Migration Behavior of Multivalent Radionuclides From Fully Radioactive Waste Glass in Compacted Sodium Bentonite

Abstract

AbstractIn a repository of high-level radioactive waste, radionuclides will leach from the waste glass and migrate into the surrounding bentonite after very long time. These processes occur simultaneously in the bentonite and should be evaluated to confirm the reliability of individual models and data for the performance assessment of high-level radioactive waste repository.Previous study [1] reported the results of the in-diffusion experiments of Cs in compacted sodium bentonite (Kunigel V1®) in contact with fully radioactive waste glass for 15 to 300 days under aerobic conditions. And Cs migration was successfully interpreted using fundamental one dimensional diffusion model. However, migration of other radionuclides in fully radioactive waste glass were extremely slow because of low solubility, low effective diffusivity and high distribution ratio, especially multivalent elements of actinide and lanthanide.In this study, the similar in-diffusion experiment reported by Ashida et al. [1] was carried out for about 15 years to evaluate the migration behavior of multivalent actinide and lanthanide elements. The bentonite was compacted into a stainless steel cell with 20 mm in diameter and 18 mm in length to produce dry densities of 0.5 and 1.0 Mg m-3saturated distilled water. The form of fully radioactive waste glass was borosilicate glass by using vitrified in CPF (Chemical Processing Facility). The glass sample was sliced into the disc with 4 mm in thickness and sandwiched by two pieces of the saturated bentonite sample in the diffusion cell under aerobic conditions. After 15 years, bentonite sample was sliced and immersed into the HNO3 to extract the radionuclides from the bentonite. Then profiles of Cs, Eu, Pu, Am and Cm in the bentonite sample were evaluated. The concentration profile of Cs in the bentonite was constant due to its high diffusivity.The experimental concentrations of Am, Cm and Eu in contact with compacted sodium bentonite were good agreement with the solubilities calculated by thermodynamic data. On the other hand, the profiles of Am and Cm show two parts with different slopes which cannot be fitted by simple one-dimensional diffusion model considering single specie. Leaching and migration behavior of radio nuclides will be discussed based on the one-dimensional diffusion model considering other mechanism of several species.[1] T. Ashida, et al. Migration behavior of cesium released from fully radioactive waste glass in compacted sodium bentonite. PNC Technical Report, TN8410 98-014(1998).