Alteration of French waste glass matrix of R7T7 type in deep geological disposal conditions

The Geological disposal is a possible option for safe and long term management of long lived and highly radioactive wastes. In order to predict the release of radionuclides in the environment, the comprehensive knowledge of glass dissolution rates as well as the properties of near- and far-field in which migration will occur is necessary. This thesis is aimed to describe the alteration of SON68 glass, inactive analog of French R7T7 glass, in contact with disposal materials: metallic iron and Callovo-Oxfordian argilite. Therefore, original experiments have been carried out on a laboratory scaled system involving 'glass-iron-argilite' interactions. The transformations of chemistry and crystal-chemistry are investigated with multi-scale probing tools: SEM, TEM, XRD, XRF, EXAFS and Raman spectroscopies. In the same time, the glass alteration is modeled to obtain a source term in good agreement with the major phenomena observed in common experiments. As an end, geochemical models of iron and argilite transformations are also developed and set together in the transport-chemistry code HYTEC to simulate chemical reactions (iron corrosion, argilite evolution, and glass alteration). Simulations and comparison with experiments have improved the overall knowledge of the glass-iron-clay system. (author)