Osmosis-induced swelling of Eurobitum bituminized radioactive waste in constant total stress conditions

Abstract

In geological disposal conditions, contact of Eurobitum bituminized radioactive waste, which contains high amounts of the hygroscopic and highly soluble NaNO 3, with groundwater will result in water uptake and swelling of the waste, and in subsequent leaching of the embedded NaNO 3 and radionuclides. The swelling of and the NaNO 3 leaching from non-radioactive Eurobitum samples, comprised between two stainless steel filters and in contact with 0.1 M KOH, was studied in restricted (semi-confined) swelling conditions, i.e. under a constant total stress, or counterpressure, of 2.2, 3.3, or 4.4 MPa ( i.e. oedometer conditions). Four tests were stopped after hydration times between 800 and 1500 days, and the samples were analyzed by micro-focus X-ray Computer Tomography (μCT) and by Environmental Scanning Electron Microscopy (ESEM). The complete set of data enabled a consistent interpretation of the observations and lead to an improved understanding of the phenomenology of the water uptake, swelling, and NaNO 3 leaching in restricted swelling conditions. Under the studied conditions, the bituminous matrix surrounding the NaNO 3 crystals and pores with NaNO 3 solution behaved as a highly efficient semi-permeable membrane, i.e. osmotic processes occurred. In the main part of the leached layers, a high average NaNO 3 concentration and related to this a high osmotic pressure prevailed, explaining why in the studied range the swelling was not measurably affected by the counterpressure. At the interface with the stainless steel filters, a low permeable re-compressed bitumen layer was formed, contributing to the slow release of NaNO 3 compared to the water uptake rate. A fully coupled Chemo-Hydro-Mechanical (CHM) constitutive model has been developed that integrates the key processes involved and that reproduces satisfactorily the results; this is presented in another work. Combination of the experimental and the modelling study allow to conclude that under semi-confined conditions the swelling of the bituminized waste, and its evolution with time, is the result of several transient processes (salts dissolution, diffusion of salts and water, advection, creep, involving a low permeability material with evolving thickness and properties) that moreover are non-linear and strongly coupled.