Underwater behaviour of bitumen coated radioactive wastes: experimental validation of the Colonbo degradation model

In the release scenario considered for geologic repository, water is thought to be the main aggressive agent with regards to bituminized radioactive waste (composed in general of 60 weight % of bitumen, 40% of soluble/insoluble salts and a few ppm of radionuclides). Since liquid water can diffuse in pure bitumen, leaching of bituminized waste results in the dissolution of the most soluble salts and leads to the development of a more or less concentrated saline solution-filled pore structure (called permeable layer). In consequence of the generation of a porous layer in the bituminized waste, leaching of salts and radionuclides can then take place. Research performed at the Atomic Energy Commission (CEA) aims therefore at understanding the consequences of ground-water immersion on the transport properties and radionuclides leaching of bituminized waste materials. To this end, a constitutive model (called COLONBO) which describes mathematically the leaching of bituminized waste has been developed. The COLONBO model is based on the following assumptions: 1. Water and dissolved salts migrate in the permeable layer according to Fick's first law. The diffusion of water and salts are quantified by effective diffusion coefficients which are unknown. 2. The mechanical properties of the bitumen matrix are not considered during leaching (free swelling). Up to now, the COLONBO model has been used only to model experimental water uptake and salt leach curves, leading (theoretical) estimates of the effective diffusion coefficients of water and salts in the permeable layer. The aim of this work was to validate experimentally the numerical results obtained with the COLONBO model. First, the correspondence between experimental and simulated water uptake and salt leach rates obtained on various bituminized waste materials is checked, leading estimates of the effective diffusion coefficients of water and salts in the permeable layer. Second, the evolution of the thickness and of the morphology of the permeable layer of partially leached bituminized waste samples is studied. The porosity and the pore distribution in the permeable layer are quantified according to a semi-automatic method based on the analysis of Environmental Scanning Electron Microscope images. The obtained experimental porosity profiles are compared successfully to those resulting from simulations performed with the COLONBO model. The effective diffusion coefficients of water and salts in the permeable layer of leached bituminized waste samples are then directly measured by through diffusion experiments. In the experiments, the flow of radioactive tracers (water and salts) through thin membranes of partially leached bituminized waste is followed in time. Due to the evolution of the bitumen specimen during the tests (continuous leaching), a specific method of analysis had to be developed to obtain reliable effective diffusion coefficients. The results show that the diffusion coefficients of water and salts increase with the porosity of the permeable layer, as expected from the COLONBO model. Overall, the direct characterization of the transport properties of the permeable layer and of the pore distribution in the permeable layer validate quantitatively the results obtained with the COLONBO model and the underlying hypotheses. Finally, constitutive models describing the leaching of elements from polymer matrices immersed in water have been applied to bituminized waste materials. With respect to COLONBO, these models account for the effect of mechanical properties of polymers on swelling and leach rates. (author)