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Immobilisation de déchets magnésiens dans un matériau alcali-activé : étude expérimentale et numérique

Abstract : The operation phase of the first generation of nuclear reactors in France has generated magnesium and graphite long lived low-level wastes (LLW-LL). Their conditioning in a hydraulic binder matrix is being addressed. In order to study the behavior of these packages, several coupled mechanisms have to be considered: the magnesium alloy can corrode within the encapsulating matrix, especially when galvanic coupling with the graphite occurs. The corrosion of the metal results in the development of corrosion products. The growth of corrosion products around the metal and the restriction of the hydraulic binder’s delayed strains may lead to the generation of internal stresses. The verification of certain safety requirements (dimensional stability of the package and low hydrogen production) is therefore essential. It requires the development of a numerical model able to predict the behavior of these packages.In particular, a sodium hydroxide activated blast furnace slag mortar is being addressed. It belongs to the family of alkali-activated materials for which the modelling of ageing behavior is rarely approached. Hence, the construction of the numerical model involves a large experimental campaign covering the thermo-chemo-mechanical behavior of the alkali-activated mortar and the corrosion of magnesium in hydraulic binders. Meso-scale homogenization calculations are undertaken in order to determine upscaled properties of the mix (matrix + wastes) and carry out simulations on the scale of the packages.Regarding the first experimental study axis, a relatively low hydration heat is measured. This is beneficial with respect to the internal stress generated from the self-restriction of the thermal strains within massive structures.Nevertheless, the materials undergoes a particular autogenous shrinkage strains showing an increase even at long term. However, its basic creep strains are shown to be important which could result in stress relaxation and avoids damage related to shrinkage restriction.Regarding the metal’s corrosion behavior in the alkali-activated mortar, it is compared to the one in two different ordinary Portland cement (OPC) based mortars. Microscopic observations are conducted on samples especially designed to monitor the galvanic corrosion of the alloy. They show the aggressiveness in OPC mortars (localized corrosion manifested by holes and layered microstructure) against limited homogeneous corrosion in alkali-activated mortar. Additionnaly, corrosion kinetics are determined using different experimental methods: mass loss and electrochemical measurements. The complementary results of these two types of measurements also show a low corrosion in the alkali-activated slag mortar with a passive state of the metal achived at 6 months of embedment. This advantage of slag mortar is explained by a high electrical resistivity with respect to OPC mortars, determined by electrochemical impedance spectroscopy.Finite element simulations are performed using Cast3m software on meso-scale in order to evaluate the mechanical effect of the corrosion layer development on the surrounding matrix. The corrosion kinetics of the alloy, the nature of corrosion products and their mechanical properties identified using SEM/EDS and nano-indentation techniques are implemented. The calculations indicate low stress generation in the alkali-activated mortar.
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Submitted on : Friday, June 1, 2018 - 1:01:51 AM
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Farah Rifai. Immobilisation de déchets magnésiens dans un matériau alcali-activé : étude expérimentale et numérique. Génie civil. Université Paris-Saclay, 2017. Français. ⟨NNT : 2017SACLN043⟩. ⟨tel-01804651⟩

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