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At least 109 records · Page 6

Performance Test on Polymer Waste Form - 12137

Polymer solidification was attempted to produce stable waste form for the boric acid concentrates and the dewatered spent resins. The polymer mixture was directly injected into the mold or drum which was packed with the boric acid concentrates and the dewatered spent resins, respectively. The waste form was produced by entirely curing the polymer mixture. A series of performance tests was conducted including compressive strength test, water immersion test, leach test, thermal stability test, irradiation stability test and biodegradation stability test for the polymer waste forms. From the results of the performance tests for the polymer waste forms, it is believed that the polymer waste form is very stable and can satisfy the acceptance criteria for permanent disposal. At present, performance tests with full scale polymer waste forms are being carried out in order to obtain qualification certificate by the regulatory institute in Korea. Polymer waste forms were prepared with the surrogate of boric acid concentrates and the surrogate of spent ion exchange resins respectively. Waste forms were also made in lab scale and in full scale. Lab. scale waste forms were directly subjected to a series of the performance tests. In the case of full scale waste form, the test specimens for the performance test were taken from a part of waste form by coring. A series of performance tests was conducted including compressive strength test, thermal stability test, irradiation stability test and biodegradation stability test, water immersion test, leach test, and free standing water for the polymer waste forms. In addition, a fire resistance test was performed on the waste forms by the requirement of the regulatory institute in Korea. Every polymer waste forms containing the boric acid concentrates and the spent ion exchange resins had exhibited excellent structural integrity of more than 27.58 MPa (4,000 psi) of compressive strength. On thermal stability testing, biodegradation testing and water immersion testing, no degradation was observed in the waste forms. Also, by measuring the compressive strength after these tests, it was confirmed that the structural integrity was still retained. A leach test was performed by using non radioactive cobalt, cesium and strontium. The leaching of cobalt, cesium and strontium from the polymer waste forms was very low. Also, the polymer waste forms were found to possess adequate fire resistance. From the results of the performance tests, it is believed that the polymer waste form is very stable and can satisfy the acceptance criteria for permanent disposal. At present, Performance tests with full scale polymer waste forms are on-going in order to obtain qualification certificate by the regulatory institute in Korea. (authors)

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Reevaluation of Vitrified High-Level Waste Form Criteria for Potential Cost Savings at the Defense Waste Processing Facility - 13598

At the Savannah River Site (SRS) the Defense Waste Processing Facility (DWPF) has been immobilizing SRS's radioactive high level waste (HLW) sludge into a durable borosilicate glass since 1996. Currently the DWPF has poured over 3,500 canisters, all of which are compliant with the U. S. Department of Energy's (DOE) Waste Acceptance Product Specifications for Vitrified High-Level Waste Forms (WAPS) and therefore ready to be shipped to a federal geologic repository for permanent disposal. Due to DOE petitioning to withdraw the Yucca Mountain License Application (LA) from the Nuclear Regulatory Commission (NRC) in 2010 and thus no clear disposal path for SRS canistered waste forms, there are opportunities for cost savings with future canister production at DWPF and other DOE producer sites by reevaluating high-level waste form requirements and compliance strategies and reducing/eliminating those that will not negatively impact the quality of the canistered waste form. (authors)

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Reevaluation Of Vitrified High-Level Waste Form Criteria For Potential Cost Savings At The Defense Waste Processing Facility

At the Savannah River Site (SRS) the Defense Waste Processing Facility (DWPF) has been immobilizing SRS's radioactive high level waste (HLW) sludge into a durable borosilicate glass since 1996. Currently the DWPF has poured over 3,500 canisters, all of which are compliant with the U. S. Department of Energy's (DOE) Waste Acceptance Product Specifications for Vitrified High-Level Waste Forms (WAPS) and therefore ready to be shipped to a federal geologic repository for permanent disposal. Due to DOE petitioning to withdraw the Yucca Mountain License Application (LA) from the Nuclear Regulatory Commission (NRC) in 2010 and thus no clear disposal path for SRS canistered waste forms, there are opportunities for cost savings with future canister production at DWPF and other DOE producer sites by reevaluating high-level waste form requirements and compliance strategies and reducing/eliminating those that will not negatively impact the quality of the canistered waste form.

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AI/ML-assisted Design of Phosphate Glass and Ceramic Nuclear Waste Forms

Borosilicate glass is the widely accepted waste form for immobilization of high and medium level nuclear wastes. Advances in nuclear energies and new reactor designs require the development of new waste forms. For example, wastes from molten salt reactors and reprocessing of nuclear fuels lead to salt-based wastes that are difficult to be immobilized by conventional borosilicate glasses due to limited solubility and waste loading. In designing new waste forms, machine learning (ML) and artificial intelligence (AI) based approaches are much needed and can be beneficial in enabling a more efficient design in large parameter spaces as compared to traditional Edisonian trial-and-error approaches. Here, we report in this paper the rationale and latest progress of our ML/AI-based design of phosphate-based waste forms.

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FY22 Development of Improved Grout Waste Forms for Supplemental Low Activity Waste Treatment

About 54 to 56 million gallons of radioactive 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. This waste will be separated into low- and high activity waste fractions, which will then be vitrified respectively into Immobilized Low Activity Waste (ILAW) and Immobilized High Level Waste (IHLW) products for subsequent disposal. The ILAW product will be disposed of in an engineered facility at the Hanford site while the IHLW product is designed for acceptance into a national deep geological disposal facility for high level nuclear waste. Treatment of the tank waste will take place in the Hanford Tank Waste Treatment and Immobilization Plant (WTP), which is under construction. However, 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

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Summary Report: Glass-Ceramic Waste Forms for Combined Fission Products

Glass-ceramic waste form development began in FY 2010 examining two combined waste stream options: (1) alkaline earth (CS) + lanthanide (Ln), and (2) + transition metal (TM) fission-product waste streams generated by the uranium extraction (UREX+) separations process. Glass-ceramics were successfully developed for both options however; Option 2 was selected over Option 1, at the conclusion of 2010, because Option 2 immobilized all three waste streams with only a minimal decrease in waste loading. During the first year, a series of three glass (Option 2) were fabricated that varied waste loading-WL (42, 45, and 50 mass%) at fixed molar ratios of CaO/MoO{sub 3} and B{sub 2}O{sub 3}/alkali both at 1.75. These glass-ceramics were slow cooled and characterized in terms of phase assemblage and preliminary irradiation stability. This fiscal year, further characterization was performed on the FY 2010 Option 2 glass-ceramics in terms of: static leach testing, phase analysis by transmission electron microscopy (TEM), and irradiation stability (electron and ion). Also, a new series of glass-ceramics were developed for Option 2 that varied the additives: Al{sub 2}O{sub 3} (0-6 mass%), molar ratio of CaO/MoO{sub 3} and B{sub 2}O{sub 3}/alkali (1.75 to 2.25) and waste loading (50, 55, and 60 mass%). Lastly, phase pure powellite and oxyapatite were synthesized for irradiation studies. Results of this fiscal year studies showed compositional flexibility, chemical stability, and radiation stability in the current glass-ceramic system. First, the phase assemblages and microstructure of all of the FY 2010 and 2011 glass-ceramics are very similar once subjected to the slow cool heat treatment. The phases identified in these glass-ceramics were oxyapatite, powellite, cerianite, and ln-borosilicate. This shows that variations in waste loading or additives can be accommodated without drastically changing the phase assemblage of the waste form, thus making the processing and performance characteristics of the waste form more predictable/flexible. However, in the future, the glass phase still needs to be accurately characterized to determine the effects of waste loading and additives on the glass structure. Initial investigations show a borosilicate glass phase rich in silica. Second, the normalized concentrations of elements leached from the waste form during static leach testing were all below 0.6 g/L after 28d at 90 C, by the Product Consistency Test (PCT), method B. These normalized concentrations are on par with durable waste glasses such as the Low-Activity Reference Material (LRM) glass. The release rates for the crystalline phases (oxyapatite and powellite) appear to be lower (more durable) than the glass phase based on the relatively low release rates of Mo, Ca, and Ln found in the crystalline phases compared to Na and B that are mainly observed in the glass phase. However, further static leach testing on individual crystalline phases is needed to confirm this statement. Third, Ion irradiation and In situ TEM observations suggest that these crystalline phases (such as oxyapatite, ln-borosilicate, and powellite) in silicate based glass ceramic waste forms exhibit stability to 1000 years at anticipated doses (2 x 10{sup 10}-2 x 10{sup 11} Gy). This is adequate for the short lived isotopes in the waste, which lead to a maximum cumulative dose of {approx}7 x 10{sup 9} Gy, reached after {approx}100 yrs, beyond which the dose contributions are negligible. The cumulate dose calculations are based on a glass-ceramic at WL = 50 mass%, where the fuel has a burn-up of 51GWd/MTIHM, immobilized after 5 yr decay from reactor discharge.

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Secondary Waste Form Down Selection Data Package – Ceramicrete

As part of high-level waste pretreatment and immobilized low activity waste processing, liquid secondary wastes will be generated that will be transferred to the Effluent Treatment Facility on the Hanford Site for further treatment. These liquid secondary wastes will be converted to stable solid waste forms that will be disposed in the Integrated Disposal Facility. Currently, four waste forms are being considered for stabilization and solidification of the liquid secondary wastes. These waste forms are Cast Stone, Ceramicrete, DuraLith, and Fluidized Bed Steam Reformer. The preferred alternative will be down selected from these four waste forms. Pacific Northwest National Laboratory is developing data packages to support the down selection process. The objective of the data packages is to identify, evaluate, and summarize the existing information on the four waste forms being considered for stabilization and solidification of the liquid secondary wastes. The information included will be based on information available in the open literature and from data obtained from testing currently underway. This data package is for the Ceramicrete waste form. Ceramicrete is a relatively new engineering material developed at Argonne National Laboratory to treat radioactive and hazardous waste streams (e.g., Wagh 2004; Wagh et al. 1999a, 2003; Singh et al. 2000). This cement-like waste form can be used to treat solids, liquids, and sludges by chemical immobilization, microencapsulation, and/or macroencapsulation. The Ceramicrete technology is based on chemical reaction between phosphate anions and metal cations to form a strong, dense, durable, low porosity matrix that immobilizes hazardous and radioactive contaminants as insoluble phosphates and microencapsulates insoluble radioactive components and other constituents that do not form phosphates. Ceramicrete is a type of phosphate-bonded ceramic, which are also known as chemically bonded phosphate ceramics. The Ceramicrete binder is formed through an acid-base reaction between calcined magnesium oxide (MgO; a base) and potassium hydrogen phosphate (KH{sub 2}PO{sub 4}; an acid) in aqueous solution. The reaction product sets at room temperature to form a highly crystalline material. During the reaction, the hazardous and radioactive contaminants also react with KH{sub 2}PO{sub 4} to form highly insoluble phosphates. In this data package, physical property and waste acceptance data for Ceramicrete waste forms fabricated with wastes having compositions that were similar to those expected for secondary waste effluents, as well as secondary waste effluent simulants from the Hanford Tank Waste Treatment and Immobilization Plant were reviewed. With the exception of one secondary waste form formulation (25FA+25 W+1B.A. fabricated with the mixed simulant did not meet the compressive strength requirement), all the Ceramicrete waste forms that were reviewed met or exceeded Integrated Disposal Facility waste acceptance criteria.

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Synroc Waste-forms for Immobilization of Advanced Reprocessing Wastes - 16167

EURO-GANEX, an advanced reprocessing technology, aims to separate both major (U, Pu) and minor (Np, Am, and Cm) actinides together from fission products. As the final waste composition is free from actinides - as opposed to current process waste, e.g. from PUREX - adapted immobilization matrices need to be developed. Synroc is a potential wasteform that has proven itself to be efficient to immobilize high-level nuclear wastes (HLW). In this study, a new composition of Synroc, 'Synroc-Z', is designed and characterized. The primary modification is to reduce the amount of zirconolite phase, which acts as the main host for actinides. The optimum hot-press conditions for Synroc-Z samples with a waste loading of 20 wt% were determined to be: 1200 deg. C and 20 MPa for 3 h. The durability of Synroc-Z was examined via the MCC-1 test at 90 deg. C. It shows similar leach resistance to Synroc-C, which is much better than current glass waste-forms. (authors)

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Efficacy of a Solution-Based Approach for Making Sodalite Waste Forms for an Oxide Reduction Salt Utilized in the Reprocessing of Used Uranium Oxide Fuel

This paper describes various approaches for making sodalite with a LiCl-Li2O oxide reduction salt used to recover uranium from used oxide fuel. The approaches include sol-gel and solution-based synthesis processes. As-made products were mixed with 5 and 10 mass% of a Na2O-B2O3-SiO2 glass binder and these, along with product without a binder, were heated using either a cold-press-and-sinter method or hot uniaxial pressing. The results demonstrate the limitation of sodalite yield due to the fast intermediate reactions between Na+ and Cl- to form halite in solution and Li2O and SiO2 to form lithium silicates (e.g., Li2SiO3 or Li2Si2O5) in the calcined and sintered pellets. The results show that pellets can be made with high sodalite fractions (~92 mass%) and low porosities using a solution-based approach and this LiCl-Li2O salt.

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Radioactive Demonstration of Mineralized Waste Forms Made from Hanford Low Activity Waste (Tank SX-105, Tank AN-103, and AZ-101/102) by Fluidized Bed Steam Reformation (FBSR)

Fluidized Bed Steam Reforming (FBSR) is a robust technology for the immobilization of a wide variety of radioactive wastes. Applications have been tested at the pilot scale for the high sodium, sulfate, halide, organic and nitrate wastes at the Hanford site, the Idaho National Laboratory (INL), and the Savannah River Site (SRS). Due to the moderate processing temperatures, halides, sulfates, and technetium are retained in mineral phases of the feldspathoid family (nepheline, sodalite, nosean, carnegieite, etc). The feldspathoid minerals bind the contaminants such as Tc-99 in cage (sodalite, nosean) or ring (nepheline) structures to surrounding aluminosilicate tetrahedra in the feldspathoid structures. The granular FBSR mineral waste form that is produced has a comparable durability to LAW glass based on the short term PCT testing in this study, the INL studies, SPFT and PUF testing from previous studies as given in the columns in Table 1-3 that represent the various durability tests. Monolithing of the granular product was shown to be feasible in a separate study. Macro-encapsulating the granular product provides a decrease in leaching compared to the FBSR granular product when the geopolymer is correctly formulated.

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Developments in Processing Criteria for Iron Phosphate Waste Form Design for Treating Electrorefiner Salt Wastes

This report describes work done under a Nuclear Energy University Partnership (NEUP) project that included a collaborative effort between Pacific Northwest National laboratory, University of Nevada Reno, University to Utah, and Missouri University of Science and Technology. In this project, the main goals were the following: (1) to assess H3PO4 dechlorination parameters for halide removal from salt simulants, (2) to evaluate crucible compatibility with iron phosphate glass melts, and (3) to evaluate waste form properties within a ternary system of P2O5 (added as H3PO4), Fe2O3 and fission product simulants.

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Evaluating the Impacts of Reactive Gas (Carbon Dioxide and Oxygen) Ingress on Leaching from Cementitious Waste Forms - 17482

Cementitious materials are currently being used as the waste forms for low-activity waste disposal (Saltstone) at the Savannah River Site. In addition, cementitious materials have been selected as the waste form (Cast Stone) for secondary wastes and are being investigated for use for supplemental low-activity waste treatment (Cast Stone) at the Hanford Site. These materials are subjected to numerous aging and degradation phenomena in the disposal environment that potentially impact their long-term durability and performance. One important phenomenon is the ingress of reactive gases (i.e., carbon dioxide and oxygen) that can react with and change the chemistry and pore structure and thus mass transport properties of the waste forms. The reaction of carbon dioxide (i.e., carbonation) reduces the pH of the waste form pore solution impacting the solubility of constituents of potential concern (COPCs). In Cast Stone and Saltstone, the reaction of oxygen (i.e., oxidation) impacts the solubility of redox-sensitive COPCs, notably the technetium-99 (Tc-99) and chromium. The objective of this research is to experimentally characterize the carbonation and oxidation impacts on chemistry and leaching behavior in cementitious waste forms using experimental techniques including United States Environmental Protection Agency (U.S. EPA) Method 1313 and U.S. EPA Method 1315. Results of experimental characterization will be used to parameterize reactive mass transport models to project leaching under a range of field scenarios in future applications. (authors)

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Evaluating High-Halide Waste Form Options for Salt-Based Nuclear Waste Simulants

In this study, waste forms were being explored for an electrochemical salt simulant, , referred to as ERV3, which is a high-LiCl/KCl salt containing simulated fission products (i.e., Sr, Cs, Nd) and Na to represent bond sodium from Experimental Breeder Reactor-II metallic fast reactor fuel. The goal was to find glassy systems that could be used to immobilize the salt in a single-step process. The envisionment of this process would be find a frit glass that could be added to the salt waste, heat treated, poured into waste canisters, and then stored for disposal. To perform this study, a literature review was conducted, the most promising seven systems were fabricated without the salt, and then mixed with salt simulant and heat treated under different processes. The criteria that were used to screen potential compositions included demonstrated alkali incorporation, could be melted at reasonably low temperature ( T ≤ 1000°C), and if the compositions had some demonstrated data for waste-form-related properties, that was a benefit. High marks were given for compositions that showed amorphous nature after slow cooling of samples containing ERV3.

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Updated Liquid Secondary Waste Grout Formulation and Preliminary Waste Form Qualification

This report describes the results from liquid secondary waste grout (LSWG) formulation and cementitious waste form qualification tests performed by Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions, LLC (WRPS). New formulations for preparing a cementitious waste form from a high-sulfate liquid secondary waste stream simulant, developed for Effluent Management Facility (EMF) process condensates merged with low activity waste (LAW) caustic scrubber, and the release of key constituents (e.g. 99 Tc and 129 I) from these monoliths were evaluated. This work supports a technology development program to address the technology needs for Hanford Site Effluent Treatment Facility (ETF) liquid secondary waste (LSW) solidification and supports future Direct Feed Low-Activity Waste (DFLAW) operations. High-priority activities included simulant development, LSWG formulation, and waste form qualification. The work contained within this report relates to waste form development and testing and does not directly support the 2017 integrated disposal facility (IDF) performance assessment (PA). However, this work contains valuable information for use in PA maintenance past FY17, and for future waste form development efforts. The provided data should be used by (i) cementitious waste form scientists to further understanding of cementitious dissolution behavior, (ii) IDF PA modelers who use quantified constituent leachability, effective diffusivity, and partitioning coefficients to advance PA modeling efforts, and (iii) the U.S. Department of Energy (DOE) contractors and decision makers as they assess the IDF PA program. The results obtained help fill existing data gaps, support final selection of a LSWG waste form, and improve the technical defensibility of long-term waste form performance estimates.

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