Integrated testing of the SRL-165 glass waste form

Integrated testing of the important components of a glass waste form waste package has been performed in order to gain a better understanding of the processes of radionuclide release and transport in the near field environment. Based upon an interpretation of the depth of penetration of hydrogen in reacted SRL-165 glass we have modeled the radionuclide release from the glass as a combined process of (1) the diffusive exchange of alkalis and boron in the glass for hydrogen species in the solution (D = 10-16 cm2/s) and (2) surface dissolution. Surface dissolution controls the release of components not exchanged by diffusion and takes place at a rate of 1.5 to 3.0 μm/yr. Subsequent to release the radionuclides may remain in the leach solution, diffuse into the tuff, or precipitate as secondary phases. Precipitation is particularly important for plutonium and americium. Diffusive transport of radionuclides through the tuff takes place at an extremely slow rate, D = 10-16 cm2/s. As such, the mass of radionuclides incorporated in the tuff by diffusion during the tests is inconsequential relative to that in the leach solution (with the exception of plutonium) and can be ignored in mass balance calculations. Mass balance calculations based upon the release of radionuclides by surface dissolution of the glass waste form are in good agreement with observed solution chemistry when allowances are made for a pulse of dissolution early in the tests. This pulse may be due to either the rapid dissolution of high-energy surface features early in the integrated tests, or an initially high surface dissolution rate that decreases with time as silica saturation is approached, or a combination of the two