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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

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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DOE OSTI2022

Impact of carbonation on leaching of constituents from a cementitious waste form for treatment of low activity waste at the DOE Hanford site

Carbonation can be a major aging process during disposal of alkaline cementitious waste forms and can impact constituent leaching by changes in material alkalinity, pore structure, and controlling mineral phases. The effect of carbonation on the leaching of major and trace constituents from Cast Stone, a cementitious waste form developed to treat high salt content low activity waste, was studied through a combination of leaching experiments and reactive transport simulations. Diffusive transport of constituents in the waste form was evaluated using reactive transport modeling of diffusion-controlled leaching test results and a geochemical speciation model derived from pH-dependent leaching. Comparisons between Cast Stone materials aged under nitrogen, air, and 2% carbon dioxide in nitrogen showed that carbonation impacts solubility, physical retention and observed diffusivity of major and trace constituents. Carbonation under 2% CO 2 decreased the diffusion-controlled leaching of chromium by two orders of magnitude. Finally, modeling results suggest that carbonation may also decrease solubility of technetium while changes to microstructure by carbonation increases effective diffusivity of constituents in Cast Stone.

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DOE OSTI2017

The Effect of Ettringite on Cementitious Waste Form Development for Low- Activity Waste - 17170

The current Cast Stone formulation, with 8% ordinary Portland cement (OPC), 45% fly ash (FA), and 47% blast furnace slag (BFS), proposed for cementitious waste forms (CWFs) at the Hanford site has been shown to be inadequate for secondary liquid wastes sent to the Effluent Treatment Facility (ETF). This is due to the high sulfate concentrations and non-alkaline conditions present in the ETF waste stream that lead to the late formation of ettringite, [Ca{sub 6}Al{sub 2}(SO{sub 4}){sub 3}(OH){sub 12}.26(H{sub 2}O)], which can consequently cause undesirable swelling and cracks in the CWF that facilitate {sup 99}Tc release. To overcome this challenge, hydrated lime (HL), Ca(OH){sub 2}, can be used instead of FA to provide the Ca necessary to sequester sulfate early in the cast stone curing process through early formation of ettringite. Early ettringite formation minimizes the risk of localized disruptive action or harmful stress that lead to undesirable swelling and cracking of the CWF. Furthermore, early formation reduces the permeability of the CWF, further reducing the risk of {sup 99}Tc release and increasing structural stability. Two liquid waste simulants, 1) WTP off-gas condensate (WTP) and 2) Effluent Management Facility (EMF) process condensate combined with low activity waste (LAW) caustic scrubber (labeled EMF/CS), were prepared and tested for ettringite formation effects on HL-containing CWF development and {sup 99}Tc leachability. After curing for 28 days, X-ray diffraction analysis revealed that ettringite was formed in the early stages of curing for the CWFs prepared using both simulants. However, because of the higher sulfate concentration in the EMF/CS simulant and limited Ca and Al sources, some sulfate did not form ettringite during the early stages of curing, resulting in significant monolith swelling and cracking during subsequent leaching tests. Despite observable cracking in monoliths prepared with the EMF/CS simulant, low {sup 99}Tc release from HL-based waste forms was measured in later leaching periods tested by the EPA Method 1315 in both simulants. Ettringite-{sup 99}Tc co-precipitation batch experiments support a possible chemical sequestration mechanism that is hypothesized to contribute to the observed low {sup 99}Tc leach rates, which are likely the result of an additional chemical reaction that sequesters {sup 99}Tc rather than simply physical factors such as reduced porosity and permeability (or tortuosity). Overall these findings quantitatively support the use of HL to overcome the deleterious effects of sulfate-rich conditions on CWFs through early formation of ettringite and provide evidence for {sup 99}Tc release rates that fall within low risk levels reported by the United States Department of Energy (US DOE). (authors)

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DOE OSTI2013

Glass-Ceramic Waste Forms for Uranium and Plutonium Residues Wastes - 13164

A program of work has been undertaken to treat plutonium-residues wastes at Sellafield. These have arisen from past fuel development work and are highly variable in both physical and chemical composition. The principal radiological elements present are U and Pu, with small amounts of Th. The waste packages contain Pu in amounts that are too low to be economically recycled as fuel and too high to be disposed of as lower level Pu contaminated material. NNL and ANSTO have developed full-ceramic and glass-ceramic waste forms in which hot-isostatic pressing is used as the consolidation step to safely immobilize the waste into a form suitable for long-term disposition. We discuss development work on the glass-ceramic developed for impure waste streams, in particular the effect of variations in the waste feed chemistry glass-ceramic. The waste chemistry was categorized into actinides, impurity cations, glass formers and anions. Variations of the relative amounts of these on the properties and chemistry of the waste form were investigated and the waste form was found to be largely unaffected by these changes. This work mainly discusses the initial trials with Th and U. Later trials with larger variations and work with Pu-doped samples further confirmed the flexibility of the glass-ceramic. (authors)

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DOE OSTI2017

Corrosion Behavior and Microstructure Influence of Glass-Ceramic Nuclear Waste Forms

Glass ceramic waste forms present a potentially viable technology for the long term immobilization and disposal of liquid nuclear wastes. Through control of chemistry during fabrication, such waste forms can have designed secondary crystalline phases within a borosilicate glass matrix. In this work, a glass ceramic containing powellite and oxyapatite secondary phases was tested for its corrosion properties in dilute conditions using single pass flow through testing (SPFT). Three glass ceramic samples were prepared using different cooling rates to produce samples with varying microstructure sizes. In testing at 90 °C in buffered pH 7 and pH 9 solutions, it was found that increasing pH and decreasing microstructure size (resulting from rapid cooling during fabrication) both led to a reduction in overall corrosion rate. The phases of the glass ceramic were found, using a combination of solutions analysis, SEM and AFM, to corrode preferably in the order of powellite > bulk glass matrix > oxyapatite.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2015

Impact of Zr Content on Radionuclide Release Rates in Metal Waste Forms

Reference alloy waste forms (RAW) underwent hybrid corrosion/immersion testing to parameterize the ANL analytical oxidative-dissolution model to enable the calculation of fractional release rates. The waste forms tested at SRNL were variations of the RAW-3 formulation that uses HT9 as the main alloy component, and are meant to enable evaluation of the impact of Zr:U ratio on the release rates of actinides and Tc-99. The test solutions were air saturated alkaline and acidic brines, representing potential repositories with those conditions. The testing approach consisted of 4 major steps; 1) bare surface corrosion measurements, 2) hybrid potentiostatic hold/exposure measurements, 3) measurement of radionuclide concentrations and relations to anodic current from potentiostatic holds, and 4) identification of corroding phases using SEM/EDS of electrodes.

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DOE OSTI2015

Densified waste form and method for forming

Materials and methods of making densified waste forms for temperature sensitive waste material, such as nuclear waste, formed with low temperature processing using metallic powder that forms the matrix that encapsulates the temperature sensitive waste material. The densified waste form includes a temperature sensitive waste material in a physically densified matrix, the matrix is a compacted metallic powder. The method for forming the densified waste form includes mixing a metallic powder and a temperature sensitive waste material to form a waste form precursor. The waste form precursor is compacted with sufficient pressure to densify the waste precursor and encapsulate the temperature sensitive waste material in a physically densified matrix.

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DOE OSTI2016

Densified waste form and method for forming

Materials and methods of making densified waste forms for temperature sensitive waste material, such as nuclear waste, formed with low temperature processing using metallic powder that forms the matrix that encapsulates the temperature sensitive waste material. The densified waste form includes a temperature sensitive waste material in a physically densified matrix, the matrix is a compacted metallic powder. The method for forming the densified waste form includes mixing a metallic powder and a temperature sensitive waste material to form a waste form precursor. The waste form precursor is compacted with sufficient pressure to densify the waste precursor and encapsulate the temperature sensitive waste material in a physically densified matrix.

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DOE OSTI2012

Secondary Waste Cast Stone Waste Form Qualification Testing Plan (Rev.1)

The Hanford Tank Waste Treatment and Immobilization Plant (WTP) is being constructed to treat the 56 million gallons of radioactive waste stored in 177 underground tanks at the Hanford Site. The WTP includes a pretreatment facility to separate the wastes into high-level waste (HLW) and low-activity waste (LAW) fractions for vitrification and disposal. The LAW will be converted to glass for final disposal at the Integrated Disposal Facility (IDF). Cast Stone – a cementitious waste form, has been selected for solidification of this secondary waste stream after treatment in the ETF. The secondary-waste Cast Stone waste form must be acceptable for disposal in the IDF. This secondary waste Cast Stone waste form qualification testing plan outlines the testing of the waste form and immobilization process to demonstrate that the Cast Stone waste form can comply with the disposal requirements. Specifications for the secondary-waste Cast Stone waste form have not been established. For this testing plan, Cast Stone specifications are derived from specifications for the immobilized LAW glass in the WTP contract, the waste acceptance criteria for the IDF, and the waste acceptance criteria in the IDF Permit issued by the State of Washington. This testing plan outlines the testing needed to demonstrate that the waste form can comply with these waste form specifications and acceptance criteria. The testing program must also demonstrate that the immobilization process can be controlled to consistently provide an acceptable waste form product. This testing plan also outlines the testing needed to provide the technical basis for understanding the long-term performance of the waste form in the disposal environment. These waste form performance data are needed to support performance assessment analyses of the long-term environmental impact of the secondary-waste Cast Stone waste form in the IDF

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DOE OSTI2024

Glass-bonded ceramic waste forms for immobilization of radioiodine from caustic scrubber wastes

Glass-bonded sodalite composite waste forms have been developed for the immobilization of liquid radioactive wastes resulting from off-gas treatment during aqueous reprocessing of used nuclear fuel, with a particular focus on 129I. The proposed composite waste form is comprised of aluminosilicate ceramic phases containing volatile radionuclides bonded with a glassy matrix. In this work, a suite of ten candidate low-temperature glass binders (ZnO-Bi2O3-based glasses and a Na2O-B2O3-SiO2 glass) were examined. Six glasses were mixed with caustic scrubber waste simulant previously converted into a sodalite-rich material (to provide glass fractions of 10 and 20 wt.%), uniaxially pressed into pellets, and sintered at 350 °C or 550 °C for 8 h in air. Iodine retention after heat treatment was assessed by neutron activation analysis, showing retention of 67-100 % of expected iodine. The aqueous durabilities of the resulting materials were then determined, following the ASTM C1308 standard test, showing iodine releases of 1 to 23 g m-2 after 4 d. The cumulative iodine release for the best performing system (a zinc-bismuth-borate glass binder) was <1 g m-2, and its iodine retention from processing was 67 %. The iodine releases compared favorably with other waste forms. In parallel, this best-performing composition was also consolidated via hot isostatic pressing (HIP) in a stainless-steel canister at 550 °C for 2 h under 100 MPa pressure. The HIPed sample was produced at the ~20 g scale and showed improved densification and minimal reaction with the canister.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Waste Form Development for Solidification of Liquid Secondary Wastes to Support Hanford Direct Feed Low Activity Waste Vitrification - 17484

The US Department of Energy/Office of River Protection DOE/ORP has funded a program led by Washington River Protection Solutions (WRPS) to develop and test cementitious waste forms for immobilization of liquid secondary waste (LSW) at the Hanford site in Southeastern Washington State. The LSW comprises a concentrated brine from processing liquid effluents at Hanford's Effluent Treatment Facility. The liquid effluents include condensates from the 242-A tank waste evaporator and future offgas condensates from the Low Activity Waste (LAW) Vitrification Facility. To facilitate waste form formulation development and testing, WRPS developed LSW simulants and engaged subject matter experts at the Savannah River National Laboratory (SRNL) and Pacific Northwest National Laboratory (PNNL). This paper describes results of recent work done to develop and test a grout formulation tailored to address the elevated sulfate levels in Hanford LSW. (authors)

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DOE OSTI2018

Waste form evaluation for RECl 3 and REO x fission products separated from used electrochemical salt

The work presented here is based off the concept that the rare earth chloride (RECl3) fission products mixture within the used electrorefiner (ER) salt can be selectively removed as RECl3 (not yet demonstrated) or precipitated out as REOCl through oxygen sparging (has been demonstrated). This paper presents data showing the feasibility of immobilizing a mixture of RECl3’s at 10 mass% into a TeO2-PbO glass and it shows that this same mixture of RECl3’s can be oxidized to REOCl at 300°C and then to REOx by 1200°C. When the REOx mixture is heated at temperatures >1200°C, the ratios of REOx’s change. The mixture of REOx was then immobilized in a LABS glass at a high loading of 60 mass%. Both the TeO2-PbO glass and LABS glass systems show good chemical durability. The advantages and disadvantages of tellurite and LABS glasses are compared.

Riley, Brian J. (ORCID:0000000277456730)↗
DOE OSTI2011

Waste Acceptance Testing of Secondary Waste Forms: Cast Stone, Ceramicrete and DuraLith

To support the selection of a waste form for the liquid secondary wastes from WTP, Washington River Protection Solutions has initiated secondary-waste-form testing work at Pacific Northwest National Laboratory (PNNL). In anticipation of a down-selection process for a waste form for the Solidification Treatment Unit to be added to the ETF, PNNL is conducting tests on four candidate waste forms to evaluate their ability to meet potential waste acceptance criteria for immobilized secondary wastes that would be placed in the IDF. All three waste forms demonstrated compressive strengths above the minimum 3.45 MPa (500 psi) set as a target for cement-based waste forms. Further, none of the waste forms showed any significant degradation in compressive strength after undergoing thermal cycling (30 cycles in a 10 day period) between -40 C and 60 C or water immersion for 90 days. The three leach test methods are intended to measure the diffusion rates of contaminants from the waste forms. Results are reported in terms of diffusion coefficients and a leachability index (LI) calculated based on the diffusion coefficients. A smaller diffusion coefficient and a larger LI are desired. The NRC, in its Waste Form Technical Position (NRC 1991), provides recommendations and guidance regarding methods to demonstrate waste stability for land disposal of radioactive waste. Included is a recommendation to conduct leach tests using the ANS 16.1 method. The resulting leachability index (LI) should be greater than 6.0. For Hanford secondary wastes, the LI > 6.0 criterion applies to sodium leached from the waste form. For technetium and iodine, higher targets of LI > 9 for Tc and LI > 11 for iodine have been set based on early waste-disposal risk and performance assessment analyses. The results of these three leach tests conducted for a total time between 11days (ASTM C1308) to 90 days (ANS 16.1) showed: (1) Technetium diffusivity: ANSI/ANS 16.1, ASTM C1308, and EPA 1315 tests indicated that all the waste forms had leachability indices better than the target LI > 9 for technetium; (2) Rhenium diffusivity: Cast Stone 2M specimens, when tested using EPA 1315 protocol, had leachability indices better than the target LI > 9 for technetium based on rhenium as a surrogate for technetium. All other waste forms tested by ANSI/ANS 16.1, ASTM C1308, and EPA 1315 test methods had leachability indices that were below the target LI > 9 for Tc based on rhenium release. These studies indicated that use of Re(VII) as a surrogate for 99Tc(VII) in low temperature secondary waste forms containing reductants will provide overestimated diffusivity values for 99Tc. Therefore, it is not appropriate to use Re as a surrogate 99Tc in future low temperature waste form studies. (3) Iodine diffusivity: ANSI/ANS 16.1, ASTM C1308, and EPA 1315 tests indicated that the three waste forms had leachability indices that were below the target LI > 11 for iodine. Therefore, it may be necessary to use a more effective sequestering material than silver zeolite used in two of the waste forms (Ceramicrete and DuraLith); (4) Sodium diffusivity: All the waste form specimens tested by the three leach methods (ANSI/ANS 16.1, ASTM C1308, and EPA 1315) exceeded the target LI value of 6; (5) All three leach methods (ANS 16.1, ASTM C1308 and EPA 1315) provided similar 99Tc diffusivity values for both short-time transient diffusivity effects as well as long-term ({approx}90 days) steady diffusivity from each of the three tested waste forms (Cast Stone 2M, Ceramicrete and DuraLith). Therefore, any one of the three methods can be used to determine the contaminant diffusivities from a selected waste form.

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