Effects of iron oxalate on rhenium incorporation into low-activity waste glass
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George, Jaime L. (ORCID:0000000218716491)↗
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Follow-on Report of Analysis of Approaches to Supplemental Treatment of Low–Activity Waste at the Hanford Nuclear Reservation (Volumes I & II)
The Hanford Site, in southeast Washington State, is preparing to disposition approximately 56,000,000 gallons (56 Mgal) of radioactive and chemically hazardous wastes currently stored in underground tanks at the site. Tank wastes will be divided into a high-activity fraction and a low-activity fraction for subsequent treatment and disposition. A waste processing and treatment facility, the Waste Treatment and Immobilization Plant (WTP), will include the high-level waste (HLW) vitrification facility (WTP HLW Vitrification Facility) for immobilizing the high-activity fraction and a low-activity waste (LAW) vitrification facility (WTP LAW Vitrification Facility) for immobilizing the low-activity fraction. Both facilities will use vitrification technology to immobilize the Hanford tank wastes in a glass waste form.
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Follow-on Report of Analysis of Approaches to Supplemental Treatment of Low-Activity Waste at the Hanford Nuclear Reservation (Vol. I)
The Hanford Site, in southeast Washington State, is preparing to disposition approximately 56,000,000 gallons (56 Mgal) of radioactive and chemically hazardous wastes currently stored in underground tanks at the site. Tank wastes will be divided into a high-activity fraction and a low-activity fraction for subsequent treatment and disposition. A waste processing and treatment facility, the Waste Treatment and Immobilization Plant (WTP), will include the high-level waste (HLW) vitrification facility (WTP HLW Vitrification Facility) for immobilizing the high-activity fraction and a low-activity waste (LAW) vitrification facility (WTP LAW Vitrification Facility) for immobilizing the low-activity fraction. Both facilities will use vitrification technology to immobilize the Hanford tank wastes in a glass waste form. The volume of LAW to be treated and disposed of following waste retrieval and WTP operations will exceed the planned processing capacity of the WTP LAW Vitrification Facility. ORP-11242,-River Protection Project System Plan, estimates a shortfall in LAW treatment capacity of approximately 56 Mgal, approximately 50% of the projected LAW volume. To maintain the planned tank waste processing mission schedule, the U.S. Department of Energy (DOE) will require additional LAW treatment capacity (termed “supplemental LAW”) external to the WTP process. LAW must be solidified by a treatment technology before the waste can be permanently disposed of in an approved DOE on-site disposal facility or a commercial (state or U.S. Nuclear Regulatory Commission [NRC-licensed]) off-site mixed low-level waste disposal facility. A decision on the approach to supplemental LAW treatment, processing, and disposal has not yet been made
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Follow-On Report of Analysis of Approaches to Supplemental Treatment of Low-Activity Waste at the Hanford Nuclear Reservation (Volumes I & II)
The Hanford Site, in southeast Washington State, is preparing to disposition approximately 56,000,000 gallons (56 Mgal) of radioactive and chemically hazardous wastes currently stored in underground tanks at the site. Tank wastes will be divided into a high-activity fraction and a low-activity fraction for subsequent treatment and disposition. A waste processing and treatment facility, the Waste Treatment and Immobilization Plant (WTP), will include the high-level waste (HLW) vitrification facility (WTP HLW Vitrification Facility) for immobilizing the high-activity fraction and a low-activity waste (LAW) vitrification facility (WTP LAW Vitrification Facility) for immobilizing the low-activity fraction. Both facilities will use vitrification technology to immobilize the Hanford tank wastes in a glass waste form.
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Panel Session 98B: Treatment of Low-Activity Tank Waste at Hanford: Considering the Alternatives
This panel focused on alternative treatment of the Hanford Low-Activity Tank Waste. Currently, Tank Waste at the Hanford Site is to be separated into low-activity (LAW) and high-level waste (HLW) fractions, and then vitrified to produce immobilized LAW glass for onsite disposal, and HLW glass for ultimate geologic disposal. This panel discussed several commissioned studies by the National Laboratories, National Academies, and General Accountability Office to evaluate the risks, costs, and benefits associated with considering options for immobilizing portions of the Hanford LAW waste forms. Panelists with presentations: Analysis of Supplemental Treatment Approaches for Low-Activity Waste at the Hanford Nuclear Reservation Overview and Conclusions (Michael Stone); Analysis of Supplemental Treatment Approaches for Low-Activity Waste at the Hanford Nuclear Reservation: Disposal Performance Evaluation (Tom Brouns); National Academies Review of the Study on Supplemental Treatment Approaches of Low-Activity Waste at the Hanford Nuclear Reservation (Charles Ferguson); GAO Observations on Immobilizing Low-Activity Waste at DoE's Hanford Site (David Trimble)
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LDR Inorganic Spiked Simulants in Pozzolan-Substituted Cast Stone for Hanford Pretreated Low-Activity Tank Waste
Pretreated Low Activity Waste (PTW/LAW) at the Hanford Site, is currently projected for disposition through a cementitious waste form. The current standard formulation, Cast Stone, uses Class F fly ash, blast furnace slag, and Portland cement. However, the future availability of Class F fly ash is uncertain, as many coal-fired power plants—the source of this byproduct—are being decommissioned or converted to natural gas. This issue has prompted research into identifying and evaluating suitable alternative materials to replace fly ash in the cementitious waste forms used by the Department of Energy (DOE). The Savannah River National Laboratory (SRNL) successfully identified four natural pozzolans for the replacement of Class F fly ash in the current Savannah River Site (SRS) low-level waste (LLW) form, Saltstone.
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Managing Hanford's Direct Feed Low Activity Waste Program - 20002
The Office of River Protection (ORP) is responsible for the management and completion of the River Protection Project (RPP) mission, which comprises both the Hanford Site tank farms operations and the completion and operation of the Waste Treatment and Immobilization Plant Project. The RPP mission is to safely retrieve, treat, and immobilize Hanford's high-level and low-activity tank waste and close the tank farms to protect the Columbia River. The Direct-Feed Low-Activity Waste (DFLAW) Program is a major subset of the overall RPP mission, providing disposition of low-activity waste. The scope is to retrieve, treat, and immobilize the low-activity waste at the Low-Activity Waste Facility. DFLAW will begin operations no later than December 2023. The DFLAW Program overarches a suite of individual projects, activities, and infrastructure upgrades. The major projects and activities include multiple contractors under both ORP and the Richland Operations Office, underscoring the need for effective integration, coordination, and collaboration. The objectives of the DFLAW Program leadership team are to: - Effectively coordinate and integrate the projects that comprise the DFLAW Program - Manage the interfaces between the projects so that the integrated DFLAW Program is completed successfully - Ensure the DFLAW portfolio of projects operate as required without gaps or conflicts at the interfaces. DOE is accomplishing these objectives through a newly established leadership model that integrates the DOE and contractor work streams and promotes a teamwork model to enable collaborative success. Long considered one of the most formidable cleanup challenges at Hanford, the Department of Energy and its contractors are on the verge of achieving a cleanup commitment that has been decades in the making. DOE is preparing to vitrify (turn to glass) Hanford's chemical and radioactive tank waste using the DFLAW process. The Modified Consent Decree milestone for completing hot commissioning of the Hanford Site's Low- Activity Waste Facility is Dec. 31, 2023. While this milestone may seem distant under normal project management circumstances, it is a relatively short period of time for the operational and cultural transformation necessary to successfully begin treating tank waste at Hanford. Direct feed means separating the waste at a tank farm to remove the more radioactive portion (i.e., solids and cesium) so that the resulting low-activity (less radioactive) waste can be fed directly to the Waste Treatment and Immobilization Plant's Low-Activity Waste Facility. Starting DFLAW will require a singular, intensive leadership focus, along with a sustained, collective commitment to excellence and teamwork by the Department and its contractors. Major upgrades to Hanford's infrastructure will occur prior to startup. Supporting DFLAW operations requires significant integration between the DFLAW facilities - the Waste Treatment Plant, Hanford's tank farms, effluent treatment facilities, disposal facilities - and between all of the site contractors to achieve success. (authors)
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Hanford Immobilized Low-Activity Waste Transportation System Testing Results - 20043
The immobilized low-activity waste (ILAW) transportation system is a first-of-a-kind system that is being designed and tested to transport ILAW glass-filled containers from Hanford's Waste Treatment and Immobilization Plant (WTP) Low-Activity Waste (LAW) Facility to the Integrated Disposal Facility (IDF) burial trench for permanent disposal. A prototype design and fabrication of one transport trailer and four engineered ILAW pallets was completed in mid-2018. Prototype qualification testing to verify adequacy of the design was completed in 2019 by Washington River Protection Solutions (WRPS) and affiliate ATKINS SNC-Lavalin Group. Prototype testing was completed to advance design maturation across all operational and facility interfaces, and under adverse environmental and operating conditions, including thermal assessment of the system at peak projected temperatures. Test design, observation, and feedback was well represented and supported by all ILAW Transportation System interfacing organizations: WTP constructor Bechtel National, Inc.; IDF operator CH2M (CHPRC); transportation contractor Mission Support Alliance (MSA); the U. S. Department of Energy Richland Operations Office (DOE/RL) and Office of River Protection (DOE/ORP); and Washington State Department of Ecology. This paper presents the results of prototype qualification testing and opportunities for design improvements based on testing. Changes to the final design as a result of prototype testing include improvements in safety, ergonomics, operational flexibility, and As-Low-As-Reasonably-Achievable (ALARA) applications. (authors)
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FY24 Development of Improved Grout Waste Forms for Alternative Low Activity Waste Treatment
Since the WTP Low Activity Waste (LAW) Vitrification Facility was not designed to process the entire inventory of Hanford LAW, up to half of the retrieved Hanford LAW will require supplemental immobilization. Immobilizing LAW in a cementitious waste form known as Cast Stone has been investigated as a possible candidate supplemental immobilization technology. In FY21, Washington River Protection Solutions, LLC (WRPS) tasked Atkins and the Vitreous State Laboratory (VSL) of The Catholic University of America (CUA) to perform testing to evaluate methods for reducing the release of COCs, particularly nitrate, 99Tc, and 129I, from cementitious waste forms made from aqueous LAW derived from Hanford Tank Waste. FY22 work built on the FY21 results and further developed formulations while targeting higher waste loadings. The objective of this work was to perform laboratory-scale testing to further refine the most promising formulation(s) that were identified in the FY23 work. The goal of the refinement was to further reduce the release rates for 99Tc, Cr, 129I, and nitrate while maintaining workability of the fresh grout, and to increase waste loading.
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Impacts of constraints and uncertainties on projected amount of Hanford low-activity waste glasses
A systematic evaluation of Hanford low-activity waste (LAW) loading in alkali-aluminoborosilicate glasses was performed. A set of 22 waste compositions were selected to represent the range of wastes anticipated across the Hanford mission. Glass composition was formulated for each waste to simultaneously satisfy a full cadre of property and composition constraints while maximizing waste loading. Glass properties were estimated using property models recently developed for Hanford LAW Facility operation. The impacts from the property and composition constraints on the glass mass to be produced were calculated and compared. Electrical conductivity, Vapor Hydration Test and SO 3 melter tolerance, and canister-centerline cooling crystal constraints have a large effect on reducing total glass mass, while the impact from Product Consistency Test, viscosity, and isothermal crystal constraints is relatively small. Additionally, effects of model prediction and process/composition uncertainties were quantified. The results identified areas of future research that could be useful to improve the efficiency of plant operation.
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Product Consistency Test Results for the Environmental Management Headquarters (EMHQ) Low-Activity Waste (LAW) Glasses
This report provides the results of the Product Consistency Test leachates from the Environmental Management Headquarters Low-Activity Waste glasses, a series of simulated nuclear waste glasses designed and fabricated at the Pacific Northwest National Laboratory. The series included quenched versions of the glasses. These data will be used in the development, validation, and implementation of enhanced property/composition models for waste glass vitrification at Hanford. The measured concentrations of the analytes in the test blank samples were below detection limits. The measured concentrations of B, Li, Na, and Si in the Approved Reference Material-1 samples included with the Product Consistency Tests fell within control chart values indicating proper test performance. The measured glass compositions for the study glasses were close to target values: therefore, little difference was seen when evaluating the normalized values using the targeted or measured glass compositions. The $NC_B$, $NC_{Na}$, and $NC_{Si}$ values were less than the Hanford Tank Waste Treatment and Immobilization Plant low-activity waste constraint of 4 g/L for all glasses.
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Low Temperature Sequential Melting and Anion Retention in Simplified Low Activity Waste
This study seeks to understand the low temperature reactions of the salt phase that occur during the vitrification of Hanford Low Activity Waste (LAW). Salts (such as nitrates, sulfates, carbonates, halides, etc.) play a key role in these low temperature reactions as they sequentially melt, decompose, and volatilize during batch-to-glass conversion. To further understand these complex processes, simplified LAW melts containing oxyanion salts (sodium salts of carbonate, sulfate, and/or nitrate) and early melting glass formers (boric acid) have been evaluated using thermal analysis, infrared absorption spectroscopy, and X-ray diffraction. Results from this study indicate that the volatilization behavior of particular salts is influenced by the presence or absence of other salts. Here, NaNO 3 volatilization is decreased by the presence of Na 2 SO 4 . The addition of either Na 2 SO 4 or NaNO 3 to the system may enhance the volatilization of Na 2 CO 3 . In all cases, Na 2 SO 4 was retained after melting and was often found to be in two different crystalline phases upon quenching.
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Enhanced Hanford Low-Activity Waste Glass Property Data Development: Phase 5 and Phase 6
This report summarizes the data collected on two test matrices of low-activity waste (LAW) glass compositions intended to expand the composition-property database: Low-Activity Waste (LAW) Phase 5: Expansion of LAW Glass Composition Boundaries and LAW Phase 6: High PCT and VHT Response Glass Matrix. Both matrix glass compositions were statistically designed to expand the LAW glass composition region. The analyses performed on these glasses include chemical composition (for target compositional verification), density, viscosity, electrical conductivity, crystal fraction, container centerline cooling with crystal identification, the product consistency test (PCT) response, the vapor hydration test (VHT) response, and sulfur solubility. Because of the slightly different scope of the two matrices, not all methods were applied to both matrices. Specifically, the following measurements were taken only on the LAW Phase 5: Expansion of LAW Glass Composition Boundaries glasses: crystal fraction as a function of temperature, density (ρ), viscosity (η), and electrical conductivity (EC, e). Combined, these data contribute a significant amount, 51 glasses, to the database for high LAW loaded enhanced waste glasses. Most of these data are focused near the boundaries of acceptable PCT and VHT responses, where prediction uncertainties are most impactful.
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Enhanced Hanford Low-Activity Waste Glass Property Data Development: Phase 4
This report summarizes and analyzes the data collected on a fourth test matrix of 25 low-activity waste glass compositions intended to expand the composition-property database and to validate the Vienna et al. (2020) property-composition models. The 25 low-activity waste glass compositions were statistically designed to be within the composition region of the 2020 models. The analyses performed on these glasses include chemical composition (for target compositional verification), density, viscosity, electrical conductivity, crystal fraction, canister centerline cooling with crystal identification, product consistency test response, vapor hydration test response, and sulfur solubility. This report discusses the results obtained from these tests.
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Scaled melter testing of alternative reductants for Low-Activity Waste vitrification: Melter feed properties and processing behavior
This study examines the use of boron nitride (BN) and coke dust as alternative reductants for low-activity waste vitrification in scaled melter systems, intended to enhance operational flexibility at the Hanford Waste Treatment and Immobilization Plant. The baseline reductant, sucrose, while widely considered advantageous for glass production rates, produces challenging off gas emissions during processing. Early crucible-scale testing indicated that BN and coke effectively control foaming and glass redox, while significantly reducing acetonitrile emissions. Both real tank waste and simulant waste melter feeds were tested with BN and coke in this study. Rheological properties for melter feeds with both reductants were within operational limits, although the particle size of coke should be controlled and sufficient agitation is necessary to ensure smooth operations. While promising for handling and reduction of emissions, both simulant melter feeds demonstrated lower average glass production rates in the simulant melter system compared with sucrose. In the radioactive system, the rates were more comparable to previously measured low activity waste feeds on the order of 1285 kg m 2 day −1 for BN and 1671 kg m −2 day −1 for coke. Further scale-up testing is required to interpret the processing rates in the context of the full scale melter systems and evaluate the cost-benefit impact of these reductants on efficiency and sustainability.
Rigby, Jessica C. [Pacific Northwest National Labo↗
Effect of sucrose on technetium and rhenium retention during vitrification of low-activity wastes
Sucrose (C 12 H 22 O 11 ) has been used in low-activity waste (LAW) melter feeds containing large fractions of nitrates, nitrites, or both because it facilitates foam suppression and denitration. This study focused on the effect of sucrose in LAW feeds on technetium (Tc) and rhenium (Re) retention. The amount of sucrose added in feeds was varied to differentiate the carbon-to-nitrogen mole ratio (C/N ratio). The results show that larger sucrose addition (higher C/N ratio) enhances Tc and Re retention. Reducing conditions induced by sucrose decomposition and early chemical reactions between sucrose and NaNO 3 /NaNO 2 are expected to increase Tc and Re retention. However, high sucrose addition decreased sulfur (S) retention slightly because sodium sulfate decomposes in reducing conditions at lower temperature. This early sulfate decomposition can affect Tc and Re retention partly because these species can be soluble in sulfate phases. This correlation indicates that the decrease of sulfate phases in the glass by early decomposition can reduce the solubility of Tc and Re in the sulfate phases, which may increase Tc and Re retention in the glass. In addition, continuous gas evolution and vigorous foaming at the foaming temperature range of 700–900°C may influence Tc and Re retention process interrupting retention or facilitating volatilization.
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Evaluation of Material Balance Approaches for Hanford Direct-Feed Low Activity Waste Processing - 20022
The Hanford Site has accumulated millions of gallons of tank waste from reprocessing spent fuel to recover plutonium, uranium, cesium, and strontium. The supernatant from the accumulated tank waste will be treated using a Direct Feed Low-Activity Waste approach. The supernatant will be treated to remove solids and cesium in the Tank-Side Cesium Removal process in the Hanford tank farm, then vitrified in a semi-batch process in the Hanford Waste Treatment and Immobilization Plant (WTP). Currently, each batch of feed is sampled at three locations prior to being fed to the melter: the feed qualification tank in the Hanford tank farm as well as the concentrate receipt vessel (CRV) and melter feed preparation vessel (MFPV) in the WTP. The feed qualification sample is taken from a large batch of accumulated feed, only two to three samples are expected each year. Approximately 275 samples from the CRVs and 1100 samples from the MFPV are expected each year. An evaluation was performed to determine if a material balance based on the feed qualification sample could replace most of the sampling in the CRVs and MFPVs. The evaluation consisted of three elements: (1) determination of the practicality of using a material balance to estimate the stream composition of the CRV and MFPV contents, (2) evaluation of whether the material balance could be automated using the existing process control system, and (3) determination of the uncertainty in glass composition using the material balance approach. It is assumed that periodic sampling at the CRV and MFPV would be performed periodically to re-baseline the material balance, evaluations are in progress to determine the frequency of this periodic sampling. Process sample locations downstream of the melter were reviewed as well, but the partitioning of semi-volatile species in the melter was determined to preclude extending the material balance approach past the melter. It was determined that replacement of the CRV sample location was feasible and did not increase process uncertainty or significantly impact waste loading. Replacement of the MFPV sample was also determined to be feasible, but that measurement of the glass former chemical addition may be needed prior to addition of these chemicals to the MFPV. This measurement could be performed by an in situ laser-induced breakdown spectroscopy (LIBS) system. Limited tests were performed to evaluate LIBS for direct measurements of the low-activity waste melter feed. The use of a material balance would eliminate over 1200 samples each year if only 10% of the CRV and MFPV batches are sampled and could likely allow the WTP laboratory to operate on days only versus 24/7 operation. (authors)
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Application of the immobilized low-activity waste glass corrosion model to the static dissolution of 24 statistically-designed alkali-borosilicate waste glasses
Glass corrosion models that capture the complex mechanisms of the glass-water reaction enable the prediction of nuclear waste glass durability in disposal scenarios. Parameterization of such models is challenging because of the need to capture changes in corrosion behavior with time, reaction conditions, and glass composition. In this report we describe and employ the immobilized low activity waste (ILAW) glass corrosion model (IGCM) in geochemical simulations of static dissolution tests, at two temperatures (40 °C and 90 °C), for a matrix of 24 enhanced low activity waste (eLAW) glasses statistically designed to cover a processable composition space defined by 8 major glass components (Al 2 O 3 , B 2 O 3 , CaO, Na 2 O, SiO 2 , SnO 2 , ZrO 2 , and Others as defined in the text). The IGCM includes a first-order chemical affinity term and an ion-exchange term that represents the net exchange of Na+ ions in the pristine glass with protons in aqueous solution. Constant, time-dependent, and time- and pH-dependent functional forms of the ion-exchange term are evaluated to reproduce the change in corrosion behavior with time in saturated, static dissolution tests. The agreement with measured aqueous concentrations of the main glass components (B, Na, and Si) improved significantly upon addition of a time-dependent term, which therefore constitutes a simple representation of the glass-water reaction progress. Due to the limited changes in pH in the static dissolution tests, past a short initial period of rapid increase, addition of a pH dependent term did not appreciably improve the fits, indicating that comprehensive model parameterization requires more than one type of glass corrosion test to capture a wide range of solution chemistries. IGCM parameters were found to be dependent on glass composition, and the parameter sets generated in this work will enable the development of composition–parameter correlation models that offer the promise of predicting IGCM parameters, and thus glass corrosion behavior, solely based on glass composition.
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