Helium behaviour in nuclear glasses

The present thesis focuses on the study of helium behavior in R7T7 nuclear waste glass. Helium is generated by the minor actinides alpha decays incorporated in the glass matrix. Therefore, four types of materials were used in this work. These are non radioactive R7T7 glasses saturated with helium under pressure, glasses implanted with 3He+ ions, glasses doped with curium and glasses irradiated in nuclear reactor. The study of helium solubility in saturated R7T7 glass has shown that helium atoms are inserted in the glass free volume. The results yielded a solubility of about 1016 at. cm-3 atm.-1. The incorporation limit of helium in this type of glass has been determined; its value amounted to about 2*1021 at. cm-3, corresponding to 2.5 at.%. Diffusion studies have shown that the helium migration is controlled by the single population dissolved in the glass free volume. An ideal diffusion model was used to simulate the helium release data which allowed to determine diffusion coefficients obeying to the following Arrhenius law: D = D0exp(-Ea/kBT), where D0 = 2.2*10-2 and 5.4*10-3 cm2 s-1 and Ea = 0.61 eV for the helium saturated and the curium doped glass respectively. These results reflect a thermally activated diffusion mechanism which seems to be not influenced by the glass radiation damage and helium concentrations studied in the present work (up to 8*1019 at. g-1, corresponding to 0.1 at.%). Characterizations of the macroscopic, structural and microstructural properties of glasses irradiated in nuclear reactor did not reveal any impact associated with the presence of helium at high concentrations. The observed modifications i.e. a swelling of 0.7 %, a decrease in hardness by 38 %, an increase between 8 and 34 % of the fracture toughness and a stabilization of the glass structure under irradiation, were attributed to the glass nuclear damage induced by the irradiation in reactor. Characterizations by SEM and TEM of R7T7 glasses implanted with helium at high concentrations, doped with curium and irradiated in nuclear reactor showed a homogeneous microstructure free of helium bubbles, pores or cracking. The results of the present work were used to develop a long-term diffusion model of helium in an industrial R7T7 nuclear waste glass. The model considers the thermal history, the fracturing and the alpha activity of the glass. (author)