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Glass formulation has a high coefficient of thermal expansion. The glass makes a good hermetic seal for the end of a stainless steel or copper tube such as a sheath of an instrumentation cable.
The primary objective of the work described herein was to develop and identify HLW glass compositions and glass forming additive blends that achieve high waste loadings and processing rates for high phosphorus HLW streams while maintaining acceptable glass properties. This was accomplished through a combination of crucible-scale tests, vertical gradient furnace tests, and confirmation tests on the DM100 melter system.
One of the primary objectives of the work described herein was to develop and identify HLW glass compositions and glass forming additive blends that achieve high waste loadings and processing rates for high manganese HLW streams while maintaining acceptable glass properties. Another objective was to determine the effect of the form of manganese (MnO, MnO2, MnCO3) on feed processing properties, glass production rates, and product quality while vitrifying a high manganese HLW stream. This was accomplished through a combination of crucible-scale tests, vertical gradient furnace tests, and confirmation tests on a DM100 melter system.
The primary objective of the work described herein was to develop and identify HLW glass compositions and glass forming additive blends that achieve high waste loadings and processing rates for high phosphorus HLW streams while maintaining acceptable glass properties. Another objective was to determine the effect of phosphate form (aluminum, iron, sodium) on feed processing properties, glass production rates, and product quality while vitrifying a high phosphorus HLW stream. This was accomplished through a combination of crucible-scale tests, vertical gradient furnace tests, and confirmation tests on a DM100 melter system.
The United States Department of Energy is responsible for managing legacy nuclear waste stored in underground tanks at the Hanford Site. To treat the waste, it is planned as the current baseline to separately vitrify low-activity waste (LAW) and high-level waste fractions. Previously, machine learning (ML) based glass property models (e.g., chemical durability, viscosity, electrical conductivity and SO3 solubility) were developed with prediction uncertainties. A waste glass optimization approach was then established to enable the capability of using these ML models in LAW glass formulation. In this study, the previous ML models were first experimentally validated, and the results were incorporated back into the database to update the ML models. The updated models and formulations showed increased waste loading while reducing the failure rate, demonstrating improved predictive accuracy, reduced uncertainties, and the effectiveness of active learning in guiding high-dimensional, nonlinear LAW glass design. This represents the first experimental validation of ML based LAW glass formulation, with practical benefits such as higher waste loading, shorter mission duration, and lower operational risk.
Baseline glass compositions have been developed and demonstrated for successful immobilization of Hanford high-level waste (HLW) prepared through a pretreatment process. Recent enhanced waste glass formulations have shown promise to increase the waste loading of pretreated sludge compositions from a broader range of HLW feeds. This project proposes to increase the loading of minimally pretreated Hanford HLW in glass by expanding the existing database and glass property-composition models. Estimated direct-feed high level waste (DFHLW) compositions were generated by the Hanford Tank Operations Contractor and used by Pacific Northwest National Laboratory to determine target glass compositions. Gaps in existing data were identified including one high-priority gap in the high Al compositional region. This report summarizes the data collected during the characterization of the DFHLW High Al Glass Matrix. These glasses were intentionally designed with high aluminum concentrations (15 to 30 wt%) and a high likelihood of nepheline formation, which is known to negatively affect glass durability. Some glasses were expected to either fail or approach property constraints to fill data gaps in poorly understood regions of the compositional space due to lack of data. Out of the 50 glasses tested, 14 glasses formed nepheline, while the model predicted nepheline formation in 20 glasses. All quenched glasses met the product consistency test durability constraint; however, 8 glasses failed this constraint after undergoing the canister centerline cooling treatment. Additionally, 17 glasses did not meet the viscosity constraints, 4 failed the EC constraints, and 2 exceeded the allowable T2% for spinel crystal formation. All glasses satisfied the SO 3 solubility limit. The resulting dataset provides valuable information to improve model accuracy and reduce prediction uncertainty. These insights will ultimately support the development of more robust glass formulation strategies, enabling higher waste loadings, reducing operational risks, and expanding the processing envelope.
The present work represents the second of two phases to address the formation of secondary sulfate phases while processing high waste loading LAW formulations with elevated halide, chromium, and phosphate feed concentrations over a wide range of LAW waste types, including those with high potassium concentrations. The Test Plan for the present work outlines a series of tests designed to assess the formation of secondary phases over a range of sulfur and halide concentrations for two LAW streams and associated glass formulations as well as crucible testing to identify additives that have the potential to suppress the formation of secondary phases for wastes with high chlorine contents. The combined results from both phases of testing and from previous tests with these LAW waste streams will be used as inputs to future work to develop concentration limits for these components in the LAW glass property composition models and to support the modification and updating of the current WTP LAW glass formulation algorithm.
Abstract The vitrification of high‐level waste (HLW) by heating a mixture of glass‐forming chemicals (GFCs) with the waste can be improved using a constrained optimization problem. This study explores how different uncertainty propagation (UP) methods implemented with the optimization process can affect the glass formulation of nuclear waste glasses. UP is the effort of propagating uncertain inputs through a system to understand and quantify output distributions. Uncertainty intervals are crafted from output distributions to inform the optimization algorithm. UP is often implemented with Monte Carlo (MC) sampling for large nonlinear systems, which can be difficult to implement within a constrained optimization algorithm that requires derivative information. Other UP methods often used for optimization under uncertainty (OUU) can be designed to work within an established constrained optimization framework. Methods of UP are evaluated in this study including iterative sampling approaches, first‐order approximations, and surrogate modeling with machine learning (ML). A method of dimensional reduction based on global sensitivity analysis is introduced to support the UP methods for the large dimensionality of the problem. Analytical UP methods able to achieve similar optimums 10 times faster than the baseline MC approach, and produce 93.9% similar output distributions are reported.
As a continuation of the Phase 1 HLW model development work as part of a phased approach to enhance and expand HLW glass property-composition models, additional data were collected for the HLW glass dataset and used to revise the models developed during Phase 1. These data are for glasses that are collectively referred to as ORP-2014 glasses. The sources of additional data for the Phase 2 work included: (i) actively designed glasses formulated to support various glass studies at VSL since the completion of Phase 1; and (ii) glasses from two statistically designed matrices to supplement the existing HLW compositional space. The Phase 2 matrix design was intended to augment and improve the coverage in the high aluminum region.
This study investigated the effects of aluminum concentration on simulated high level waste glass properties to eventually establish an aluminum limit (as single-component or multiple-component constraints) for glass formulations for high-aluminum Hanford wastes. A test matrix of 25 high-aluminum glasses (20 = Al 2 O 3 = 28.57 wt%) was generated, and the chemical compositions were measured. The following properties were measured: crystal formation after centerline canister cooling, crystallinity as a function of temperature, density, viscosity, electrical conductivity, toxic leaching characteristics using the Toxicity Characteristic Leaching Procedure, product consistency using the Product Consistency Test, and SO 3 solubility. These results are reported here.
Projections of the number of high level waste (HLW) canisters to be produced in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) (e.g., [1]) are based upon the inventory of the tank wastes, the anticipated performance of the sludge treatment processes, and current understanding of the capability of the borosilicate glass waste form. The WTP HLW melter design, unlike earlier Department of Energy (DOE) melter designs, incorporates a glass bubbler system. The bubblers create active glass pool mixing and thereby improve heat and mass transfer and glass melting rate. The WTP HLW melters each have a glass surface area of 3.75 m 2 and depth of ~1.1 m. The two melters in the HLW facility together are designed to produce up to 7.5 MT of glass per day at 100% availability. Further increases in HLW waste processing rates can potentially be achieved by optimization of the feed and glass formulations, increasing the melter operating temperature above 1150⁰C, and by increasing the waste loading in the glass product. Increasing the waste loading also has the added benefit of decreasing the number of canisters for storage.
Abstract Nuclear waste glass vitrification furnaces are lined with refractory ceramic blocks to contain the molten glass. The refractory liner is susceptible to corrosion and has a finite service lifetime. For this reason, predicting the refractory corrosion in contact with molten glass is integral to estimating melter service lifetime. Standardized laboratory tests varying time and temperature are commonly performed to estimate refractory material loss as a function of glass composition. These data are time and resource‐intensive to collect and are susceptible to considerable measurement error. In order to accelerate glass formulation and design for nuclear waste vitrification, methods are needed to increase laboratory‐scale throughput while maintaining data quality. In this work, a method to remove the residual glass from a corroded coupon using hydrofluoric acid is presented that accelerates the throughput of sample analysis while simultaneously facilitating more accurate measurements.
A composite thermal protection structure, for applications such as atmospheric re-entry vehicles, that can withstand temperatures as high as 3600.degree. F. The structure includes an exposed surface cap having a specially formulated coating, an insulator base adjacent to the cap with another specially formulated coating, and one or more pins that extend from the cap through the insulator base to tie the cap and base together, through ceramic bonding and mechanical attachment. The cap and insulator base have corresponding depressions and projections that mate and allow for differences in thermal expansion of the cap and base. A thin coating of a reaction cured glass formulation is optionally provided on the structure to allow reduce oxidization and/or to reduce catalytic efficiency.
The Vitreous State Laboratory at The Catholic University of America (VSL) is developing and testing glass formulations for RPP-WTP waste envelopes to provide data to meet the RPP-WTP contract requirements and to support system design activities. That work is based upon small-scale batch melts (“crucible melts”) using waste envelope simulants. Selected formulations have also been tested in small-scale continuously-fed joule-heated melters (DM10 and DM100 systems) and, ultimately, in the LAW Pilot Melter. Such melter tests provide information on key process factors such as feed processing behavior, dynamic effects during processing, sulfate incorporation, processing rates, off-gas amounts and compositions, foaming control, etc., that cannot be reliably obtained from crucible melts. This sequential scale-up approach in the vitrification testing program ensures that maximum benefit is obtained from the more costly pilot-scale tests and that the most effective use is made of that resource. The principal objective of the work described in this report was to collect the necessary small-scale melter test data with a LAW Sub-Envelope C1 waste simulant in order to support the next series of tests with the same melter feed on the LAW Pilot Melter. This work was conducted under a corresponding Test Specification and Test Plan.
The present work was intended to expand the available HLW glass property-composition data relating to nepheline formation on CCC heat treatment and to develop improved models to predict nepheline formation that would allow processing of high waste loading high-Al HLW glass formulations at the WTP.
Gaps in glass composition-property data for direct-feed high-level waste (DFHLW) have recently been identified. One such gap is the region of high sulfur solubility since previous, pretreated, high-level wastes contained very little sulfur. Filling this data gap will significantly broaden the range of process flowsheet options including minimal washing and will allow for optimized waste loading in DFHLW glasses. This report summarizes the data collected during the characterization of the DFHLW High S Glass Matrix (HS24). A glass matrix of 50 glass compositions was developed to evenly cover the DFHLW composition region for high sulfur glass. Matrix glasses were designed to expand the composition region outside the current component concentration and property limits so as to reduce uncertainties at the limits. The 50 matrix glasses were fabricated and tested for properties important to the success of DFHLW vitrification including: compositions, canister centerline cooling (CCC) crystallinity and isothermal crystallinity, density, viscosity, electrical conductivity (EC), product consistency test (PCT) response, toxicity, and sulfate solubility. Melter materials corrosion testing is reported elsewhere. These glasses were intentionally designed to have high SO 3 solubilities (0.7 to 2.2 SO 3 wt%) in compositional regions that had not been previously explored. Forty-eight glasses showed the measured SO 3 content retained >80% of the target SO 3 and the densities of all the glasses ranged from 2.49 g·cm -3 to 2.74 g·cm -3 . While the model predicted nepheline formation in 5 glasses, one of the tested 50 CCC glasses formed nepheline, and 35 glasses formed Cr-containing phases such as spinels and eskolaite. Only five glasses were amorphous after CCC treatment where 44 glasses with detectable crystals contained =10 wt% crystals and only one glass had > 10 wt% crystals. None of the glasses exceeded the allowable T 2% for spinel crystal formation at 950 ºC (i.e., no glasses had >2 wt% spinel at 950 ºC) during isothermal crystal fraction tests where 10 glasses showed no crystalline phases at or below 950 ºC. All the glasses (except one which failed being slightly lower than the target) satisfied the SO 3 constraint while 98 glasses did not meet the viscosity constraints and 4 failed the EC constraints. Six quenched (Q) and six CCC glasses failed the Defense Waste Processing Facility (DWPF) Environmental Assessment (EA) glass PCT threshold and 3 Q and 4 CCC failed the PCT design constraint. One glass exceeded the WTP delisting limits for Cr via EPA Method 1311 (i.e., Toxicity Characteristic Leaching Procedure, TCLP). It should be emphasized that some of these glasses were specifically designed to approach or even exceed certain property constraints, as filling data gaps in these regions will provide the greatest benefit for future model development by improving accuracy and reducing uncertainties. These insights will ultimately support the development of more robust glass formulation strategies, enabling higher waste loading, reducing operational risks, and expanding the processing envelope.
A family of glass/ceramic composite materials has been investigated for use as sealants in planar solid oxide fuel cells. These materials are modified versions of a barium calcium aluminosilicate glass developed previously for the same purpose. The composition of the glass in mole percentages is 35BaO + 15CaO + 5Al2O3 + 10B2O3 + 35SiO2. The glass seal was found to be susceptible to cracking during thermal cycling of the fuel cells. The goal in formulating the glass/ ceramic composite materials was to (1) retain the physical and chemical advantages that led to the prior selection of the barium calcium aluminosilicate glass as the sealant while (2) increasing strength and fracture toughness so as to reduce the tendency toward cracking. Each of the composite formulations consists of the glass plus either of two ceramic reinforcements in a proportion between 0 and 30 mole percent. One of the ceramic reinforcements consists of alumina platelets; the other one consists of particles of yttria-stabilized zirconia wherein the yttria content is 3 mole percent (3YSZ). In preparation for experiments, panels of the glass/ceramic composites were hot-pressed and machined into test bars.
A diffusion experiment for glasses was formulated, such theoretical and earth bound results as were available were outlined, and the preliminary earth based experimental work in preparation for a weightless experiment was done. The fundamental premise of the work was that diffusion studies of the glass forming ion can be conducted in zero-g environments, and diffusion data obtained from these experiments are unique and valuable because of earth based experimental difficulties.