Recent work by the authors has demonstrated that cesium was being incorporated in a hydrated phase as their cement-based waste forms cured. The objective of the present study was to identify the hydrated phases responsible for the observed cesium incorporation. Four calcium aluminosilicate glasses having a 1:2 Al2 O3 /CaO ratio and a 25–70 mole % silica content were mixed with ˜0.3 molar CsOH or CsCl solutions (water/solid ratio = 10) and allowed to hydrate at 38° and 90°C for periods up to 90 days. Paste equivalent samples, having a water/solid ratio of 1.0 were also prepared to gauge the cementing properties of these mixtures. Solutions were analyzed for Ca, Al, Si, and Cs while solids were characterized using x-ray powder diffraction and scanning electron microscopy.
Glasses exposed to the CsOH solution were more reactive than their counterparts exposed to the CsCl solution. In addition, reactivity as well as crystallinity seemed to be higher at 90° than at 38°C. At least two cesium-containing zeolites were identified in the 90°C CsOH solution experiment: A cesium-containing wairarkite analogue and possibly another cesium-containing zeolite unidentified at this time. The relatively complete removal of cesium from the solution, in one case, as well as the fact that the mixtures are self-cementing suggests that the glasses may be “engineered” to serve as overpack material in a deep-seated geologic repository.