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DOE OSTI2015

Groundwork for Universal Canister System Development

The mission of the United States Department of Energy’s Office of Environmental Management is to complete the safe cleanup of the environmental legacy brought about from five decades of nuclear weapons development and government-sponsored nuclear energy research. Some of the wastes that that must be managed have been identified as good candidates for disposal in a deep borehole in crystalline rock (SNL 2014a). In particular, wastes that can be disposed of in a small package are good candidates for this disposal concept. A canister-based system that can be used for handling these wastes during the disposition process (i.e., storage, transfers, transportation, and disposal) could facilitate the eventual disposal of these wastes. This report provides information for a program plan for developing specifications regarding a canister-based system that facilitates small waste form packaging and disposal and that is integrated with the overall efforts of the DOE’s Office of Nuclear Energy Used Fuel Disposition Campaign's Deep Borehole Field Test. Wastes to be considered as candidates for the universal canister system include capsules containing cesium and strontium currently stored in pools at the Hanford Site, cesium to be processed using elutable or nonelutable resins at the Hanford Site, and calcine waste from Idaho National Laboratory. The initial emphasis will be on disposal of the cesium and strontium capsules in a deep borehole that has been drilled into crystalline rock. Specifications for a universal canister system are derived from operational, performance, and regulatory requirements for storage, transfers, transportation, and disposal of radioactive waste. Agreements between the Department of Energy and the States of Washington and Idaho, as well as the Deep Borehole Field Test plan provide schedule requirements for development of the universal canister system. Future work includes collaboration with the Hanford Site to move the cesium and strontium capsules into dry storage, collaboration with the Deep Borehole Field Test to develop surface handling and emplacement techniques and to develop the waste package design requirements, developing universal canister system design options and concepts of operations, and developing system analysis tools. Areas in which further research and development are needed include material properties and structural integrity, in-package sorbents and fillers, waste form tolerance to heat and postweld stress relief, waste package impact limiters, sensors, cesium mobility under downhole conditions, and the impact of high pressure and high temperature environment on seals design.

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DOE OSTI2012

An Overview of Project Planning for Hot-Isostatic Pressure Treatment of High-Level Waste Calcine for the Idaho Cleanup Project - 12289

The Calcine Disposition Project is responsible for retrieval, treatment by hot-isostatic pressure, packaging, and disposal of highly radioactive calcine stored at the Idaho Nuclear Technology and Engineering Center at the Idaho National Laboratory Site in southeast Idaho. In the 2009 Amended Record of Decision: Idaho High-Level Waste and Facilities Disposition Final Environmental Impact Statement the Department of Energy documented the selection of hot-isostatic pressure as the technology to treat the calcine. The Record of Decision specifies that the treatment results in a volume-reduced, monolithic waste form suitable for transport outside of Idaho by a target date of December 31, 2035. That target date is specified in the 1995 Idaho Settlement Agreement to treat and prepare the calcine for transport out of Idaho in exchange for allowing storage of Navy spent nuclear fuel at the INL Site. The project is completing the design of the calcine-treatment process and facility to comply with Record of Decision, Settlement Agreement, Idaho Department of Environmental Quality, and Department of Energy requirements. A systems engineering approach is being used to define the project mission and requirements, manage risks, and establish the safety basis for decision making in compliance with DOE O 413.3B, 'Program and Project Management for the Acquisition of Capital Assets'. The approach draws heavily on 'design-for-quality' tools to systematically add quality, predict design reliability, and manage variation in the earliest possible stages of design when it is most efficient. Use of these tools provides a standardized basis for interfacing systems to interact across system boundaries and promotes system integration on a facility-wide basis. A mass and energy model was developed to assist in the design of process equipment, determine material-flow parameters, and estimate process emissions. Data generated from failure modes and effects analysis and reliability, availability, maintainability, and inspectability analysis were incorporated into a time and motion model to validate and verify the capability to complete treatment of the calcine within the required schedule. The Calcine Disposition Project systems engineering approach, including use of industry-proven design-for-quality tools and quantitative assessment techniques, has strengthened the project's design capability to meet its intended mission in a safe, cost-effective, and timely manner. Use of these tools has been particularly helpful to the project in early design planning to manage variation; improve requirements and high-consequence risk management; and more effectively apply alternative, interface, failure mode, RAMI, and time and motion analyses at the earliest possible stages of design when their application is most efficient and cost effective. The project is using these tools to design and develop HIP treatment of highly radioactive calcine to produce a volume-reduced, monolithic waste form with immobilization of hazardous and radioactive constituents. (authors)

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DOE OSTI2021

Annual Status Report (FY 2020): Performance Assessment for the Environmental Restoration Disposal Facility

DOE O 435.1 and DOE M 435.1-1 require that a determination of continued adequacy of the performance assessment (PA) (CP-60089), composite analysis, and disposal authorization statement (DAS) be made annually, and these guidelines must be used to consider the results of data collection and analysis from research, field studies, and monitoring as well as provide the need to update any radioactive waste management basis documents. Beginning in 1996, the Environmental Restoration Disposal Facility (ERDF) started accepting low-level radioactive, hazardous, and mixed wastes generated during cleanup activities at the Hanford Site. ERDF is composed of a series of cells or disposal areas and can accommodate future design expansions as needed. Currently, there are 10 cells. During this reporting period (fiscal year 2020, which extended from October 1, 2019, through September 30, 2020), approximately 3.39E+04 U.S. tons (3.07E+04 metric tons) of waste was disposed at ERDF. From ERDF inception through September 30, 2020, approximately 18.5 million U.S. tons of waste has been disposed at ERDF, which equates to the consumption of approximately 88% of the disposal volume. As a condition of the DAS, disposal operations within ERDF must be in accordance with the waste acceptance criteria (ERDF-00011) that provide specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with DOE M 435.1-1 requirements. The ERDF waste acceptance criteria stipulate that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. There have been no changes to the physical configuration of ERDF or to the waste forms (source, physical form, etc.). No new Unreviewed Disposal Question Screenings or Evaluations have been generated during this reporting period. Therefore, there are no noted impacts to the PA, composite analysis, DAS, or radioactive waste management basis documents resulting from the evaluations and screenings. Sum of fraction analysis shows that the disposed inventory meets both the concentration and inventory threshold requirements. A sum of fractions value is computed for ERDF sensitive radionuclides contributing to the all pathways and air pathway inventory limits. Computed values were 8.85E-02 and 1.78E-01, respectively. The disposed waste inventory remained well under the PA imposed limits. Required monitoring was satisfactorily completed during the fiscal year reporting period (fiscal year 2020). Compliance with performance objectives were met as each of the reported values were well below the established limit. Overall, there are no substantive changes to primary PA assumptions nor changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the DAS is maintained.

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DOE OSTI2016

Heavy ion irradiations on synthetic hollandite-type materials: Ba{sub 1.0}Cs{sub 0.3}A{sub 2.3}Ti{sub 5.7}O{sub 16} (A=Cr, Fe, Al)

The hollandite supergroup of minerals has received considerable attention as a nuclear waste form for immobilization of Cs. The radiation stability of synthetic hollandite-type compounds described generally as Ba{sub 1.0}Cs{sub 0.3}A{sub 2.3}Ti{sub 5.7}O{sub 16} (A=Cr, Fe, Al) were evaluated by heavy ion (Kr) irradiations on polycrystalline single phase materials and multiphase materials incorporating the hollandite phases. Ion irradiation damage effects on these samples were examined using grazing incidence X-ray diffraction (GIXRD) and transmission electron microscopy (TEM). Single phase compounds possess tetragonal structure with space group I4/m. GIXRD and TEM observations revealed that 600 keV Kr irradiation-induced amorphization on single phase hollandites compounds occurred at a fluence between 2.5×10{sup 14} Kr/cm{sup 2} and 5×10{sup 14} Kr/cm{sup 2}. The critical amorphization fluence of single phase hollandite compounds obtained by in situ 1 MeV Kr ion irradiation was around 3.25×10{sup 14} Kr/cm{sup 2}. The hollandite phase exhibited similar amorphization susceptibility under Kr ion irradiation when incorporated into a multiphase system. - Graphical abstract: 600 keV Kr irradiation-induced amorphization on single phase hollandites compounds occurred at a fluence between 2.5×10{sup 14} Kr/cm{sup 2} and 5×10{sup 14} Kr/cm{sup 2}. The hollandite phase exhibited similar amorphization susceptibility under Kr ion irradiation when incorporated into a multiphase system. This is also the first time that the critical amorphization fluence of single phase hollandite compounds were determined at a fluence of around 3.25×10{sup 14} Kr/cm{sup 2} by in situ 1 MeV Kr ion irradiation. Display Omitted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Performance Assessment for the Environmental Restoration Disposal Facility (Annual Status Report FY 2022)

DOE O 435.1 and DOE M 435.1-1 require that a determination of continued adequacy of the performance assessment (PA) (CP-60089), composite analysis (CA), and disposal authorization statement (DAS) be made on an annual basis, and that the determination must consider the results of data collection and analysis from research, field studies, and monitoring as well as the need to update any Radioactive Waste Management Basis (RWMB) documents. Beginning in 1996, the Environmental Restoration Disposal Facility (ERDF) started accepting low-level radioactive, hazardous, and mixed wastes that were generated during cleanup activities at the Hanford Site. ERDF is composed of a series of cells or disposal areas and can accommodate future design expansions as needed. Currently, there are eight cells and two supercells in ERDF. Each supercell is the equivalent of two cells. During this reporting period (fiscal year 2022, extending from October 1, 2021, through September 30, 2022), approximately 8.52E+04 metric tons (9.39E+04 U.S. tons) of waste was disposed at ERDF. From ERDF inception through September 30, 2022, approximately 17.0 million metric tons (18.7 million U.S. tons) of waste has been disposed at ERDF, which equates to consumption of approximately 89.1% of the currently constructed disposal volume. According to the design of ERDF, the facility has the ability to be expanded as needed. As a condition of the DAS, disposal operations within ERDF must be in accordance with the waste acceptance criteria (ERDF-00011) that provide specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with the requirements of DOE M 435-1.1. The ERDF waste acceptance criteria stipulate that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. There have been no changes to the physical configuration of ERDF or to the waste forms (source, physical form, etc.). No new unreviewed disposal question screenings or evaluations have been generated in this reporting period. Therefore, there are no noted impacts to the PA, CA, DAS, or RWMB resulting from the evaluations and screenings. Sum-of-fractions analysis shows that the disposed inventory meets both the concentration and inventory threshold requirements. A sum-of-fractions value is computed for ERDF sensitive radionuclides contributing to the groundwater pathways and the air pathway inventory limits. Computed values were 5.50E-04 and 3.30E-03, respectively. The disposed waste inventory remained well under the PA imposed limits, as shown in Table 4 and Table 5 in the main text of this report. Required monitoring was satisfactorily completed during the fiscal year reporting period. Compliance with performance objectives were met as each of the reported values were well below the established limit. Overall, there are no substantive changes to primary PA assumptions or changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the DAS is maintained.

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DOE OSTI2022

Performance Assessment for the Environmental Restoration Disposal Facility (Annual Status Report FY 2021)

DOE O 435.1 and DOE M 435.1-1 require that a determination of continued adequacy of the performance assessment (PA) (CP-60089), composite analysis (CA), and disposal authorization statement (DAS) be made on an annual basis, and that the determination must consider the results of data collection and analysis from research, field studies, and monitoring as well as the need to update any Radioactive Waste Management Basis (RWMB) documents. Beginning in 1996, the Environmental Disposal Facility (ERDF) started accepting low-level radioactive, hazardous, and mixed wastes that were generated during cleanup activities at the Hanford Site. ERDF is composed of a series of cells or disposal areas and can accommodate future design expansions as needed. Currently, there are eight cells and two supercells in ERDF. Each supercell is the equivalent of two cells. During this reporting period (fiscal year 2021, extending from October 1, 2020, through September 30, 2021), approximately 9.14E+04 metric tons (1.01E+05 U.S. tons) of waste was disposed at ERDF. From ERDF inception through September 30, 2021, approximately 16.9 million metric tons (18.9 U.S. tons) of waste has been disposed of at ERDF, which equates to consumption of approximately 88.7% of the currently constructed disposal volume. According to the design of ERDF, the facility has the ability to be expanded as needed. As a condition of the DAS, disposal operation within ERDF must be in accordance with the waste acceptance criteria (ERDF-00011) that provide specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with the requirements of DOE M 435-1.1. The ERDF waste acceptance criteria stipulate that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. There have been no changes to the physical configuration of ERDF or to the waste forms (source, physical form, etc.). No new unreviewed disposal question screenings or evaluations have been generated in this reporting period. Therefore, there are no noted impacts to the PA, CA, DAS, or RWMB resulting from the evaluations and screenings. Sum-of-fractions analysis shows that the disposed inventory meets both the concentration and inventory threshold requirements. A sum-of-fractions value is computed for ERDF sensitive radionuclides contributing to the all pathways and the air pathway inventory limits. Computed values were 7.63E-03 and 1.49E-03, respectively. The disposed waste inventory remained well under the PA imposed limits, as shown in Table 4 and Table 5 in the main text of this report. Required monitoring was satisfactorily completed during the fiscal year reporting period. Compliance with performance objectives were met as each of the reported values were well below the established limit. Overall, there are no substantive changes to primary PA assumptions or changes to the PA analysis conclusion; therefore, compliance with DOE O 435.1 and the DAS is maintained.

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DOE OSTI2014

Radionuclide Migration through Sediment and Concrete: 16 Years of Investigations

The Waste Management Project provides safe, compliant, and cost-effective waste management services for the Hanford Site and the U.S. Department of Energy (DOE) complex. Part of these services includes safe disposal of low-level waste and mixed low-level waste at the Hanford Low-Level Waste Burial Grounds in accordance with the requirements of DOE Order 435.1, Radioactive Waste Management. To partially satisfy these requirements, performance assessment analyses were completed and approved. DOE Order 435.1 also requires continuing data collection to increase confidence in the critical assumptions used in these analyses to characterize the operational features of the disposal facility that are relied on to satisfy the performance objectives identified in the order. Cement-based solidification and stabilization is considered for hazardous waste disposal because it is easily done and cost-efficient. One critical assumption is that concrete will be used as a waste form or container material at the Hanford Site to control and minimize the release of radionuclide constituents in waste into the surrounding environment. Concrete encasement would contain and isolate the waste packages from the hydrologic environment and act as an intrusion barrier. Any failure of concrete encasement may result in water intrusion and consequent mobilization of radionuclides from the waste packages. The radionuclides iodine-129, selenium-75, technetium-99, and uranium-238 have been identified as long-term dose contributors (Mann et al. 2001; Wood et al. 1995). Because of their anionic nature in aqueous solutions, these constituents of potential concern may be released from the encased concrete by mass flow and/or diffusion and migrate into the surrounding subsurface environment (Serne et al. 1989; 1992; 1993a, b; 1995). Therefore, it is necessary to assess the performance of the concrete encasement structure and the ability of the surrounding soil to retard radionuclide migration. Each of the test methods performed throughout the lifetime of the project has focused on different aspects of the concrete waste form weathering process. Diffusion of different analytes [technetium-99 (Tc-99), iodine-125 (I-125), stable iodine (I), uranium (U), and rhenium (Re)] has been quantified from experiments under both saturated and unsaturated conditions. The water-saturated conditions provide a conservative estimate of the concrete’s performance in situ, and the unsaturated conditions provide a more accurate estimate of the diffusion of contaminants from the concrete.

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DOE OSTI2016

Summary of Remediated and Unremediated Nitrate Salt Surrogate Testing in Support of the Waste Treatment Permit Application to the New Mexico Environment Department (NMED)

The inadvertent creation of transuranic waste carrying hazardous waste codes D001 and D002 requires the treatment of the material to eliminate the hazardous characteristics and allow its eventual shipment and disposal at the Waste Isolation Pilot Plant (WIPP). This report briefly summarizes the surrogate testing that was done in support of our understanding of this waste form.

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DOE OSTI2021

Organic Iodine Capture from Vessel Off-gas

The Department of Energy (DOE) Nuclear Fuel Cycle and Supply Chain Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has performed research and development on iodine control and iodine waste forms for the past several years. This research and development has included iodine adsorption tests using a laboratory-scale test system containing multiple-segmented fixed beds of iodine adsorbents. Iodine capture performance has been tested using non-radioactive synthetic gas mixtures blended from air, nitrogen, NO, NO2, water, and the target iodine compounds diatomic iodine (I2), representing likely inorganic iodides, and methyl iodide (iodomethane, CH3I) and 1-iodobutane (butyl iodide) a surrogates for potential organic iodides, that could exist in dissolver off-gas (DOG) and vessel off-gas (VOG) streams from used nuclear fuel aqueous reprocessing.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
DOE OSTI2021

Iodine Sorption on AgZ-PAN

The Department of Energy (DOE) Nuclear Fuel Cycle and Supply Chain Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has performed research and development on iodine control and iodine waste forms for the past several years. This research and development has included iodine adsorption tests using a laboratory-scale test system containing multiple-segmented fixed beds of iodine adsorbents. Iodine capture performance has been tested using (a) non-radioactive synthetic gas mixtures blended from air, nitrogen, NO, NO 2 , water, to simulate dissolver off-gas (DOG) and vessel off-gas (VOG) streams from used nuclear fuel aqueous reprocessing, (b) inorganic and organic iodine species, and (c) different sorbents. An initial test of silver-functionalized mordenite in polyacrylonitrile matrix (AgZ-PAN) was conducted to assess if this sorbent, initially designed for selective sorption of Xe that evolves into used fuel reprocessing off-gas streams, could also be a candidate for iodine sorption. This test was conducted using the same deep-bed test system and methodologies used in many prior iodine sorption tests using other sorbents. Diatomic iodine (I2) was used as the target iodide in a gas stream containing air, NO, NO 2 , and moisture designed to simulate an aqueous reprocessing dissolver off-gas (DOG) stream.

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DOE OSTI2012

NRC Consultation and Monitoring at the Savannah River Site: Focusing Reviews of Two Different Disposal Actions - 12181

Section 3116 of the Ronald W. Reagan National Defense Authorization Act for Fiscal Year 2005 (NDAA) requires the U.S. Department of Energy (DOE) to consult with the U.S. Nuclear Regulatory Commission (NRC) for certain non-high level waste determinations. The NDAA also requires NRC to monitor DOE's disposal actions related to those determinations. In Fiscal Year 2011, the NRC staff reviewed DOE performance assessments for tank closure at the F-Tank Farm (FTF) Facility and salt waste disposal at the Saltstone Disposal Facility (SDF) at the Savannah River Site (SRS) as part of consultation and monitoring, respectively. Differences in inventories, waste forms, and key barriers led to different areas of focus in the NRC reviews of these two activities at the SRS. Because of the key role of chemically reducing grouts in both applications, the evaluation of chemical barriers was significant to both reviews. However, radionuclide solubility in precipitated metal oxides is expected to play a significant role in FTF performance whereas release of several key radionuclides from the SDF is controlled by sorption or precipitation within the cementitious wasteform itself. Similarly, both reviews included an evaluation of physical barriers to flow, but differences in the physical configurations of the waste led to differences in the reviews. For example, NRC's review of the FTF focused on the modeled degradation of carbon steel tank liners while the staff's review of the SDF performance included a detailed evaluation of the physical degradation of the saltstone wasteform and infiltration-limiting closure cap. Because of the long time periods considered (i.e., tens of thousands of years), the NRC reviews of both facilities included detailed evaluation of the engineered chemical and physical barriers. The NRC staff reviews of residual waste disposal in the FTF and salt waste disposal in the SDF focused on physical barriers to flow and chemical barriers to radionuclide release from the waste. Because the waste inventory and concentration at both sites is sufficient to generate unacceptable doses to an off-site member of the public or inadvertent intruder in the absence of engineered barriers, the NRC staff review focused on the engineering features DOE plans to put in place to limit radionuclide release. At the FTF, DOE expects that peak doses are delayed beyond a 10,000 year performance period by a combination of (1) the flow-limiting effect of the steel tank liner and (2) chemical conditions created by the stabilizing grout overlying the waste that limit the solubility of key radionuclides for tens of thousands of years. At the SDF, DOE expects that flow will be significantly limited by water shedding along the closure cap lower drainage layer and that radionuclide release will be further limited by radionuclide precipitation or sorption within the high pH, chemically reducing conditions created within the saltstone waste form. Because the performance of both facilities depends on the performance of engineered barriers for thousands of years, the reviews included a detailed evaluation of the expected long-term behavior of these barriers. As previously discussed, NRC staff reviews of DOE waste determinations during consultation are designed to evaluate the three NDAA criteria, whereas the review of an updated PA during monitoring only addresses whether the NRC staff has reasonable assurance that the planned disposal action will meet the performance objectives of 10 CFR Part 61. The NRC staff review of the Waste Determination for the FTF did not include conclusions about whether the planned disposal of residual waste at the FTF would meet the NDAA criteria because of the substantial uncertainties in the degree of waste removal DOE would achieve and other technical uncertainties. The main product of the NRC staff review of the planned FTF disposal action is the recommendation that DOE should conduct waste release experiments to increase support for key modeling assumptions related to: (1) the evolution of pH and Eh in the grouted tank system over time; (2) identification of HRR association with solid phases comprising the residual wastes; and (3) expected solubility of HRRs under a range of environmental or service conditions that the residual wastes in the contaminated zone are expected to be exposed to over time. Implementation of this recommendation is deemed crucial for NRC staff to have reasonable assurance that the performance objectives in 10 CFR Part 61, Subpart C can be met. Given the risk-significance of Tank 18 to the overall PA and the short timeline for closure of this tank, the NRC staff recommended that DOE should initiate discussions with NRC staff regarding implementation of this recommendation for Tank 18 as soon as practical. The NRC staff also recommended that experiments to address this recommendation should be conducted prior to final closure of Tank 18. Results of the Tank 18 residual waste experiments, if conducted, will be evaluated by NRC staff to determine the need for additional data collection, experiments, and modeling for Tank 18, as well as other FTF tanks. Additional information regarding the NRC staff's recommendations in this area, including details on the suggested implementation of other recommendations will be provided in the NRC staff's plan for monitoring the FTF later in FY 2012, after DOE makes a final decision on the waste determination. The NRC staff's review of waste disposal at the SDF is ongoing. When complete, the SDF TER will indicate whether the NRC staff continues to have reasonable assurance that waste disposal at the SDF will meet the performance objectives of 10 CFR Part 61 (NDAA Criterion 3). The TER also will include risk insights that will form the basis of the NRC staff's revised monitoring plan for the SDF. The NRC staff will publish an updated monitoring plan for the SDF later in FY 2012. (authors)

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DOE OSTI2026

Modeling glass degradation and release of radionuclides from vitrified waste for performance assessment simulations

The release of radionuclides initially encapsulated in a slowly degrading solid waste form and contained in an eventually corroding canister defines the source term for numerical simulations for the assessment of a geologic repository for high-level radioactive waste. While the details of waste degradation, canister corrosion, and dissolution and mobilization of the radionuclides in pore water include complex chemical reaction and transport processes that are coupled to the thermal, hydrological, microbiological, and mechanical conditions in the repository, the source-term model suitable for use in a numerical performance assessment model should be a defensible abstraction of these mechanisms. We developed a radiological source-term model and implemented it into a non-isothermal flow and transport simulator. While the proposed source-term model is applicable to various waste forms, canister systems, and disposal concepts, we specifically considered radionuclide releases from vitrified high-level waste placed in a cylindrical canister disposed in a deep vertical borehole repository. In this model, waste degradation is a function of temperature, and it can be adjusted to evaluate the influence of and propagate uncertainties in pH, passivation reactions, and chemical conditions as well as geometrical factors. The time-dependent, congruent release of safety-relevant radionuclides present in the decaying inventory is then calculated. Finally, the radionuclides are mobilized by diffusive and advective transport according to the thermo-hydraulic conditions prevailing in the near field of the repository, from where they migrate through the geosphere to the accessible environment. We examine the influence of the source-term model’s parameters on performance assessment calculations through sensitivity and uncertainty propagation analyses, identifying influential factors and confirming the upper bound of their impact. These considerations align with the overarching goal of repository design, which is to demonstrate that engineered and natural barriers can collectively delay radionuclide migration for timescales far exceeding human planning, thereby providing multiple, redundant barriers against environmental contamination.

iTOUGH2↗
DOE OSTI2017

The corrosion behavior of technetium metal exposed to aqueous sulfate and chloride solutions

Here, metal waste forms are being studied as possible disposal forms for technetium and other fission products from spent nuclear fuel. As an initial step in assessing the viability of waste forms, technetium corrosion and passivity behavior was assessed across a broad pH spectrum (pH –1 to pH 13). Measurements indicate that the open circuit potential falls into the region of Tc +7 stability, more noble than the region of presumed passivity. Potentiodynamic polarization tests indicate that the Tc samples are not passive. Both electrochemical results and visual inspection suggest the presence of a nonprotective film. The corrosion rate is relatively independent of pH and low, as measured by linear polarization resistance. No evidence of passivity was observed in the Tc +4 region of the potential-pH diagram following in-situ abrasion, suggesting that Tc does not passivate, regardless of potential.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Laboratory Evaporation Testing Of Hanford Waste Treatment Plant Low Activity Waste Off-Gas Condensate Simulant

The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream, LAW Off-Gas Condensate, from the off-gas system. The baseline plan for disposition of this stream is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation and recycled to the LAW vitrification facility again. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable de-coupled operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also decrease the LAW vitrification mission duration and quantity of canistered glass waste forms. This LAW Off-Gas Condensate stream contains components that are volatile at melter temperatures and are problematic for the glass waste form. Because this stream recycles within WTP, these components accumulate in the Condensate stream, exacerbating their impact on the number of LAW glass containers that must be produced. Approximately 32% of the sodium in Supplemental LAW comes from glass formers used to make the extra glass to dilute the halides to be within acceptable concentration ranges in the LAW glass. Diverting the stream reduces the halides in the recycled Condensate and is a key outcome of this work. Additionally, under possible scenarios where the LAW vitrification facility commences operation prior to the WTP Pretreatment facility, identifying a disposition path becomes vitally important. This task examines the impact of potential future disposition of this stream in the Hanford tank farms, and investigates auxiliary evaporation to enable another disposition path. Unless an auxiliary evaporator is used, returning the stream to the tank farms would require evaporation in the 242-A evaporator. This stream is expected to be unusual because it will be very high in corrosive species that are volatile in the melter (chloride, fluoride, sulfur), will have high ammonia, and will contain carryover particulates of glass-former chemicals. These species have potential to cause corrosion of tanks and equipment, precipitation of solids, release of ammonia gas vapors, and scale in the tank farm evaporator. Routing this stream to the tank farms does not permanently divert it from recycling into the WTP, only temporarily stores it prior to reprocessing. Testing is normally performed to demonstrate acceptable conditions and limits for these compounds in wastes sent to the tank farms. The primary parameter of this phase of the test program was measuring the formation of solids during evaporation in order to assess the compatibility of the stream with the evaporator and transfer and storage equipment. The origin of this LAW Off-Gas Condensate stream will be the liquids from the Submerged Bed Scrubber (SBS) and the Wet Electrostatic Precipitator (WESP) from the LAW facility melter offgas system. The stream is expected to be a dilute salt solution with near neutral pH, and will likely contain some insoluble solids from melter carryover. The soluble components are expected to be mostly sodium and ammonium salts of nitrate, chloride, and fluoride. This stream has not been generated yet, and, thus, the composition will not be available until the WTP begins operation, but a simulant has been produced based on models, calculations, and comparison with pilot-scale tests. This report discusses results of evaporation testing of the simulant. Two conditions were tested, one with the simulant at near neutral pH, and a second at alkaline pH. The neutral pH test is comparable to the conditions in the Hanford Effluent Treatment Facility (ETF) evaporator, although that evaporator operates at near atmospheric pressure and tests were done under vacuum. For the alkaline test, the target pH was based on the tank farm corrosion control program requirements, and the test protocol and equipment was comparable to that used for routine evaluation of feed compatibility studies for the 242-A evaporator. One of the radionuclides that is volatile in the melter and expected to be in high concentration in this LAW Off-Gas Condensate stream is Technetium-99 (99Tc). Technetium will not be removed from the aqueous waste in the Hanford WTP, and will primarily end up immobilized in the LAW glass by repeated recycle of the off-gas condensate into the LAW melter. Other radionuclides that are also expected to be in appreciable concentrations in the LAW Off-Gas Condensate are 129I, 90Sr, 137Cs, and 241Am. The concentrations of these radionuclides in this stream will be much lower than in the LAW, but they will still be higher than limits for some of the other disposition pathways currently available. At this time, these scoping tests did not evaluate the partitioning of the radionuclides to the evaporator condensate, since ample data are available separately from other experience in the DOE complex. Results from the evaporation testing show that the neutral SBS simulant first forms turbidity at ~7.5X concentration, while the alkaline-adjusted simulant became turbid at ~3X concentration. The major solid in both cases was Kogarkoite, Na3FSO4. Sodium and lithium fluorides were also detected. Minimal solids were formed in the evaporator bottoms until a substantial fraction of liquid was removed, indicating that evaporation could minimize storage volume issues. Achievable concentration factors without significant insoluble solids were 17X at alkaline pH, and 23X at neutral pH. In both runs, significant ammonia carried over and was captured in the condenser with the water condensate. Results also indicate that with low insoluble solids formation in the initial testing at neutral pH, the use of Reverse Osmosis is a potential alternate method for concentrating the solution, although an evaluation is needed to identify equipment that can tolerate insoluble solids. Most of the ammonia remains in the evaporator bottoms during the neutral pH evaporation, but partitions to the condensate during alkaline evaporation. Disposition of both streams needs to consider the management of ammonia vapor and its release. Since this is an initial phase of testing, additional tasks related to evaporation methods are expected to be identified for development. These tasks likely include evaluation and testing of composition variability testing and evaluations, corrosion and erosion testing, slurry storage and immobilization investigations, and evaporator condensate disposition.

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DOE OSTI2020

PORFLOW Implementation of Special Waste from Models for Slit and Engineered Trenches in the E-Area Low Level Waste Facility Performance Assessment

The implementation of special waste forms (SWFs) in the deterministic PORFLOW Slit Trench (ST) and Engineered Trench (ET) models to be used in the next revision of the E-Area Low Level Waste Facility’s (ELLWFs) Performance Assessment (PA) is outlined in this report. Four SWF implementation methods will be used: effective K d , delayed release, solubility-controlled/diffusion-controlled release, and complex SWF model updates. In addition, the implementation of models that address the presence of tall used equipment storage boxes in ST08-10 is considered a special waste form and will be described.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

A Critical Review of Ion Exchange in Nuclear Waste Glasses to Support the Immobilized Low-Activity Waste Integrated Disposal Facility Rate Model

There are over 50 million gallons of waste in underground tanks at the Hanford site in Washington State which was generated as a byproduct of nuclear materials fabrication for United States strategic defensive purposes. The waste, also known as high-level waste (HLW), is comprised of both radioactive and non-radioactive contaminants. To deal with the tank waste, the United States Department of Energy (DOE) plans to separate out the liquid, or supernatant, and salt-cake portions and treat them as low-activity waste (LAW). The LAW and HLW will be vitrified in separate facilities at the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The LAW will be disposed of at the on-site Integrated Disposal Facility (IDF). The main species of concern in the immobilized low-activity waste (ILAW) include 99 Tc, 129 I, and U and other non-radioactive contaminants. Ultimately, it must be demonstrated that the contaminants released from the waste form pose minimal risk to humans and the environment. To aid in this demonstration, work is currently being done to expand the understanding of long-term glass waste form behavior, especially with regards to exposure to aqueous environments.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2012

'Radiotoxicity Index': An Inappropriate Discriminator for Advanced Fuel Cycle Technology Selection - 12276

A radiotoxicity index (RI) is often used as a figure of merit for evaluating for evaluating the attractiveness of employing an advanced fuel cycle (i.e., a fuel cycle that uses some combination of separations and other reactor technologies, such as fast reactors), rather than continued use of the current 'once-through' fuel cycle. The RI is calculated by multiplying the amount of every radionuclide found in a waste form for some unit amount of waste times the drinking water dose conversion factor, DCF, for each radionuclide, then summing these together. Some argue that if the RI for an advanced fuel cycle is lower than the RI for a once-through fuel cycle, then implementation of the particular advanced fuel cycle has merit because it reduces the radiotoxicity of the waste. Use of an RI for justifying separations technologies and other components of advanced fuel cycles is not only inappropriate, but can be misleading with respect to judging benefits of advance fuel cycle options. The disposal system, through its use of multiple engineered and natural barriers to migration, eliminates most of the radionuclides contributing to the RI such that additional separations technologies will make little difference to peak dose rates. What must also be considered is the health/dose risk caused to workers and the public by the construction and operation of the separations facility itself. Thus, use of RI may lead to selection of separations technologies that may have a negligible effect on lowering the potential health risks associated with disposal, but will increase real worker and public health risks in the near term. The use of the radiotoxicity index (RI) as a figure of merit for justifying advanced fuel cycles involving separations technologies is not only inappropriate, but can be misleading with respect to judging benefits of advance fuel cycle options. The disposal system, through its use of multiple engineered and natural barriers to migration, eliminates most of the radionuclides contributing to the RI such that additional separations technologies will make little difference to peak dose rates. What must also be considered is the health/dose risk caused to workers and the public by the construction and operation of the separations facility itself. Thus, use of RI may lead to selection of separations technologies that may have a negligible effect on lowering the potential health risks associated with disposal, but will increase real worker and public health risks in the near term. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗