Abstract
A mathematical model was used to predict radionuclide release from bitumen and glass waste forms over extended time periods. To calculate some model parameters, we used experimental data derived from 12yr field tests with six borosilicate waste glass blocks (each ∼30 kg in weight) and a bitumen block (310 kg), containing real intermediate-level NPP operational waste (NaNO3, 86 wt.% of a dry salt content; 137Cs, 82% of the radioactive inventory). Specific radioactivities of the glass material containing 35 wt.% waste oxides were βtot(90Sr+90Y), 3.74×106 Bq/kg, and αtot(239Pu), 1.3×104Bq/kg. The bitumen block with ∼31 wt.% salt content and βtot(90Sr+90Y), 4.0·106 Bq/kg, and αtot(239Pu), 3.0×103 Bq/kg was manufactured on base of a hard bitumen BN-IV. Tests with the waste forms were performed under saturated conditions of an experimental near-surface repository with a free access of groundwater to the waste blocks through a covering of host loamy soil and backfill of coarse sand. The way used to quantify the amount of leached radioactivity was to measure the volume and radioactivity concentrations of contacting groundwater.
In the model, radionuclide release from the waste glass is assumed to be controlled by the processes of diffusion limited ion exchange and glass network dissolution. The mechanism of radionuclide release from the bitumen matrix is believed to remain the same throughout the long-term storage period, except for the initial stage when an enhanced leaching from the surface layer occurs. This long-term release is assumed to be controlled by diffusion of radionuclides through the bitumen matrix. So, identical formulae were applied to calculate the values of leached radioactivity fractions for two waste forms.
Radioactivity release curves were plotted for field data and calculation results. For both waste forms, there was good agreement between the modelled and available experimental data. According to the modelling results, fmax = 2.3×10−3% of the initial radioactivity will release from the waste glass into the environment within a proposed institutional control period of 300 years under conditions of the near-surface repository and in the absence of additional engineered barriers. For the bitumen block and the same 300-yr period, the total (maximum) leached radioactivity fraction will be fmax = 4.2×10−3%.
The main result of the modelling and experimental studies concerning the leaching behaviour of the bituminised and vitrified waste materials is that the fractional radioactivity release for two waste forms is on the same order of magnitude. Numerical release values per a unit of a surface area to volume ratio are also rather close for two waste forms (exposed surface area to volume ratio for the bitumen block is 2 to 4 times greater then for the glass).
A mechanistic model for long-term nuclear waste glass dissolution integrating chemical affinity and interfacial diffusion barrier