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DOE OSTI2013

GeoMelt{sup R} ICV{sup TM} Treatment of Sellafield Pond Solids Waste - 13414

Kurion, Inc., in partnership with AMEC Ltd., is demonstrating its GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} Technology to Sellafield Ltd. (SL). SL is evaluating the proposition of directly converting a container (skip/box/drum) of raw solid ILW into an immobilized waste form using thermal treatment, such that the resulting product is suitable for interim storage at Sellafield and subsequent disposal at a future Geological Disposal Facility. Potential SL feed streams include sludges, ion-exchange media, sand, plutonium contaminated material, concrete, uranium, fuel cladding, soils, metals, and decommissioning wastes. The solid wastes have significant proportions of metallic constituents in the form of containers, plant equipment, structural material and swarf arising from the nuclear operations at Sellafield. GeoMelt's proprietary ICV process was selected for demonstration, with the focus being high and reactive metal wastes arising from solid ILW material. A composite surrogate recipe was used to demonstrate the technology towards treating waste forms of diverse types and shapes, as well as those considered difficult to process; all the while requiring few (if any) pre-treatment activities. Key strategic objectives, along with their success criterion, were established by SL for this testing, namely: 1. Passivate and stabilize the raw waste simulant, as demonstrated by the entire quantity of material being vitrified, 2. Immobilize the radiological and chemo-toxic species, as demonstrated via indicative mass balance using elemental analyses from an array of samples, 3. Production of an inert and durable product as evidenced by transformation of reactive metals to their inert oxide forms and satisfactory leachability results using PCT testing. Two tests were performed using the GeoMelt Demonstration Unit located at AMEC's Birchwood Park Facilities in the UK. Post-melt examination of the first test indicated some of the waste simulant had not fully processed, due to insufficient processing time and melt temperature. A second test, incorporating operational experience from the first test, was performed and resulted in all of the 138 kg of feed material being treated. The waste simulant portion, at 41 kg, constituted 30 wt% of the total feed mass, with over 90% of this being made up of various reactive and non-reactive metals. The 95 liters of staged material was volume reduced to 41 liters, providing a 57% overall feed to product volume reduction in a fully passivated two-phase glass/metal product. The GeoMelt equipment operated as designed, vitrifying the entire batch of waste simulant. Post-melt analytical testing verified that 91-99+% of the radiological tracer metals were uniformly distributed within the glass/cast refractory/metal product, and the remaining fraction was captured in the offgas filtration systems. PCT testing of the glass and inner refractory liner showed leachability results that outperform the DOE regulatory limit of 2 g/m{sup 2} for the radiological species of interest (Sr, Ru, Cs, Eu, Re), and by more than an order of magnitude better for standard reference analytes (B, Na, Si). (authors)

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DOE OSTI2012

Interstitial and substitutional zirconium in SrTiO3

We investigate Zr in SrTiO3 (STO) as a model for nuclear waste forms in which the fission product Sr90 eventually decays to stable Zr through beta emission. The transformation of a divalent into a tetravalent constituent is expected to affect the long-term structural and chemical stability of this solid. Computational methods of electronic structure theory, specifically the density functional theory (DFT) within the supercell model, are used to predict the thermodynamic stability and electronic states of interstitial and Sr- or Ti-substituted Zr atoms in the STO lattice. Native defects such as vacancies and antisites are also considered. When Zr replaces Sr, its most stable configuration is to simply occupy the Sr site (instead of, for example, replacing a Ti and displacing the Ti to the Sr site.) For Zr added to the lattice, its most stable configuration is to replace a Ti, making a ZrTi impurity plus a Ti interstitial (as opposed to the Zr just remaining as an interstitial atom.) ZrSr is predicted to be a double electron donor, ZrTi is electrically inactive and interstitial Zr and Ti are predicted to be quadruple donors, with all donor levels in the conduction band. ZrSr and the tetravalent interstitials are all predicted to increase the crystal volume, and the interstitials also are predicted to lead to a tetragonal distortion of the lattice. Experiments with injection of Zr atoms into STO qualitatively confirm these predictions of crystal structural changes.

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DOE OSTI2019

Annual Status Report (FY 2018): 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), composite analysis, and disposal authorization statement be made on an annual basis, and it must consider the results of data collection and analysis from research, field studies, and monitoring. 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 10 cells. During this reporting period (fiscal year 2018, which extends from October 1, 2017, through September 30, 2018), approximately 193,358 U.S. tons of waste was disposed at ERDF. From ERDF inception through September 30, 2018, approximately 18.3 million U.S. tons of waste had been disposed at ERDF, which equates to consumption of approximately 87% of the disposal volume. As a condition of the Disoposal Authorization Statement, disposal operations within ERDF must be in accordance with the waste acceptance criteria (WAC) that provides specific radionuclide disposal limits, waste form restrictions, and descriptions of acceptable waste packages in compliance with the requirements of DOE 435-1.1. The ERDF WAC stipulates that waste destined for disposal at ERDF be controlled based on source, physical form, and contaminant concentration and activity levels. Concentration limits included in the ERDF WAC were extracted from the ERDF PA. A sum of fraction analysis of of the ERDF inventory against the threshold concentration limits from inception through fiscal year 2018 produces a result <1. This result provides confirmation of compliance with PA imposed radionuclide limits.

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DOE OSTI2013

Treatment of Bottled Liquid Waste During Remediation of the Hanford 618-10 Burial Ground - 13001

A problematic waste form encountered during remediation of the Hanford Site 618-10 burial ground consists of bottled aqueous waste potentially contaminated with regulated metals. The liquid waste requires stabilization prior to landfill disposal. Prior remediation activities at other Hanford burial grounds resulted in a standard process for sampling and analyzing liquid waste using manual methods. Due to the highly dispersible characteristics of alpha contamination, and the potential for shock sensitive chemicals, a different method for bottle processing was needed for the 618-10 burial ground. Discussions with the United States Department of Energy (DOE) and United States Environmental Protection Agency (EPA) led to development of a modified approach. The modified approach involves treatment of liquid waste in bottles, up to one gallon per bottle, in a tray or box within the excavation of the remediation site. Bottles are placed in the box, covered with soil and fixative, crushed, and mixed with a Portland cement grout. The potential hazards of the liquid waste preclude sampling prior to treatment. Post treatment verification sampling is performed to demonstrate compliance with land disposal restrictions and disposal facility acceptance criteria. (authors)

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DOE OSTI2012

The Windscale Advanced Gas Cooled Reactor (WAGR) Decommissioning Project A Close Out Report for WAGR Decommissioning Campaigns 1 to 10 - 12474

The reactor core of the Windscale Advanced Gas-Cooled Reactor (WAGR) has been dismantled as part of an ongoing decommissioning project. The WAGR operated until 1981 as a development reactor for the British Commercial Advanced Gas cooled Reactor (CAGR) power programme. Decommissioning began in 1982 with the removal of fuel from the reactor core which was completed in 1983. Subsequently, a significant amount of engineering work was carried out, including removal of equipment external to the reactor and initial manual dismantling operations at the top of the reactor, in preparation for the removal of the reactor core itself. Modification of the facility structure and construction of the waste packaging plant served to provide a waste route for the reactor components. The reactor core was dismantled on a 'top-down' basis in a series of 'campaigns' related to discrete reactor components. This report describes the facility, the modifications undertaken to facilitate its decommissioning and the strategies employed to recognise the successful decommissioning of the reactor. Early decommissioning tasks at the top of the reactor were undertaken manually but the main of the decommissioning tasks were carried remotely, with deployment systems comprising of little more than crane like devices, intelligently interfaced into the existing structure. The tooling deployed from the 3 tonne capacity (3te) hoist consisted either purely mechanical devices or those being electrically controlled from a 'push-button' panel positioned at the operator control stations, there was no degree of autonomy in the 3te hoist or any of the tools deployed from it. Whilst the ATC was able to provide some tele-robotic capabilities these were very limited and required a good degree of driver input which due to the operating philosophy at WAGR was not utilised. The WAGR box proved a successful waste package, adaptable through the use of waste box furniture specific to the waste-forms generated throughout the various decommissioning campaigns. The use of low force compaction for insulation and soft wastes provided a simple, robust and cost effective solution as did the direct encapsulation of LLW steel components in the later stages of reactor decommissioning. Progress through early campaigns was good, often bettering the baseline schedule, especially when undertaking the repetitive tasks seen during Neutron Shield and Graphite Core decommissioning, once the operators had become experienced with the equipment, though delays became more pronounced, mainly as a result of increased failures due to the age and maintainability of the RDM and associated equipment. Extensive delays came about as a result of the unsupported insulation falling away from the pressure vessel during removal and the inability of the ventilation system to manage the sub micron particulate generated during IPOPI cutting operations, though the in house development of revised and new methodologies ultimately led to the successful completion of PV and I removal. In a programme spanning over 12 years, the decommissioning of the reactor pressure vessel and core led to the production 110 ILW and 75 LLW WAGR boxes, with 20 LLW ISO freight containers of primary reactor wastes, resulting in an overall packaged volume of approximately 2500 cubic metres containing the estimated 460 cubic metres of the reactor structure. (authors)

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DOE OSTI2016

The Evolution of Chemical Waste Treatment in the Nuclear Industry Simple Solutions for Complex Problems - 16694

The U.S. nuclear waste treatment industry was born in the 1980s and early 1990s with the end of the Cold War, the peak of commercial nuclear power, and after implementation of federal regulations that drove new disposal requirements for radioactive waste generators. New regulations resulted in soaring costs for radioactive waste disposal, and thus an industry was born that focused on recycling, volume reduction, and waste form improvement. New treatment facilities and technologies were started that primarily dealt with low-level radioactive wastes; however, there was little to no treatment capacity for wastes commingled with hazardous chemicals. Large volumes of 'mixed wastes', of which many became known as 'orphan wastes', were being stored on U.S. Department of Energy (DOE) sites with no path for disposal and thus posed a risk to workers, the public, and the environment. Perma-fix Environmental Services, Inc. (Perma-Fix), which started in the hazardous waste industry in 1990 and had developed facilities and technologies to treat hazardous wastes, evolved in the late 90's to meet this mixed waste market opportunity. By adapting our technologies and collaborating with waste generators to understand their needs, we successfully developed treatment and disposition solutions for some of the most challenging mixed wastes in the U.S. By establishing a pathway for treatment and disposal of orphan wastes, Perma-Fix played an important role in the safe treatment and disposition of orphan wastes, which facilitated closure of DOE sites such as Rocky Flats, Mound, and Fernald. We found that understanding chemistry and having experience in managing the hazardous constituents of mixed wastes allowed us to apply solutions that were not overly complex and expensive. Further, by adapting proven hazardous waste treatment solutions to wastes commingled with contaminants such as polychlorinated biphenyls (PCBs), mercury, and organics we were able to safely manage even more problematic mixed wastes. During the 1980's, commercial low-level radioactive waste treatment and disposal solutions were being developed. At the same time, the federal government began dealing with increasing stakeholder demands for permanent solutions of more complex radioactive wastes such as high-level waste (HLW) and transuranic (TRU) wastes. HLW and TRU waste disposal became a contentious political issue between the federal government, regulatory agencies, and the public. As a result, DOE was mandated to develop treatment and disposal methodologies to address these wastes. DOE's Waste Isolation Pilot Plant (WIPP) facility solved most issues with disposition of TRU wastes; however, for HLW (for example tank wastes at Hanford, Savannah River, and Idaho) the complexity of the wastes and the fact that government entities were developing political solutions for waste treatment resulted in a variety of complex and expensive solutions. Decades later we still do not have a permanent solution for HLW. Whether some simple commercial approaches are possible, what regulatory changes should occur, and what the implications may be if we do not change our current path, will be discussed. After two decades, we see the low-level nuclear waste industry maturing and replicating the path of the hazardous waste industry. When new hazardous waste federal regulations were enacted in the 1970's and 1980's, the hazardous waste industry began to boom with new company start-ups and construction of numerous treatment and disposal facilities. Initially, this was a good business to be in, managing dangerous wastes in an environmentally safe and responsible manner, and it was profitable. However, over-capacity and fierce competition drove down pricing, and companies failed. This ultimately led to a major consolidation within the hazardous waste industry. Similarly and more recently in the nuclear industry, over-capacity and competition has driven down profitability, companies have failed, and there is a major consolidation occurring within sectors of the industry. For consolidation to be successful and healthy for either industry, a leader must emerge to set the direction for the others and establish a sustainable path that is acceptable for waste generators, stakeholders, and investors. This was the case for the hazardous waste industry. This paper will examine the parallels between the hazardous and nuclear waste industries as they have matured and evolved, and what discuss the long term implications of consolidation within the nuclear industry. (authors)

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DOE OSTI2017

Non-pertechnetate Technetium Sensor Research and Development

Several significant uncertainties remain regarding the understanding and modeling of the fate and speciation of technicium-99 ( 99 Tc) in Hanford waste tanks, glass, and low-temperature waste forms. A significant (2% to 25%) fraction of the 99Tc in the water-soluble portion of the tank waste may be present as one or more non pertechnetate species that have not been identified and to date, cannot be effectively separated from the wastes. This task will provide a sensor specifically tuned to detect the Tc(I)-carbonyl species believed to constitute the main fraction of the non-pertechnetate form of technetium. By direct measurement of the non-pertechnetate species, such a sensor will help reduce the uncertainties in the modeling of the fate and speciation of 99 Tc in Hanford tanks and waste forms. This report summarizes work performed in FY2016 that was sponsored by the Department of Energy’s Office of Environmental Management and demonstrates the protocol for using fluorescent Tc(I)-tricarbonyl complex as a means to detect the non-pertechnetate species within tank waste solutions. The protocol was optimized with respect to ligand concentration, solvent choice, reaction temperature and time. This work culminated in the quantitation of Tc(I)-tricarbonyl within a waste simulant, using a standard addition method for measurement. This report also summarizes the synthesis and high-yield preparation of the low-valence technetium species, [Tc(CO) 3 (H 2 O) 3 ] + , which will be used as the technetium standard material for the demonstration of the non-pertechnetate species in actual wastes.

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DOE OSTI2012

A Preliminary Performance Assessment for Salt Disposal of High-Level Nuclear Waste - 12173

A salt repository is one of the four geologic media currently under study by the U.S. DOE Office of Nuclear Energy to support the development of a long-term strategy for geologic disposal of commercial used nuclear fuel (UNF) and high-level radioactive waste (HLW). The immediate goal of the generic salt repository study is to develop the necessary modeling tools to evaluate and improve the understanding of the repository system response and processes relevant to long-term disposal of UNF and HLW in a salt formation. The current phase of this study considers representative geologic settings and features adopted from previous studies for salt repository sites. For the reference scenario, the brine flow rates in the repository and underlying interbeds are very low, and transport of radionuclides in the transport pathways is dominated by diffusion and greatly retarded by sorption on the interbed filling materials. I-129 is the dominant annual dose contributor at the hypothetical accessible environment, but the calculated mean annual dose is negligibly small. For the human intrusion (or disturbed) scenario, the mean mass release rate and mean annual dose histories are very different from those for the reference scenario. Actinides including Pu-239, Pu-242 and Np-237 are major annual dose contributors, and the calculated peak mean annual dose is acceptably low. A performance assessment model for a generic salt repository has been developed incorporating, where applicable, representative geologic settings and features adopted from literature data for salt repository sites. The conceptual model and scenario for radionuclide release and transport from a salt repository were developed utilizing literature data. The salt GDS model was developed in a probabilistic analysis framework. The preliminary performance analysis for demonstration of model capability is for an isothermal condition at the ambient temperature for the near field. The capability demonstration emphasizes key attributes of a salt repository that are potentially important to the long-term safe disposal of UNF and HLW. The analysis presents and discusses the results showing repository responses to different radionuclide release scenarios (undisturbed and human intrusion). For the reference (or nominal or undisturbed) scenario, the brine flow rates in the repository and underlying interbeds are very low, and transport of radionuclides in the transport pathways is dominated by diffusion and greatly retarded by sorption on the interbed filling materials. I-129 (non-sorbing and unlimited solubility with a very long half-life) is the dominant annual dose contributor at the hypothetical accessible environment, but the calculated mean annual dose is negligibly small that there is no meaningful consequence for the repository performance. For the human intrusion (or disturbed) scenario analysis, the mean mass release rate and mean annual dose histories are very different from those for the reference scenario analysis. Compared to the reference scenario, the relative annual dose contributions by soluble, non-sorbing fission products, particularly I-129, are much lower than by actinides including Pu-239, Pu-242 and Np-237. The lower relative mean annual dose contributions by the fission product radionuclides are due to their lower total inventory available for release (i.e., up to five affected waste packages), and the higher mean annual doses by the actinides are the outcome of the direct release of the radionuclides into the overlying aquifer having high water flow rates, thereby resulting in an early arrival of higher concentrations of the radionuclides at the biosphere drinking water well prior to their significant decay. The salt GDS model analysis has also identified the following future recommendations and/or knowledge gaps to improve and enhance the confidence of the future repository performance analysis. - Repository thermal loading by UNF and HLW, and the effect on the engineered barrier and near-field performance. - Closure and consolidation of salt rocks by creep deformation under the influence of thermal perturbation, and the effect on the engineered barrier and near-field performance. - Brine migration and radionuclide transport under the influence of thermal perturbation in generic salt repository environment, and the effect on the engineered barrier and near-field performance and far-field performance. - Near-field geochemistry and radionuclide mobility in generic salt repository environment (high ionic strength brines, elevated temperatures and chemically reducing condition). - Degradation of engineer barrier components (waste package, waste canister, waste forms, etc.) in a generic salt repository environment (high ionic strength brines, elevated temperatures and chemically reducing condition). - Waste stream types and inventory estimates, particularly for reprocessing high-level waste. (authors)

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DOE OSTI2014

Non-Pertechnetate Technetium Sensor Research and Development

There remain several significant uncertainties in the understanding and modeling of the fate and speciation of 99 Tc in Hanford waste tanks, glass, and low-temperature waste forms. A significant (2% to 25%) fraction of the 99 Tc in the water-soluble portion of the tank waste may be present as a non-pertechnetate species that has not been identified and, based on experimentation to date, cannot be effectively separated from the wastes. This task will provide a sensor specifically tuned to detect the Tc(I)-carbonyl species believed to constitute the main fraction of the non-pertechnetate form of technetium. By direct measurement of the non-pertechnetate species, such a sensor will help reduce the uncertainties in the modeling of the fate and speciation of 99 Tc in Hanford tanks and waste forms. This report summarizes work done in FY 2014 exploring the chemistry of a low-valence technetium species, [Tc(CO) 3 (H 2 O) 3 ] + , a compound of interest due to its implication in the speciation of alkaline-soluble technetium in several Hanford tank waste supernatants. Progress made in FY 2014 was sponsored by the Department of Energy’s Office of Environmental Management and is summarized in this report.

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DOE OSTI2013

Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada: Review of the Performance Assessments and Composite Analyses (2012 Annual Summary Report)

The Maintenance Plan for the Performance Assessments and Composite Analyses for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada Test Site (National Security Technologies, LLC 2007a) requires an annual review to assess the adequacy of the performance assessments (PAs) and composite analyses (CAs), with the results submitted to the U.S. Department of Energy (DOE) Office of Environmental Management. The Disposal Authorization Statements for the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) also require that such reviews be made and that secondary or minor unresolved issues be tracked and addressed as part of the maintenance plan (DOE 1999a, 2000). The U.S. Department of Energy, National Nuclear Security Administration Nevada Site Office performed an annual review of the Area 3 and Area 5 RWMS PAs and CAs for fiscal year (FY) 2012. This annual summary report presents data and conclusions from the FY 2012 review, and determines the adequacy of the PAs and CAs. Operational factors (e.g., waste forms and containers, facility design, and waste receipts), closure plans, monitoring results, and research and development (RD) activities were reviewed to determine the adequacy of the PAs. Likewise, the environmental restoration activities at the Nevada National Security Site (NNSS) relevant to the sources of residual radioactive material that are considered in the CAs, the land-use planning, and the results of the environmental monitoring and RD activities were reviewed to determine the adequacy of the CAs. Important developments in FY 2012 include the following: Release of a special analysis for the Area 3 RWMS assessing the continuing validity of the PA and CA; Development of a new Area 5 RWMS closure inventory estimate based on disposals through FY 2012; Evaluation of new or revised waste streams by special analysis; and Development of version 4.114 of the Area 5 RWMS GoldSim PA model. The Area 3 RWMS has been in inactive status since July 1, 2006, with the last shipment received in April 2006. The FY 2012 review of operations, facility design, closure plans, monitoring results, and RD results for the Area 3 RWMS indicates no changes that would impact PA validity. A special analysis using the Area 3 RWMS v2.102 GoldSim PA model was prepared to update the PA results for the Area 3 RWMS in FY 2012. The special analysis concludes that all performance objectives can be met and the Area 3 RWMS PA remains valid. There is no need to the revise the Area 3 RWMS PA. Review of Area 5 RWMS operations, design, closure plans, monitoring results, and RD activities indicates no significant changes other than an increase in the inventory disposed. The FY 2012 PA results, generated with the Area 5 RWMS v4.114 GoldSim PA model, indicate that there continues to be a reasonable expectation of meeting all performance objectives. The results and conclusions of the Area 5 RWMS PA are judged valid, and there is no need to the revise the PA. A review of changes potentially impacting the CAs indicates that no significant changes occurred in FY 2012. The continuing adequacy of the CAs was evaluated with the new models, and no significant changes that would alter CA results or conclusions were found. The revision of the Area 3 RWMS CA, which will include the Underground Test Area source term (Corrective Action Unit [CAU] 97), is scheduled for FY 2024, following the completion of the Yucca Flat CAU 97 Corrective Action Decision Document/Corrective Action Plan in FY 2016. Inclusion of the Frenchman Flat CAU 98 results in the Area 5 RWMS CA is scheduled for FY 2016, pending the completion of the CAU 98 closure report in FY 2015. Near-term RD efforts will focus on continuing development of the Area 3 and Area 5 RWMS GoldSim PA/CA and inventory models.

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DOE OSTI2014

2013 Annual Summary Report for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada: Review of the Performance Assessments and Composite Analyses

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DOE OSTI2016

Chemical analysis of simulated high level waste glasses to support stage III sulfate solubility modeling

The U.S. Department of Energy (DOE), Office of Environmental Management (EM) is sponsoring an international, collaborative project to develop a fundamental model for sulfate solubility in nuclear waste glass. The solubility of sulfate has a significant impact on the achievable waste loading for nuclear waste forms within the DOE complex. These wastes can contain relatively high concentrations of sulfate, which has low solubility in borosilicate glass. This is a significant issue for low-activity waste (LAW) glass and is projected to have a major impact on the Hanford Tank Waste Treatment and Immobilization Plant (WTP). Sulfate solubility has also been a limiting factor for recent high level waste (HLW) sludge processed at the Savannah River Site (SRS) Defense Waste Processing Facility (DWPF). The low solubility of sulfate in glass, along with melter and off-gas corrosion constraints, dictate that the waste be blended with lower sulfate concentration waste sources or washed to remove sulfate prior to vitrification. The development of enhanced borosilicate glass compositions with improved sulfate solubility will allow for higher waste loadings and accelerate mission completion.The objective of the current scope being pursued by SHU is to mature the sulfate solubility model to the point where it can be used to guide glass composition development for DWPF and WTP, allowing for enhanced waste loadings and waste throughput at these facilities. A series of targeted glass compositions was selected to resolve data gaps in the model and is identified as Stage III. SHU fabricated these glasses and sent samples to SRNL for chemical composition analysis. SHU will use the resulting data to enhance the sulfate solubility model and resolve any deficiencies. In this report, SRNL provides chemical analyses for the Stage III, simulated HLW glasses fabricated by SHU in support of the sulfate solubility model development.

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DOE OSTI2018

Final Letter Report on PCT/monolithic Long-Term Glass Ceramic Corrosion Tests M3NT-18SR030105147

The Savannah River National Laboratory (SRNL) is collaborating with the Pacific Northwest National Laboratory (PNNL) to study advanced waste form glass ceramics for immobilization of waste from Used Nuclear Fuel (UNF) separations processes.

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DOE OSTI2016

2015 Annual Summary Report for the Area 3 and Area 5 RWMs

This annual summary report presents results and conclusions of the Fiscal Year (FY) 2015 review to assess the adequacy of the performance assessments (PAs) and composite analyses (CAs) in support of the Disposal Authorization Statements for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site (NNSS). The report presents results and conclusions of the FY 2015 review and determines the adequacy of the PAs and CAs. Operational factors (e.g., waste forms and containers, facility design, and waste receipts), closure plans, monitoring results, and research and development (R&D) activities were reviewed to determine the adequacy of the PAs. Likewise, the environmental restoration activities at the NNSS relevant to the sources of residual radioactive material that are considered in the CAs, the land-use planning, and the results of the environmental monitoring and R&D activities were reviewed to determine the adequacy of the CAs.

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DOE OSTI2017

2016 Annual Summary Report for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada National Security Site, Nye County, Nevada: Review of the Performance Assessments and Composite Analyses

The Maintenance Plan for the Performance Assessments and Composite Analyses for the Area 3 and Area 5 Radioactive Waste Management Sites at the Nevada Test Site (National Security Technologies, LLC 2007a) requires an annual review to assess the adequacy of the performance assessments (PAs) and composite analyses (CAs), with the results submitted to the U.S. Department of Energy (DOE) Office of Environmental Management. The Disposal Authorization Statements for the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) also require that such reviews be made and that secondary or minor unresolved issues be tracked and addressed as part of the maintenance plan.The U.S. Department of Energy, National Nuclear Security Administration Nevada Field Office (NNSA/NFO) performed an annual review of the Area 3 and Area 5 RWMS PAs and CAs for federal fiscal year (FY) 2016. This annual summary report presents results and conclusions of the FY 2016 review, and determines the adequacy of the PAs and CAs. Operational factors (e.g., waste forms and containers, facility design, and waste receipts), closure plans, monitoring results, and research and development (R&D) activities were reviewed to determine the adequacy of the PAs. Likewise, the environmental restoration activities at the Nevada National Security Site (NNSS) relevant to the sources of residual radioactive material that are considered in the CAs, the land-use planning, and the results of the environmental monitoring and R&D activities were reviewed to determine the adequacy of the CAs. Important developments in FY 2016 include the following: Development of a new Area 5 RWMS closure inventory estimate based on disposals through FY 2016, Evaluation of new or revised waste streams by special analysis, and Development and acceptance of version 4.200 of the Area 5 RWMS GoldSim PA/CA model. The Area 3 RWMS has been in inactive status since July 1, 2006, with the last shipment received in April 2006. The FY 2016 review of operations, facility design, closure plans, monitoring results, and R&D results for the Area 3 RWMS indicates no changes that would impact PA validity. The conclusion of the annual review is that all performance objectives can be met and the Area 3 RWMS PA remains valid. There is no need to revise the Area 3 RWMS PA. Review of Area 5 RWMS operations, design, closure plans, monitoring results, and R&D activities indicates that no significant changes have occurred. The FY 2016 PA results, generated with the Area 5 RWMS v4.200 GoldSim PA model, indicate that there continues to be a reasonable expectation of meeting all performance objectives. All results remain less than 50% of their performance objectives. The results and conclusions of the Area 5 RWMS PA are judged valid, and there is no need to the revise the PA. A review of changes potentially impacting the CAs indicates that no significant changes occurred in FY 2016. A new Corrective Action Unit (CAU), CAU 576, with corrective action sites near the Area 3 RWMS and Area 5 RWMS was identified in FY 2016. The sites are currently under investigation and not expected to be important sources for the CA. The continuing adequacy of the CAs was evaluated with the new models, and no significant changes that would alter the CAs’ results or conclusions were found. The revision of the Area 3 RWMS CA, which will include the Yucca Flat Underground Test Area (CAU 97) source, is scheduled for FY 2024, following the completion of the Corrective Action Decision Document/Corrective Action Plan. Inclusion of the Frenchman Flat Underground Test Area (CAU 98) source in the Area 5 RWMS CA is planned pending the completion of the CAU 98 Closure Report in FY 2017. Near-term R&D efforts will focus on continuing development of the PA, CA, and inventory models for the Area 3 and Area 5 RWMSs.

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DOE OSTI2016

Ensuring Longevity: Ancient Glasses Help Predict Durability of Vitrified Nuclear Waste

How does glass alter with time? For the last hundred years this has been an important question to the fields of object conservation and archeology to ensure the preservation of glass artifacts. This same question is part of the development and assessment of durable glass waste forms for the immobilization of nuclear wastes. Researchers have developed experiments ranging from simple to highly sophisticated to answer this question, and, as a result, have gained significant insight into the mechanisms that drive glass alteration. However, the gathered data have been predominately applicable to only short-term alteration times, i.e. over the course of decades. What has remained elusive is the long-term mechanisms of glass alteration[1]. These mechanisms are of particular interest to the international nuclear waste glass community as they strive to ensure that vitrified products will be durable for thousands to tens of thousands of years. For the last thirty years this community has been working to fill this research gap by partnering with archeologists, museum curators, and geologists to identify hundred to million-year old glass analogues that have altered in environments representative of those expected at potential nuclear waste disposal sites. The process of identifying a waste glass relevant analogue is challenging as it requires scientists to relate data collected from short-term laboratory experiments to observations made from long-term analogues and extensive geochemical modeling.

Ancient Glass↗

DOE OSTI2017

Precipitation of Epsilon Particles in Metal Doped Ceria Irradiated with Energetic Ions

Metallic particles precipitated from fission products in oxide fuel matrix (e.g., UO{sub 2}) have a great impact on the thermal and mechanical properties of the fuel. A burn-up of 40 MWd/kg U results in the conversion of 4% of the uranium to approximately 3% fission products and 1% transuranium elements. Epsilon phase is the major metallic phase of the precipitates with a hexagonal-closed packed (HCP) crystal structure. It can exist in a variety of metallic forms in UO{sub 2}, but typically, it consists of five metals: Mo, Pd, Rh, Ru and Tc. Epsilon particles can form over a wide range of stoichiometries in the five metal system. Simulated compositions with Re as a surrogate for Tc have been investigated as a waste form for {sup 99}Tc, an isotope with a long half-life of 2.13 10{sup 5} years and a high solubility under oxidizing conditions in addition to Mo in the corrosion process. There is a pressing need to understand the factors influencing the formation and growth of the metallic phase in fuel. Efforts are currently underway to perform careful neutron irradiation of nuclear fuel under controlled conditions in a test reactor, recover metallic phases that may be present, and characterize the resulting structure and chemistry. Due to the long duration, high cost and radiological concerns associated with neutron irradiation and sample characterizations, ion irradiation studies of a surrogate material with a full control of the processing parameters can emulate different stages of the particle precipitation, which can add a tremendous value to reactor-based studies. This presentation reports our recent ion irradiation results on the metallic particle precipitation under various irradiation and thermal annealing conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2013

Potential of hybrid functionalized meso-porous materials for the separation and immobilization of radionuclides

Functionalized meso-porous materials are a class of hybrid organic-inorganic material in which a meso-porous metal oxide framework is functionalized with multifunctional organic molecules. These molecules may contain one or more anchor groups that form strong bonds to the pore surfaces of the metal oxide framework and free functional groups that can impart and or modify the functionality of the material such as for binding metal ions in solution. Such materials have been extensively studied over the past decade and are of particular interest in absorption applications because of the tremendous versatility in choosing the composition and architecture of the metal oxide framework and the nature of the functional organic molecule as well as the efficient mass transfer that can occur through a well-designed hierarchically porous network. A sorbent for nuclear applications would have to be highly selective for particular radio nuclides, it would need to be hydrolytically and radiolytically stable, and it would have to possess reasonable capacity and fast kinetics. The sorbent would also have to be available in a form suitable for use in a column. Finally, it would also be desirable if once saturated with radio nuclides, the sorbent could be recycled or converted directly into a ceramic or glass waste form suitable for direct repository disposal or even converted directly into a material that could be used as a transmutation target. Such a cradle-to- grave strategy could have many benefits in so far as process efficiency and the generation of secondary wastes are concerned.This paper will provide an overview of work done on all of the above mentioned aspects of the development of functionalized meso-porous adsorbent materials for the selective separation of lanthanides and actinides and discuss the prospects for future implementation of a cradle-to-grave strategy with such materials. (author)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗