X-ray tomography of feed-to-glass transition of simulated borosilicate waste glasses

The feed composition of a high level nuclear waste (HLW) glass melter affects the overall melting rate by influencing the chemical, thermophysical, and morphological properties of a relatively insulating cold cap layer over the molten phase where the primary feed vitrification reactions occur. Data from X ray computed tomography imaging of melting pellets comprised of a simulated high-aluminum HLW feed heated at a rate of 10°C/min reveal the distribution and morphology of bubbles, collectively known as primary foam, within this layer for various SiO₂/(Li₂CO₃+H₃BO₃+Na₂CO₃) mass fractions at temperatures between 600°C and 1040°C. To track melting dynamics, cross-sections obtained through the central profile of the pellet were digitally segmented into primary foam and a condensed phase. Pellet dimensions were extracted using Photoshop CS6 tools while the DREAM.3D software package was used to calculate pellet profile area, average and maximum bubble areas, and two-dimensional void fraction. The measured linear increase in the pellet area expansion rates – and therefore the increase in batch gas evolution rates – with SiO₂/(Li₂CO₃+H₃BO₃+Na₂CO₃) mass fraction despite an exponential increase in viscosity of the final waste glass at 1050°C and a lower total amount of gas-evolving species suggest that the retention of primary foam with large average bubble size at higher temperatures results from faster reaction kinetics rather than increased viscosity. However, viscosity does affect the initial foam collapse temperature by supporting the growth of larger bubbles. Because the maximum bubble size is limited by the pellet dimensions, larger scale studies are needed to understand primary foam morphology at high temperatures. This temperature-dependent morphological data can be used in future investigations to synthetically generate cold cap structures for use in models of heat transfer within a HLW glass melter.