Annual progress report to Battelle Pacific Northwest National Laboratories on prediction of phase separation of simulated nuclear waste glasses

The objective of this research is to predict the immiscibility boundaries of multi-component borosilicate glasses, on which many nuclear waste glass compositions are based. The method used is similar to the prediction method of immiscibility boundaries of multi-component silicate glass systems successfully made earlier and is based upon the superposition of immiscibility boundaries of simple systems using an appropriate parameter. This method is possible because many immiscibility boundaries have similar shapes and can be scaled by a parameter. In the alkali and alkaline earth binary silicate systems, for example, the critical temperature and compositions were scaled using the Debye-Hueckel theory. In the present study on borosilicate systems, first, immiscibility boundaries of various binary alkali and alkaline borate glass systems (e.g. BaO-B2O3) were examined and their critical temperatures were evaluated in terms of Debye-Hueckel theory. The mixing effects of two alkali and alkaline-earth borate systems on the critical temperature were also explored. Next immiscibility boundaries of ternary borosilicate glasses (e.g. Na2O-SiO2-B2O3, K2O-SiO2-B2O3, Rb2O-SiO2-B2O3, and Cs2O-SiO2-B2O3) were examined. Their mixing effects are currently under investigation