Modelling of long-term diffusion–reaction in a bentonite barrier for radioactive waste confinement

Abstract Bentonites have been proposed as buffer material for barriers in geological disposal facilities for radioactive waste. This material is expected to fill up by swelling the void between the canisters containing the waste and the surrounding ground. However, the bentonite barriers may be submitted to changes of humidity, temperature variation, fluid interaction, mass transport, etc. This could modify the physico-chemical performance of the barrier, mainly on the interface with the steel container and with the geological barrier. The engineered barrier development necessitates thus the study of the physico-chemical stability of its mineral component as a function of time under the conditions of the repository in the long-term. The purpose of the present study was two-fold. Firstly, it was hoped to simulate the chemical transformations (geochemical and cation exchange reactions) coupled with diffusion of chemical-elements into the engineered barrier under repository conditions by applying a thermokinetic hydrochemical code (KIRMAT: Kinetic Reactions and Mass transport). Secondly, it was hoped to apply a simplified method to estimate the swelling capacity evolution by a volume balance in the fluid-saturated engineered barrier, considering that the decay of swelling capacity is directly proportional on the volume of transformed montmorillonite and, taking into account that it may be partially compensated by the volume of neo-formed swelling clays. The system modelled herein was considered to consist of 1-m thick zone of water-saturated engineered barrier. This non-equilibrated system was placed in contact with a geological fluid on one side, which was then allowed to diffuse into the barrier, while the other side was kept in contact with a source of metallic iron. Reducing initial conditions( P O 2 ≅ 0; Eh = − 200 mV) and a constant reaction temperature (100 °C) were considered. The results showed that the EB in contact with the geological fluid was highly transformed after 10,000 years, whereas the most significant chemical processes were illitization, cation exchange and saponization, extending up to 20 cm into the EB. Chemical transformations of minor importance in the EB were identified as well, such as a neo-formation of silicates (quartz, cristobalite), anhydrite, laumontite, magnetite and chlorite in the system. A simplified method based on volume balance showed that the swelling capacity of the bentonite barrier is slightly affected after 10,000 years of diffusion–reaction ( D close to 1) because the volume of neo-formed swelling-clays is almost directly proportional to the volume of transformed Na/Ca-montmorillonite, except for a strong illitization and/or neo-formation of non-swelling clays. In the present study, this simple approach predicted that the decay of swelling capacity of the engineered barrier is drastically affected close to the geological barrier-engineered barrier interface. Out this zone the swelling capacity decay lies between 5% and 11%.