Glass-ceramics were developed initially for the immobilization of miscellaneous Pu-residues at the UK’s Sellafield site from which it was uneconomic to recover Pu for reuse. Renewed interest in the immobilization of a portion of the UK PuO2 stockpile has led to glass-ceramics being evaluated for bulk Pu immobilization. The Nuclear Decommissioning Authority (NDA) in the UK have proposed hot isostatic pressing (HIP) as a potential consolidation technique for the processing of these wasteforms. In this study, zirconolite based glass-ceramics were investigated to determine an optimum formulation. The yield of zirconolite is shown to vary with glass composition and glass fraction, such that a higher Al content favours zirconolite formation. The sample preparation process is discussed to highlight the importance of a high temperature heat-treatment during sample preparation to achieve high quality HIPed wasteforms.

The liquidus temperature (TL) of rare earth (RE) was determined for alumino-borosilicate glasses for treating americium and curium that have been studied previously. Their work covers a wide range of glass composition with various crystalline phases as primary phase. Present work is aimed at understanding the effect of glass composition on TL for waste glasses designed for vitrifying RE oxides wastes. In a sufficiently narrow composition region, this effect can be represented by a first-order model fitted measured TL versus composition data. Test glasses were formulated by varying of component fractions one-at-a-time. The glasses contained SiO2, B2O3, and Al2O3 as glass formers and Nd2O3 with CeO2 as simulated RE waste. Twenty glasses were made to investigate crystallization as a function of temperature and glass composition. The primary crystalline phase was Ce-borosilicate (Ce3BSi2O10), secondary phases were Al-containing crystals (Al2O3 and Al10Si2O19), and crystalline CeO2. A first-order model was fitted to crystal fraction versus glass composition data. Generally, SiO2 and B2O3 tend to suppress crystallization, Al2O3 has little effect, and, as expected, RE components (Nd2O3 and CeO2) promote it. The correlation coefficient, R2, was 0.89 for the primary crystalline phase TL as a linear function of composition.

NUMO and JAEA have been conducting a joint research since FY2011, which is aimed to enhance the methodology of repository design and performance assessment in preliminary investigation stage for the deep geological disposal of high-level radioactive waste. As a part of this joint research, we have been developing glass dissolution models which include various processes derived from glass-overpack-bentonite buffer interaction, considering the precipitation of Fe-silicates associated with steel overpack corrosion, and Si transport through altered layer of glass. The objective of this modeling work is to show comprehensively the lifetime of the vitrified waste due to glass matrix dissolution timescales through sensitivity analysis, and to identify the feature/process that most strongly influences the lifetime, and to identify future R&D issues that would help to improve the nuclide transport analysis with confidential value and the safety case in future. The sensitivity analysis suggested that the duration of the glass dissolution might be predicted in the ranges from 3.8×103 to 1.9×105 years. Also, the results indicated that the precipitation of Fe–silicate has the strongest influence on the long-team behavior of vitrified waste.

Water degradation of glass waste forms has been studied extensively under a variety of conditions including of bulk glass immersed completely in static or dynamic water. In practice, the vitrified nuclear waste cracks as soon as poured into a container because of differences in thermal expansion coefficients. In addition, in repository the canisters may be only partially immersed in water. Later, water condenses on the surface of glass which corrodes releasing ions. In this work experiments have been performed to understand these effects on the degradation of International Simple Glass (ISG). Simulated cracks were found to develop pitting corrosion in the crack openings when tested by immersing ISG in water. Under load, these pits concentrated stress and grew as large planar cracks inside the glass. The condensation of water on glass surfaces leads to formation of pits and growth of calcium silicate crystals.