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At least 37 records · Page 2

Durability testing of actual Hanford waste glasses and their non-radioactive simulant glasses

The low-activity waste (LAW) fraction of Hanford tank waste will be converted to glass at the Waste Treatment and Immobilization Plant (WTP) and disposed on the Hanford site. The chemical durability of LAW glasses has been researched for decades to satisfy contract requirements. Most LAW glass durability data has been generated on non-radioactive simulant glasses fabricated via crucible melts. These non-radioactive glasses were chosen due to safety and cost reasons with confidence that radioactive waste glasses would exhibit similar behavior. To reduce the risk of significant differences in laboratory test response data between WTP melter waste glass and simulant glass, Product Consistency Tests (PCT, i.e., ASTM C1285-21) and Environmental Protection Agency (EPA) 1313 durability tests were performed on actual and simulant LAW glasses fabricated using laboratory-scaled melters. Actual and simulant glass durability test results are presented and statistically compared. Finally, differences in test responses were found to be within experimental uncertainty.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Glass Design Using Machine Learning Property Models with Prediction Uncertainties: Nuclear Waste Glass Formulation

The United States Department of Energy is responsible for managing the legacy nuclear waste stored in underground tanks at the Hanford Site. The waste will be separately vitrified as low-activity waste and high-level waste fractions. Waste glass formulation algorithms have been traditionally developed using partial quadratic mixture property-composition models. Recently, machine learning (ML) techniques have been used to predict glass properties and discover new glass materials for nuclear waste vitrification, and these advancements can be utilized to improve waste glass composition design. In this proof-of-principle study, ML algorithms such as Gaussian process regression (GPR) were used to interpolate glass properties (e.g., viscosity, electrical conductivity, chemical durability). After selecting appropriate sets of GPR hyper-parameters for each property, an optimization program was developed to formulate glass compositions to maximize waste loading while simultaneously satisfying property within constraints. The results of the ML-based waste loadings and glass compositions were compared to those obtained using the traditional methods. Comparing to the previous glass design framework, the ML-based optimization methods offer improved glass designs and a streamlined approach to generation of optimally designed data and near real-time updates.

glass formulation, machine learning, constraints, ↗

Origin of the Apollo 15 very low Ti green glass. A perspective from the compositional diversity in the very low Ti glasses

The very low Ti green glasses from the Apollo 15 site have intrigued scientists for over 20 years. Their primitive composition has been used to understand magmatic processes and the structure of the moon. The compositional variability observed in the Apollo 15 glass population has long been a point of debate. Initial studies did not recognize the compositional diversity in the glasses. Stolper et al. documented the major element variability and concluded it could not be produced by magmatic processes and therefore concluded that these glasses must be of impact origin. Subsequent studies confirmed a volcanic origin for the glass population and attempted to elucidate magmatic processes to account for its compositional variability. Models that have been proposed for these glasses include the following: (1) the crystallization of single or multiple phases (olivine, pyroxene, Fe metal, immiscible sulfide); (2) the incompatible behavior of Ni and Co during multiple phase crystallization at extremely low fO2; and (3) magma or source mixing. All of these models have problems. Type (1) models appear not to be consistent with recent trace element studies on the glasses; model (2) is dependent on the debatable incompatible behavior of Ni and Co, and, in models of type (3), the origin and nature of mixing models are somewhat unconstrained. This study compares the Apollo 15 green glasses with the very low Ti picritic glasses from other landing sites.

Shearer, C. K.↗

Effect of zeolite type, temperature, and pH on Stage III glass alteration behavior for two nuclear waste glasses

We report long-term laboratory scale static alteration tests (up to 1500 d) were conducted on two low-activity waste glasses (LAWA44 and IDF18-A161) at S/V = 2000 m –1 . Tests were seeded with either analcime, clinoptilolite, zeolite P1, or zeolite P2 to induce Stage III glass alteration behavior. The effect of several parameters on glass Stage III behavior was studied with consideration of several variables, including temperature (22 °C – 90 °C) and pH (floating or initially set using KOH at values from 9.5 to 11.5). Temporal solution data and solids characterization at the end of the experiments are reported. Solution data demonstrated the occurrence of a sustained rate acceleration at temperatures down to 40 °C and the activation energy for these Stage III rates was determined for both glasses. Three major secondary phases were identified at the end of the experiments for both glasses: zeolite P1, zeolite P2, and/or analcime (along with minor phases: zeolites, clays, carbonates). The identification of the crystalline phases at the end of the experiment often differed from the zeolite seed phase. In addition, the use of the Avrami equation showed unimpeded zeolite growth (3-dimensional) in certain conditions, suggesting that in certain conditions the glass dissolution rate is controlled by zeolite formation kinetics whereas in other conditions the glass corrosion process impeded zeolite formation kinetics. The morphological evolution of the samples revealed the growth of the zeolites which completely fill the intergranular space in the powder bed. These results are discussed with regards to previous seeded and unseeded Stage III dissolution rate experiments performed on low- and high-activity nuclear waste glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Glass and a carbon‐free United States: What is glass's role in the upcoming green revolution?

Abstract The climate is changing rapidly due to anthropogenic greenhouse gases. Glass is a significant contributor to these emissions, with 95 million tons of CO 2 being emitted due to glass manufacturing in recent years. Furthermore, glass recycling remains poor in the United States, and most glass is left to landfill after a single use. The lack of recycling and the carbon footprint of manufacturing have made glass an environmentally damaging material despite its theoretical infinite recyclability. Additionally, glass has the potential to enable next‐generation energy materials, enabling the necessary technology for a green economy. In this review, we briefly cover the challenges of glass manufacturing and how to make glass the benchmark material for a carbon‐neutral economy.

Wilkinson, Collin↗

Deformation, Stress Relaxation, and Crystallization of Lithium Silicate Glass Fibers Below the Glass Transition Temperature

The deformation and crystallization of Li(sub 2)O (center dot) 2SiO2 and Li(sub 2)O (center dot) 1.6SiO2 glass fibers subjected to a bending stress were measured as a function of time over the temperature range -50 to -150 C below the glass transition temperature (Tg). The glass fibers can be permanently deformed at temperatures about 100 C below T (sub)g, and they crystallize significantly at temperatures close to, but below T,, about 150 C lower than the onset temperature for crystallization for these glasses in the no-stress condition. The crystallization was found to occur only on the surface of the glass fibers with no detectable difference in the extent of crystallization in tensile and compressive stress regions. The relaxation mechanism for fiber deformation can be best described by a stretched exponential (Kohlrausch-Williams-Watt (KWW) approximation), rather than a single exponential model.The activation energy for stress relaxation, Es, for the glass fibers ranges between 175 and 195 kJ/mol, which is considerably smaller than the activation energy for viscous flow, E, (about 400 kJ/mol) near T, for these glasses at normal, stress-free condition. It is suspected that a viscosity relaxation mechanism could be responsible for permanent deformation and crystallization of the glass fibers below T,

Ray, Chandra S.↗

Effect of glass forming additives on low-activity waste feed conversion to glass

A significant effort was invested in the past to develop and refine mathematical models that relate the composition of nuclear waste glasses with their properties, such as viscosity, electrical conductivity, or chemical durability. However, less attention has been paid to the formulation of the melter feed itself, such as the chemical form and the particle size of the glass forming and modifying additives (GFMA), which have a significant effect on the feed-to-glass conversion process during melting. To address this issue, we systematically changed the mineral composition of a simulated low-activity waste melter feed and inspected its melting behavior. When substituting minerals with corresponding oxides and hydroxides, we found that different alumina sources (kyanite, gibbsite, boehmite, or corundum) had the strongest effect on the feed melting process, whereas the sources of Ca, Mg, and Zr had little effect. Further, the x-ray diffraction analysis showed that the alumina sources differ in their dissolution kinetics: early dissolving alumina sources, such as gibbsite (Al(OH) 3 ) and boehmite (AlO(OH)), increase the transient glass-forming melt viscosity at early stages, when gases still evolve, causing extended foaming, whereas alumina sources that dissolve at high temperatures, such as kyanite (Al 2 SiO 5 ) and corundum (Al 2 O 3 ), keep the transient glass-forming melt viscosity low and lead to a faster foam collapse. Using viscosity-composition relationship to estimate the viscosity of transient glass-forming melts in the primary foaming range, we found that the primary foam began to collapse at 360 to 800 Pa s, and fully collapsed between 65 and 260 Pa s. This result agrees with our previous studies, according to which the glass-forming melt viscosity at the cold cap foam bottom ranged from 24 to 85 Pa s.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Statistical generic design of glass and optimization: Selective review on oxide glasses

Designing a single glass composition for a multidimensional property space is challenging, and the difficulty increases with the number of design criteria. Traditionally, the task is accomplished using multiple statistical models that describe the relationships between composition (C) and property (P) values, i.e., C-P models. Recently, the structure (S)-property (P) statistical modeling has emerged as a complementary approach. The S-P modeling approach has also been shown to be a preferred method for modeling glass properties, particularly when a small data set is available, such as in single-component studies, or when strong nonlinearities exist between composition and properties. The combined model package, C-S-P, implements the concept of generic glass design, i.e., designing glass for performance by first selecting a specific or optimized set of glass network structural groups using S-P models and then transferring the designed structures (genes) to a particular composition using C-S models. This article reviews a set of supporting cases from the previous C-S-P modeling studies of phosphate, silicate, and borosilicate glasses, which are relevant for many critical commercial applications. The methodology for developing the statistical C-S-P database is presented, enabling the application of P?S?C to achieve a generic glass design and optimization, targeting multiple design criteria for both performance and processing properties simultaneously.

Network structure↗

Evaluation Of Glass Density to Support the Estimation of Fissile Mass Loadings in Sludge Batch 10 Glasses

Per a directive from the Department of Energy Savannah River Operations Office (DOE-SR) in 2008, the fissile mass loading concentration must remain below 897 g/m 3 in each high-level waste (HLW) glass canister produced by the Defense Waste Processing Facility (DWPF). To support Sludge Batch 5 (SB5) processing, the Savannah River National Laboratory (SRNL) developed a technical basis that facilitates the evaluation of fissile mass loading of the glass product. The calculation is based on the iron (Fe) concentration in the glass as determined by measurements from the Slurry Mix Evaporator acceptability analysis as well as the glass density. In April 2022, a subsequent DOE-SR directive increased the fissile mass loading limit to 2500 g/m 3 beginning with Sludge Batch 11. Thus, the 897 g/m 3 limit still applies to Sludge Batch 10 (SB10) processing. For SB5 through initial Sludge Batch 9 (SB9) processing prior to coupled operation with the Salt Waste Processing Facility (SWPF), SRNL provided DWPF a bounding glass density value that was based on a statistical evaluation of density measurements. To eliminate the need for experimental work, a composition-based density model for HLW glasses was developed at SRNL in 2019. The objective of this report is to present the bounding glass density determined with the composition-based density model for SB10 sludge-only (SO) and coupled processing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Friction behavior of glass and metals in contact with glass in various environments

Sliding friction experiments have been conducted for heat-resistant glass and metals in contact with glass. These experiments were conducted in various environments including vacuum, moist air, dry air, octane, and stearic acid in hexadecane. Glass exhibited a higher friction force in moist air than it did in vacuum when in sliding contact with itself. The metals, aluminum, iron, and gold, all exhibited the same friction coefficient when sliding on glass in vacuum as glass sliding on glass. Gold-to-glass contacts were extremely sensitive to the environment despite the relative chemical inertness of gold.

Buckley, D. H.↗

Geochemistry of impact glasses from the K/T boundary in Haiti - Relation to smectites and a new type of glass

Detailed element analyses were carried out on 12 black and seven yellow glasses from the K/T boundary section at Beloc (Haiti), and of three samples from smectite mantles around black glasses. The results obtained for bulk black and yellow glasses show differences between these, confirming the results of Sigurdsson et al. (1991) and Izett (1991), and the results obtained on individual spherules and shards are in agreement with bulk data. The present data also demonstrate, for the first time, the existence of yellow glass samples with high CaO but low S contents, which might have formed by fusion of various proportions of carbonates and evaporites or carbonates alone. One of the black glasses was found to have higher than average SiO2 and K2O abundances but lower concentrations of all other major elements. This suggests the existence of a third glass type, named the high Si-K variety (HSi,K) glass.

Koeberl, Christian↗

Raman and Infrared Spectroscopy of Yttrium Aluminum Borate Glasses and Glass-ceramics

Raman spectra of glasses and glass-ceramics in the Y2O3-Al2O3-B2O3 system are reported. Glasses with B2O3 contents ranging from 40 to 60 mole percent were prepared by melting 20 g of the appropriate oxide or carbonate powders in alumina crucibles at 1400 C for 45 minutes. Subsequent heat treatments of the glasses at temperatures ranging from 600 to 800 C were performed in order to induce nucleation and crystallization. It was found that Na2CO3 added to the melt served as a nucleating agent and resulted in uniform bulk crystallization. The Raman spectra of the glasses are interpreted primarily in terms of vibrations of boron - oxygen structural groups. Comparison of the Raman spectra of the glass-ceramic samples with spectra of aluminate and borate crystalline materials reveal that these glasses crystallize primarily as yttrium aluminum borate, YAl3(BO3)4.

Bradley, J.↗

Evolution of glass structure during femtosecond laser assisted crystallization of LaBGeO 5 in glass

Single crystal LaBGeO 5 architecture formed in La 2 O 3 -B 2 O 3 -2GeO 2 glass serves as a model system for understanding of the transformation from glass to single crystal under fs laser irradiation. This transformation is highly sensitive to glass composition, raising the need to understand how the glass structure and composition evolve during crystallization. In this work, micro X-ray absorption spectroscopy and X-ray fluorescence mapping were used to study the glass structure and composition preceding LaBGeO5 crystallization in the region surrounding the single crystal growth front. The results show precipitation of germanium nanoparticles, as well as anisotropic segregation of Ge and La prior to LaBGeO5 crystallization, which are explained assuming electromigration in high fields within the plasma formed by the fs laser irradiation. However, these nanoparticles do not serve as sites for heterogeneous nucleation. Furthermore, the similarity of local structure around Ge in the starting glass and the ultimate crystal appears to enhance the crystallization process.

36 MATERIALS SCIENCE↗