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• W2970088930 abstract "High concentrations of Na2O and Al2O3 in the liquid high-level radioactive waste (HLW) stored at the Hanford Site can cause nepheline (NaAlSiO4) to precipitate in a vitrified monolithic waste form upon cooling. Nepheline phase formation removes glass- former SiO2 and -modifier Al2O3 from the immobilization matrix in greater proportion to alkalis, which can reduce glass durability and consequently increase the leach rate of radionuclides into the surrounding environment. Current uncertainty in defining the HLW glass composition region prone to precipitating nepheline necessitates targeting a conservative waste loading, which raises operational costs by extending the liquid radioactive waste disposal mission and increases the required permanent repository storage capacity. An accurate thermochemical representation of HLW glass compositions is necessary to obtain a comprehensive understanding of the composition-temperature space for nepheline formation, which can facilitate the development of a phase field model of the mesoscale microstructural evolution of nepheline crystallization in HLW glass. As such an understanding of nepheline nucleation and grain growth kinetic behavior may lead to significant improvements in the production efficiency of durable HLW glass, generating thermochemical descriptions of the constituent phases is of primary importance. Thus, a database consisting of the oxides of the nepheline-forming Na2O-Al2O3- SiO2 system and HLW glass nepheline solutes B2O3, K2O, CaO, Li2O, MgO, Fe2O3, and FeO has been developed to yield a thermochemical model capable of characterizing nepheline precipitation in HLW glass at equilibrium. Due to their high molar concentrations within vitrified glass, Na2O, Al2O3, B2O3, and SiO2 were considered major oxides whereas more dilute B2O3, K2O, CaO, Li2O, MgO, Fe2O3, and FeO were treated as minor constituents. All pseudo-binary systems composed of the major as well as major- minor oxide systems were thermodynamically assessed according to the CALculation of PHAse Diagrams (CALPHAD) methodology. Additionally, all pseudo-ternary systems consisting of the major oxides were assessed due to the increased probability of interactions between these higher concentration oxides. Gibbs energies of solid solution phases and the oxide liquid were modeled using the compound energy formalism (CEF) and two- sublattice partially ionic liquid (TSPIL) model, respectively. Accuracy of the thermodynamic database was validated by comparing model calculations to HLW glass experimental data. Both annealed and canister centerline cooled (CCC) glass sample data were considered. Additionally, nepheline phase compositional data was included for comparison with database computations. Results of these comparisons indicate that the database-derived calculations agree well with HLW glass experimental data. As phase precipitation in a CCC glass sample is dependent on kinetics, however, a phase field or similar model will need to be utilized to obtain a non-equilibrium description…" @default.
• W2970088930 created "2019-09-05" @default.
• W2970088930 creator A5050180660 @default.
• W2970088930 date "2019-01-01" @default.
• W2970088930 modified "2023-09-26" @default.
• W2970088930 title "Modeling Complex Oxides: Thermochemical Behavior of Nepheline-Forming Na-Al-Si-B-K-Li-Ca-Mg-Fe-O and Hollandite-Forming Ba-Cs-Ti-Cr-Al-Fe- Ga-O Systems" @default.
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