The effects of phosphorus pentoxide additions on the thermal, rheological, and structural properties of sodium borosilicate glass
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Engineering topics
Publications and source records attributed to Kruger, A. A..
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To provide mission support to the WTP for the vitrification of legacy nuclear tank waste at the Hanford site, a reduced-scale vitrification pilot system is being designed to process simulated and actual radioactive tank wastes. The waste stored in underground tanks will be separated into HLW and LAW fractions, where the majority is LAW by mass (approximately 90%) and HLW by activity (greater than 95%). The first tank waste to be processed at the WTP will be LAW. Because Hanford tank waste and the resultant melter feed compositions are known to vary widely, pilot-scale operations are essential to identify potential problems, provide needed data, confirm assumptions, and determine impacts to full-scale melters and off-gas systems from these different feeds. In addition, the reduced-scale melter system must be capable of quickly providing results to operations without the typically high cost of full-scale radioactive operations and to provide an engineering platform in close proximity to local operations staff. The objectives of this computational modeling effort are to produce process conditions like those encountered in the WTP LAW melters and to minimize the volume of radioactive waste necessary for the evaluations. To this end, melter design features are being explored to increase production without significantly increasing surface area or melter-glass volumes or compromising data quality. In support of these objectives, a set of computational fluid dynamic models was developed to provide insight into the flow patterns within these small melters and evaluate design features to increase production without significantly increasing glass inventory. Computed velocities were evaluated at the interface between the cold cap and the molten-glass pool and within the bulk-glass pool. Since melt rate correlates with the velocity underneath the cold cap, this information can be used to select design features that produce the highest gains. (authors)
Abstract not provided
The Hanford Low-Activity Waste (LAW) vitrification facility will receive LAW batches with abruptly changing compositions that span relatively broad ranges. In particular, the concentration ratios of sodium-to-sulfate, -chloride, -chromate, -phosphate, -potassium, and -aluminate create challenges in glass formulation. Glass compositions that simultaneously satisfy several processability, product quality, and composition constraints with sufficient confidence must be formulated for each LAW batch in near-realtime to enable desired throughput. A method for developing glass compositions while maximizing the waste loading and the process robustness was developed. This method compiled the glass composition-property data collected over nearly two decades, primarily by Pacific Northwest National Laboratory, The Catholic University of America, and Savannah River National Laboratory, in support of both the Hanford Tank Waste Treatment and Immobilization Plant project and the U.S. Department of Energy Office of River Protection Enhanced Waste Glass project. These data were used to develop models that link the melter feed composition to the resulting glass properties. Mathematical constructs were developed to optimize glass compositions for each waste batch in real-time that will simultaneously satisfy processability, product quality, and composition constraints with sufficient statistical confidence. Property prediction and various process uncertainties were reflected in the formulation. The formulation approach directly lends itself to adjustment of glass formulation to achieve program goals. This presentation will summarize the formulation approach and supporting data. (authors)
Computational modeling is a powerful complement to laboratory experiments and testing of systems at various scales. When properly applied and validated, computational fluid dynamics (CFD) can provide information not readily obtainable by physical testing, especially in cases where the operating environment does not permit visual observation or the insertion of typical data acquisition instrumentation as in the case of waste glass vitrification. A series of CFD and heat transfer models over a range of scales are being developed to support melter operations at the Hanford Waste Treatment and Immobilization Plant. This paper provides a description of the models and the resulting information they provide that can be used to improve melter throughput, as well as aid in evaluating and resolving operating plant issues or upsets. This work is important for the WTP operation by providing a potential for model-predictive control of the melter operation. Increases in the rate of glass production and avoiding idling can significantly decrease the duration and cost of the vitrification campaign, potentially saving billions of dollars. (authors)
Analyses were performed to evaluate the impacts of using the advanced glass models, constraints, and uncertainty descriptions on projected Hanford glass mass. The maximum allowable waste oxide loading (WOL) was estimated for waste compositions while simultaneously satisfying all applicable glass property and composition constraints with sufficient confidence. Different components of prediction and composition/process uncertainties were systematically included in the calculations to evaluate their impacts on glass mass. The analyses estimated the production of 23,360 MT of immobilized high-level waste (IHLW) glass when no uncertainties were taken into account. Accounting for prediction and composition/process uncertainties resulted in 5.01 relative percent increase in estimated glass mass of 24,531 MT. Roughly equal impacts were found for prediction uncertainties (2.58 RPD) and composition/process uncertainties (2.43 RPD). The immobilized low-activity waste (ILAW) mass was predicted to be 282,350 MT without uncertainty and with waste loading “line” rules in place. Accounting for prediction and composition/process uncertainties resulted in only 0.08 relative percent increase in estimated glass mass of 282,562 MT. Without application of line rules the glass mass decreases by 10.6 relative percent (252,490 MT) for the case with no uncertainties. Addition of prediction uncertainties increases glass mass by 1.32 relative percent and the addition of composition/process uncertainties increase glass mass by an additional 7.73 relative percent (9.06 relative percent increase combined). The glass mass estimate without line rules (275,359 MT) was 2.55 relative percent lower than that with the line rules (282,562 MT), after accounting for all applicable uncertainties.
Analyses were performed to evaluate the impacts of using the advanced glass models, constraints (Vienna et al. 2016), and uncertainty descriptions on projected Hanford glass mass. The maximum allowable waste oxide loading (WOL) was estimated for waste compositions while simultaneously satisfying all applicable glass property and composition constraints with sufficient confidence. Different components of prediction and composition/process uncertainties were systematically included in the calculations to evaluate their impacts on glass mass. The analyses estimated the production of 23,360 MT of immobilized high-level waste (IHLW) glass when no uncertainties were taken into account. Accounting for prediction and composition/process uncertainties resulted in 5.01 relative percent increase in estimated glass mass of 24,531 MT. Roughly equal impacts were found for prediction uncertainties (2.58 RPD) and composition/process uncertainties (2.43 RPD). The immobilized low-activity waste (ILAW) mass was predicted to be 282,350 MT without uncertainty and with waste loading “line” rules in place. Accounting for prediction and composition/process uncertainties resulted in only 0.08 relative percent increase in estimated glass mass of 282,562 MT. Without application of line rules the glass mass decreases by 10.6 relative percent (252,490 MT) for the case with no uncertainties. Addition of prediction uncertainties increases glass mass by 1.32 relative percent and the addition of composition/process uncertainties increase glass mass by an additional 7.73 relative percent (9.06 relative percent increase combined). The glass mass estimate without line rules (275,359 MT) was 2.55 relative percent lower than that with the line rules (282,562 MT), after accounting for all applicable uncertainties
About 50 million gallons of high-level mixed waste is currently stored in underground tanks at the United States Department of Energy’s (DOE’s) Hanford site in the State of Washington. The Hanford Tank Waste Treatment and Immobilization Plant (WTP) will provide DOE’s Office of River Protection (ORP) with a means of treating this waste by vitrification for subsequent disposal. Corrosion of the melter materials of construction by the low activity waste (LAW) glass can significantly affect the life of the WTP LAW melters. The materials that are in contact with molten LAW glass include Inconel 690 alloy and Monofrax™ K-3 refractory. This report presents the results from experiments that were conducted to evaluate the corrosion of Inconel 690 and Monofrax™ K-3 refractory in representative high waste loading LAW glass formulations under conditions where loss of volatile constituents was minimized.
The U.S. Department of Energy Office of River Protection (ORP) has initiated and leads an integrated Advanced Waste Glass (AWG) program to increase the loading of Hanford tank wastes in glass while meeting melter lifetime expectancies and process, regulatory, and product performance requirements. The integrated ORP program is focused on providing a technical, science-based foundation for making key decisions regarding the successful operation of the Hanford Tank Waste Treatment and Immobilization Plant (WTP) facilities in the context of an optimized River Protection Project (RPP) flowsheet. The fundamental data stemming from this program will support development of advanced glass formulations, key product performance and process control models, and tactical processing strategies to ensure safe and successful operations for both the low-activity waste (LAW) and high-level waste vitrification facilities. These activities will be conducted with the objective of improving the overall RPP mission by enhancing flexibility and reducing cost and schedule.
This report describes the results of testing specified by the Test Plans (VSL-08T1520-1 Rev 0 and VSL-08T1510-1 Rev 0). The work was performed in compliance with the quality assurance requirements specified in the Test Plans. Results required by the Test Plans are reported. The test results and this report have been reviewed for correctness, technical adequacy, completeness, and accuracy.
The U.S. Department of Energy (DOE) is building a Tank Waste Treatment and Immobilization Plant (WTP) at the Hanford Site in Washington to remediate 55 million gallons of radioactive waste that is being temporarily stored in 177 underground tanks. Efforts are being made to increase the loading of Hanford tank wastes in glass while meeting melter lifetime expectancies and process, regulatory, and product quality requirements. This road map guides the research and development for formulation and processing of crystal-tolerant glasses, identifying near- and long-term activities that need to be completed over the period from 2014 to 2019. The primary objective is to maximize waste loading for Hanford waste glasses without jeopardizing melter operation by crystal accumulation in the melter or melter discharge riser. The potential applicability to the Savannah River Site (SRS) Defense Waste Processing Facility (DWPF) will also be addressed in this road map. The planned research described in this road map is motivated by the potential for substantial economic benefits (significant reductions in glass volumes) that will be realized if the current constraints (T 1% for WTP and T L for DWPF) are approached in an appropriate and technically defensible manner for defense waste and current melter designs. The basis of this alternative approach is an empirical model predicting the crystal accumulation in the WTP glass discharge riser and melter bottom as a function of glass composition, time, and temperature. When coupled with an associated operating limit (e.g., the maximum tolerable thickness of an accumulated layer of crystals), this model could then be integrated into the process control algorithms to formulate crystal-tolerant high-level waste (HLW) glasses targeting high waste loadings while still meeting process related limits and melter lifetime expectancies. The modeling effort will be an iterative process, where model form and a broader range of conditions, e.g., glass composition and temperature, will evolve as additional data on crystal accumulation are gathered. Model validation steps will be included to guide the development process and ensure the value of the effort (i.e., increased waste loading and waste throughput). A summary of the stages of the road map for developing the crystal-tolerant glass approach, their estimated durations, and deliverables is provided.
Spinel crystals precipitate in high-level waste glasses containing Fe, Cr, Ni, Mn, Zn, and Ru. The liquidus temperature (T{sub L}d) of spinel as the primary crystallization phase is a function of glass composition, and the spinel solubility (c{sub o}) is a function of both glass composition and temperature (T). Previously reported models of T{sub L} as a function of composition are based on T{sub L} measured directly, which requires laborious experimental procedures. Viewing the curve of c{sub o} versus T as the liquidus line allows a significant broadening of the composition region for model fitting. This paper estimates T{sub L} as a function of composition based on c{sub o} data obtained with the X-ray diffraction technique.
The major factor limiting waste loading in continuous high-level radioactive waste (HLW) melters is an accumulation of particles in the glass discharge riser during a frequent and periodic idling of more than 20 days. An excessive accumulation can produce robust layers a few centimeters thick, which may clog the riser, preventing molten glass from being poured into canisters. Since the accumulation rate is driven by the size of particles we investigated with x-ray microtomography, scanning electron microscopy, and image analysis the impact of spinel forming components, noble metals, and alumina on the size, concentration, and spatial distribution of particles, and on the accumulation rate. Increased concentrations of Fe and Ni in the baseline glass resulted in the formation of large agglomerates that grew over the time to an average size of ~185+-155 {mu}m, and produced >3 mm thick layer after 120 h at 850 deg C. The noble metals decreased the particle size, and therefore significantly slowed down the accumulation rate. Addition of alumina resulted in the formation of a network of spinel dendrites which prevented accumulation of particles into compact layers.
Plans for the treatment of high level waste (HL W) at the Hanford Tank Waste Treatment and Immobilization Plant (WTP) are based upon the inventory of the tank wastes, the anticipated performance of the pretreatment processes, and current understanding of the capability of the borosilicate glass waste form. The WTP HLW melter design, unlike earlier DOE melter designs, incorporates an active glass bubbler system. The bubblers create active glass pool convection and thereby improve heat and mass transfer and increase glass melting rates. The WTP HLW melter has 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 HL W waste processing rates can potentially be achieved by increasing the melter operating temperature above 1150°C 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.