de dégradation des polymères, pour pouvoir optimiser l’étape d’incinération.Dans cette étude, le taux de dégradation est mesuré par la perte de masse des composés. Une macro-thermobalance permettant de travailler avec des masses de polymère (polyéthylène et néoprène) allant de 5g à 65g a été développée et mise au point afin de mener les études paramétriques (masse d’échantillon, température du four, pourcentage d’oxygène dans le gaz, type de contenant) nécessaires à l’évaluation des vitesses de dégradation du polyéthylène et du néoprène. Ces études seront par la suite étendues à l’évaluation des cinétiques de combustion de systèmes organiques complexes confinés dans différents vecteurs.Parallèlement, deux modèles, l’un décrivant la phase gazeuse par CFD et le polymère par un modèle « 0D » considérant la température homogène dans l’échantillon, et l’autre décrivant les deux phases par CFD (Computational Fluid Dynamic) ont été développés. L’objectif de ces modèles, résolus en mode transitoire, est de calculer la vitesse de dégradation du polyéthylène lors de sa combustion dans la macro-thermobalance afin de décrire le comportement observé expérimentalement.Les résultats expérimentaux et de modélisation montrent l’importance de la position de la flamme et des transferts thermique dans le polymère sur sa vitesse de dégradation. Pour le néoprène dont la dégradation produit du char, il est montré expérimentalement que l’étape d’oxydation du char est, aux températures de l’étude (>600°C), limitée par le transfert d’oxygène dans les résidus solides. / The LPTI / CEA (Innovative Thermal Processes Laboratory) is developing a process for the incineration-vitrification of radioactive waste. The first step consists in the elimination of the organic charge (polymer) by incineration of the waste suspended in an oven. The objective of the work presented in this document is to study the operating parameters likely to modify the rate of degradation of the polymers, in order to optimize the incineration step.In this study, the degradation rate is measured by the mass loss of the compounds. A macro-thermobalance allowing to work with masses of polymer (polyethylene and neoprene) going from 5g to 65g was developed in order to carry out the parametric studies (mass of sample, temperature of the furnace, percentage of oxygen in gas, type of container) needed to evaluate the degradation rates of polyethylene and neoprene. These studies will then be extended to evaluate the kinetics of combustion of complex organic systems confined in different vectors.In parallel, two models were developped. The first describes the gas phase by CFD and the polymer by a "0D" model considering the homogeneous temperature in the sample, and the second is describing the two phases by CFD (Computational Fluid Dynamic). The objective of these models, solved in transient mode, is to calculate the rate of degradation of the polyethylene during its combustion in the macro-thermobalance to describe the behavior observed experimentally.Experimental and modeling results show the importance of flame position and heat transfer in the polymer on its rate of degradation. For the neoprene whose degradation produces carboneous residues (char), it is shown experimentally that the stage of oxidation of the char is, at the study temperatures (> 600 ° C), limited by the transfer of oxygen in the solid residues.

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Porous Wall Hollow Glass Microspheres (PWHGMs) were developed by the Savannah River National Laboratory. What makes these microspheres unique is the interconnected porosity spread throughout their wall allowing various materials to travel from the surface to the hollow interior. With their characteristic porosity, the PWHGMs are a great tool for encapsulating or filtrating different materials. Unfortunately, there is little information available on the mechanical properties of PWHGMs. The main goal of this research was to develop a method to crush individual microspheres and statistically analyze the results. One objective towards completing this goal was to measure the microsphere diameter distribution. Microsphere diameter is a major factor affecting strength as well as the Weibull parameters. Two different methods, microscopy counting and laser light scattering, used in the research yielded similar distributions. The main objective of this research was to analyze the crush strength of individual microspheres. Using nanoindentation, data were collected to analyze the crush strength of PWHGMs in uniaxial compression. Nanoindentation data were used to analyze how the strength of the PWHGMs changes through the different stages of production and at different diameter ranges. Data for 3M commercial microspheres were compared to ARC microspheres. Most data were analyzed using a statistical technique known as the two parameter Weibull analysis. The data indicated that the strength generally decreased as the microsphere diameter increased. Scattering in the data was nearly the same across all sample sets tested. Results indicated that the PWHGMs were weaker than the ARC hollow glass microspheres (HGMs). This is primarily due to the addition of wall porosity in the PWHGM. / Master of Science