Prediction of Radioactive Waste Glass Durability by the Hydration Thermodynamic Model: Application to Saturated Repository Environments

Abstract

ABSTRACTThe effects of groundwater chemistry on glass durability were examined using the hydration thermodynamic model. The relative durabilities of SiO2, obsidian, basalt, nuclear waste glasses, medieval window glasses, and a frit glass were determined in tuffaceous (J–13) groundwater, basaltic (GR–4) groundwater, WIPP–A brine, and Permian Basin brine (PBB–3) using the monolithic MCC–I durability test. In the groundwater–dominated MCC–l experiments, the interaction of the glasses and the initial groundwater (leachant) caused the formation of unique assemblages of secondary phases. The secondary phase formation, in turn, controlled the final groundwater (leachate) pH and ionic strength, I[t].Correlations of the final leachate pH and I[t] with the Si release from the glass indicated that it is the influence of the secondary phase formation on the leachate pH and I[t] that controls the final dissolution rate of the glass. Since I[t] and the pH of the leachates are functions of the precipitation reactions, inclusion of the experimentally determined solution pH in the free energy of hydration model provides for the functional dependence of the dissolution rate on the secondary precipitation. Therefore, superposition of the linear equation for the groundwater and deionized water experiments occurs and the hydration free energy model can be used to compare glass durability in deionized water and in repository groundwaters.