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Etude du phénomène de l'expansion sulfatique dans les bétons : comportement des enrobés de déchets radioactifs sulfatés

Abstract : Sulphate attack is one of the major degradation processes of concrete. It is especially important in storing cemented radioactive wastes containing sulphate. In this thesis, we have thoroughly investigated the degradation mechanisms of cemented radioactive wastes by sulphate. The CaO-Al2O3-SO3-H2O systems with and without alkalis are studied. For the system without alkalis, experimental results show that it is the formation of a secondary ettringite under external water supply by steric effect that causes the expansion. For the system with alkalis, the ettringite doesn't appear while a new mineral called "U", a sodium-substituted AFm phase is detected. This phase is shown to be responsible for the expansion and destruction of the specimens. The conditions for the formation, the product of solubility and many means of its synthesis are discussed, and a complete list of the inter-reticular distances file is given. The behaviour of the different types of cemented wastes containing sulphate are then studied with a special focus on the U phase on entity which was heretofore very little understood. The following three hypothetical mechanisms of sulphate expansion are proposed: the formation of the secondary U phase, the transformation of the U phase to the ettringite and the topochemical hydration of thenardite into mirabilite. Experiments on a simplified system have demonstrated clearly that the formation of the secondary U phase can induce enormous expansion by steric effect, this justifying the first assumption. Simulation by the mass and volume balances is carried out thereafter and enables us to estimate the expansion induced by the formation of the secondary U phase in the cemented wastes. The second assumption is also well verified by a series of leaching tests in different solutions on mixtures containing the U phase. On the basis of the analysis of the specimens under leaching, it has been assumed that the expansion is associated with the interparticulate electric repulsion of colloidal ettringite formed from the transformation of the phase U and in presence of the lime. The kinetics of the transformation process is analysed based upon the diffusion theory. The transformation from thenardite to mirabilite is not justified. In summary, the U phase can induce expansion mainly through two mechanisms which act individually or simultaneously: the formation of the secondary phase U and the transformation of the phase U to ettringite. This work constitutes the first step necessary for predicting the service life of the structures storing the cemented radioactive wastes.
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Guanshu Li. Etude du phénomène de l'expansion sulfatique dans les bétons : comportement des enrobés de déchets radioactifs sulfatés. Mécanique [physics.med-ph]. Ecole Nationale des Ponts et Chaussées, 1994. Français. ⟨tel-00523043⟩

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