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Disposal Concepts for a High-Temperature Repository in Shale.

Disposal of large, heat-generating waste packages containing the equivalent of 21 pressurized water reactor (PWR) assemblies or more is among the disposal concepts under investigation for a future repository for spent nuclear fuel (SNF) in the United States. Without a long (>200 years) surface storage period, disposal of 21-PWR or larger waste packages (especially if they contain high-burnup fuel) would result in in-drift and near-field temperatures considerably higher than considered in previous generic reference cases that assume either 4-PWR or 12-PWR waste packages (Jové Colón et al. 2014; Mariner et al. 2015; 2017). Sevougian et al. (2019c) identified high-temperature process understanding as a key research and development (R&D) area for the Spent Fuel and Waste Science and Technology (SFWST) Campaign. A two-day workshop in February 2020 brought together campaign scientists with expertise in geology, geochemistry, geomechanics, engineered barriers, waste forms, and corrosion processes to begin integrated development of a high-temperature reference case for disposal of SNF in a mined repository in a shale host rock. Building on the progress made in the workshop, the study team further explored the concepts and processes needed to form the basis for a high-temperature shale repository reference case. The results are described in this report and summarized..

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Characterization of undissolved solids from the dissolution of North Anna reactor fuel

Here, samples of undissolved solids (UDS) from the dissolution of North Anna reactor fuel were characterized to investigate the effects of using air or oxygen as the oxidant during tritium removal. The UDS composition data also support the development of a waste form for disposal. There was no discernible effect of the oxidant used during the tritium removal process or the size fraction on the UDS composition. Scanning electron microscopy (SEM) and energy dispersive (x-ray) spectroscopy were used to estimate the oxygen content of the UDS and it was found to be potentially significant, on the order of 30% by mass and 80% by atom.

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Review of Options for Ammonia/Ammonium Management

This report is a review of literature supporting practical ammonia/ammonium destruction processes. Melter research supporting Hanford Low Activity Waste (LAW) glass production has shown that significant amounts of ammonia will be in the melter offgas condensate. Further work with secondary waste forms indicates the potential need to remove the ammonia, perhaps by an oxidative process. This review finds likely practical chemical methods to oxidize ammonia in aqueous solution at moderate temperatures and atmospheric pressure, using easily obtained reagents. Leading candidates include nitrite oxidation to produce nitrogen gas, various peroxide oxidative processes, and air stripping. This work reviews many other processes and provides reasoning to not consider those processes further for this application.

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Testing of an Iodine and Tritium Removal System for Advanced Tritium Pretreatment Off-Gas

The reprocessing of used nuclear fuel would release volatile radionuclides into the off-gas of a processing plant, including 3 H, 14 C, 85 Kr, and 129 I. For a reprocessing plant sited within the United States and governed by US regulations, the abatement of some or all of these radionuclides from the plant off-gas would be required before discharge of that gas to the environment. A potential simplification of the off-gas management system can be achieved through an efficient advanced tritium pretreatment (ATPT) step in which the UO 2 fuel is oxidized by NO 2 prior to dissolution. Oxidation of the UO 2 fuel matrix results in the release of tritium contained within. Up-front removal of tritium from the fuel in a pretreatment step, followed by the abatement of tritium from the advanced tritium pretreatment off-gas (ATPTOG) stream, can minimize or eliminate the distribution of tritium throughout the plant, also decreasing or eliminating the need for tritium capture on multiple off-gas streams. The use of NO 2 as the oxidant allows tritium pretreatment to be performed at lower temperatures and may result in the quantitative release of iodine from the fuel. A total of five tests examined AgA as a potential iodine sorbent at an operating temperature of 150°C and both 3A MS and silica gel as potential tritium sorbents with an operating temperature of 40°C. 3A MS and silica gel are intended for use as regenerative sorbents, in which the adsorbed tritium (as tritiated water or tritiated nitric acid) is loaded onto the sorbent at operating temperature and then subsequently desorbed at high temperature into a small-volume gas stream for recovery and conversion to a waste form. This testing leaves many fundamental questions regarding the ATPTOG iodine and tritium abatement systems unanswered. These include questions regarding sorbent capacity and sorbate desorption. Overall, this testing indicates that tritium and iodine abatement from an ATPTOG stream by solid sorbents is currently at a low stage of technological development and that deployment of such an abatement system would require substantial additional research and development.

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Status of SRNL Radiological Field Lysimeter Experiment (RadFLEx) – Year 7

The Radiological Field Lysimeter Experiment (RadFLEx) began in 2012 and is a collaboration between the Savannah River National Laboratory (SRNL) and Clemson University. The purpose of this facility is to study the long-term (2 to 20 years) fate and transport of radionuclides in the Savannah River Site (SRS) vadose zone under natural field and meteorological conditions. The unique facility houses 48 5-L cores filled with sediments amended with various radionuclide sources. The results from these studies have been applied to the development of geochemical models used to assess the risk posed by subsurface nuclear waste disposal, environmental remediation, and waste form development. This report describes the refurbishment of the exterior of the RadFLEx facility and the synthesis and deployment of six plutonium(Pu) sources, four neptunium (Np) sources and one radium (Ra) source. It is anticipated that these newly installed lysimeter cores will be studied for up to 10 years.

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Glass Property Models and Constraints for Estimating the Glass to be Produced at Hanford by Implementing Current Advanced Glass Formulation Efforts

Recent glass formulation and melter testing data have suggested that significant increases in waste loading in HLW and LAW glasses are possible over current system planning estimates. The data (although limited in some cases) were evaluated to determine a set of constraints and models that could be used to estimate the maximum loading of specific waste compositions in glass. It is recommended that these models and constraints be used to estimate the likely HLW and LAW glass volumes that would result if the current glass formulation studies are successfully completed. It is recognized that some of the models are preliminary in nature and will change in the coming years. Plus the models do not currently address the prediction uncertainties that would be needed before they could be used in plant operations. The models and constraints are only meant to give an indication of rough glass volumes and are not intended to be used in plant operation or waste form qualification activities. A current research program is in place to develop the data, models, and uncertainty descriptions for that purpose. A fundamental tenet underlying the research reported in this document is to try to be less conservative than previous studies when developing constraints for estimating the glass to be produced by implementing current advanced glass formulation efforts. The less conservative approach documented herein should allow for the estimate of glass masses that may be realized if the current efforts in advanced glass formulations are completed over the coming years and are as successful as early indications suggest they may be. Because of this approach there is an unquantifiable uncertainty in the ultimate glass volume projections due to model prediction uncertainties that has to be considered along with other system uncertainties such as waste compositions and amounts to be immobilized, split factors between LAW and HLW, etc.

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M-Star® Software Test and Verification for Impeller Mixing in a Tank

Before a sample of the Slurry Mix Evaporator (SME) can be taken, the SME product sampling procedure requires that the agitator power be stable between 20 and 30 kW for at least one hour. The SME transfer to Melter Feed Tank (MFT) procedure also requires the SME agitator power be stabilized between 20 and 30 kW prior to transfer. These requirements are specified to ensure samples are homogeneous, as discussed in the Waste Form Qualification Report. During SME Batch 804, the agitator power dropped to 19 kW and struggled to achieve and maintain 20 kW. It was later discovered that the cause of the power drop was due to one of the bottom blades of the agitator breaking off. Both the sample and the transfer occurred without the power stabilizing between 20 and 30 kW. Therefore, the quality of SME Batch 804 is indeterminate, and homogeneity was questionable.

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Performance Assessment for the E-Area Low-Level Radioactive Waste Disposal Facility at the Savannah River Site: Chapter 8

This chapter, together with Appendix H, provides the necessary CWTS inventory limits and trigger values for every parent radionuclide not screened out in Sections 2.3.6, 2.3.7, and 2.3.8. Also provided are details associated with how generic and special waste forms are handled on a DU-specific basis, and a discussion of the conversion of preliminary inventory limits (via transport runs summarized in Chapter 5) into final inventory limits for use in the CWTS limits system. Using the final inventory limits, a projected 2065 CWTS inventory is generated for use in the PA closure analysis outlined in Chapter 9.

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Radionuclide Waste Disposal: Development of Multi-scale Experimental and Modeling Capabilities (Final Report)

The DOE EPSCoR Implementation project “Radioactive waste management: Development of multi-scale experimental and modeling capabilities” helped to develop a team of scientists and engineers from Clemson University, South Carolina State University, and the University of South Carolina to address the disposition of nuclear wastes and study the transport of radioisotopes from a waste repository in the near and far field. The project involved 20 faculty from the three institutions as well as 13 postdoctoral fellows, 32 graduate students, and 32 undergraduate students and was active from 2014-2019. Additionally, we forged new collaborations with nine researchers from DOE laboratories SRNL, LLNL, and ANL as well as the University of Manchester and the China Academy of Engineering Physics. The overarching goal of the project was to understand the conditions under which important classes of co-reactants, ranging from counter ions in crystal lattices to dissolved oxygen in pores, control the chemistry and transport characteristics of radionuclides in engineered waste forms and natural soils. Our approach was to characterize the time and length scales over which non-equilibrium states are maintained by rate-limiting, or rate-enhancing, reactions between radionuclides and co-reactants due to interactions between physical mass-transfer processes (i.e., advection, diffusion) and (biogeo) chemical reactions. We have focused our project on three specific classes of reactions relevant to radionuclide transport at DOE legacy sites: ion exchange/substitution, ligand complexation, and redox-mediated reactions. Understanding radionuclide migration requires detailed knowledge of how changes to a system – whether engineered or natural – drive the behavior of co-reactants, which in turn provide the geochemical context controlling radionuclide transport. Student engagement and training were a primary focus of the project in order to create a pipeline of researchers who could work in the area of nuclear waste disposition to support the state and the nation. Over the duration of the project we worked with 32 undergraduate, graduated 18 M.S. students and 14 Ph.D. students, and advised 13 postdoctoral fellows. The Ph.D students and postdocs have primarily taken positions at DOE laboratories, academia, and industry. Through our collaborative team, numerous follow on projects have been started with over $5M in sponsored research. Additionally, thus far the team has published 53 peer reviewed papers and given over 75 technical presentations.

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Concept of Operations for Advanced Reactor Spent Nuclear Fuel Management

This presentation presents a preliminary description of a concept of operations to incorporate advanced-reactor spent nuclear fuel (SNF) into an integrated waste-management system (IWMS). The evaluation includes SNF from four advanced-reactor concepts with the following fuel types: (1) small modular reactors using oxide fuels, (2) tristructural-isotropic (TRISO) fuels, (3) metallic fuels, and (4) fuel salts. To provide context for the proposed concept of operations for advanced reactors, a comparison is made with traditional light-water reactors (LWRs) to identify potential gaps in the IWMS. The technical differences between advanced reactors and LWRs are assessed to determine the feasibility of managing advanced-reactor waste streams using existing operations and technology. This presentation emphasizes fuel types from Advanced Reactor Demonstration Program reactors: Xe 100, which uses TRISO fuel and Natrium, with its metallic fuels while also analyzing management options for molten-salt reactors and advanced light-water reactors (ALWRs). Understanding the storage, transportation, and disposal requirements of SNF is dependent on both the quantity and characteristics of the SNF generated by nuclear reactors. This presentation provides a high level overview, comparing the anticipated concept of operations for different SNFs from advanced reactors. The IWMS includes at-reactor storage, transportation, potential off-site storage, potential treatment, and disposition. To assess the potential effect of advanced-reactor concept of operations on the IWMS, estimates were made for fuel characteristics that contribute to storage, transportation, disposal, and possible treatment of advanced-reactor SNF. These include canister heat load, dose rates, and criticality-control limits, which are important for determining the condition and configuration of the advanced reactor SNF. At-reactor storage of LWR SNF traditionally involves a spent-fuel pool (SFP) before transfer to an independent spent-fuel storage installation. However, some advanced-reactor concepts, particularly those using TRISO and salt fuels, do not anticipate the use of an SFP. This difference in at-reactor storage could impact the IWMS. Additionally, transportation of advanced-reactor SNF may include additional processes tied to potential off gassing, and transportation of microreactor SNF may occur within the reactor vessel. Some advanced-reactor SNF could also undergo treatment to meet requirements of an acceptable waste form for disposition, and the treatment location will be a major contributor to efficiently performing IWMS responsibilities. Moreover, the quantity of SNF generated is an important consideration for IWMS because it could affect the size of the transportation fleet and potential off-site storage requirements. Additionally, volume and heat load are the primary drivers for SNF disposition. This presentation compares potential packaging options for advanced reactor SNF with traditional LWR packaging to provide a high-level comparison for the needs of the IWMS for advanced-reactor SNF.

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When Is the Simple Radiotoxicity Approach Useful for Advanced Fuel Cycle System Assessments Given the Existence of Complex Performance Dose Assessments?

Engineers often face the general question of which approximations are appropriate for a given analytical task. In particular, when is a simpler model useful if a more complex model also exists? This paper explores this question in the domain of radiotoxicity relative to geologic disposal performance dose assessments. Criterion 1 requires that the simpler approach, radiotoxicity, must be calculated correctly. The concept of ingestion radiotoxic inventories is analogous to the inventory of toxic chemicals in other industries. From a decision analysis perspective, it is also somewhat analogous to the nuclear reactor safety concept of “passive safety.” This paper explains some of the issues in calculating radiotoxicity, motivated by the author’s observations of errors in the literature: not accounting for radioactive progeny, misunderstanding natural “ore,” and focusing on transuranic (TRU) isotopes without adequate attention to actinide decay products. For example, Th/233U fuel cycles do have lower amounts of TRU isotopes than U/239Pu fuel cycles, but that does not necessarily mean lower long-term hazard. Criterion 2 requires that the uncertainties in the more complex approach, performance dose assessments, must raise issues for the assessments’ intended purposes—in which case, radiotoxic inventory may be of assistance until those issues are resolved. Performance dose assessments were developed for, and are legally the way to show, compliance with regulations, but the uncertainties are large. Less obvious is the degree to which dose assessments are applicable to other purposes—comparing fuel cycle options prior to site selection and showing the safety of a fuel cycle and waste management approach to the public. In the last sense especially, performance dose assessments are analogous to probabilistic risk assessments for nuclear reactor safety. The United States lacks a selected consensus site, selected fuel cycle approach (direct disposal versus recycling), and selected waste form. Thus, the paper does not intend to discuss all the issues with performance dose assessments but rather intends to focus on only those performance dose uncertainties that raise issues when comparing fuel cycles. Uncertainties associated with whether a generic geological environment is attractive or a specific location meets requirements are beyond the scope of this paper. Ingestion radiotoxicity correlates with heat, gamma, and inhalation radiotoxicity. Thus, options that are relatively high in ingestion radiotoxicity tend to be high in other parameters. Therefore, reduction in ingestion radiotoxicity means both that the potential source term for release is lower but also that one driving force for release (heat) is also lower. However, the most important time frames differ as heat is mainly an issue in decades and centuries after reactor discharge, but ingestion radiotoxicity is mainly an issue during longer time periods. Ingestion radiotoxicity points to the importance of actinides in long-term waste management, followed by specific fission products such as 99Tc, 129I, 93Zr, 135Cs, and 79Se.

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Summary Report for the Analysis of the Sludge Batch 8 (Macrobatch 10) DWPF Pour Stream Glass Sample

In order to comply with the Defense Waste Processing Facility (DWPF) Waste Form Compliance Plan for Sludge Batch 8, Savannah River National Laboratory (SRNL) personnel characterized a pour stream sample that was collected while canister S04274 was being filled. This report summarizes the results of the compositional analysis for reportable oxides and radionuclides, and the normalized Product Consistency Test (PCT) results. The PCT responses indicate that the DWPF produced glass is significantly more durable than the Environmental Assessment glass. Results and further details are documented in SRNL-STI-2018- 00699, “Analysis of the Sludge Batch 8 (Macrobatch 10) DWPF Pour Stream Glass Sample.”

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The Effects of Mixing Multi-Component HLW Glasses on Spinel Crystal Size

The Hanford Waste Treatment and Immobilization Plant will vitrify radioactive waste into borosilicate glass. The high-level waste (HLW) glass formulations are constrained by processing and property requirements, including restrictions aimed at avoiding detrimental impacts of spinel crystallization in the melter. To understand the impact of glass chemistry on crystallization, two HLW glasses precipitating small (?5 µm) spinel crystals were individually mixed with a glass that precipitated large (?45 µm) spinel crystals in ratios of 25, 50, and 75 wt%. The size of spinel crystals in the mixed glasses varied from 5 to 20 µm. Small crystal size was attributed to: (1) high concentrations of nuclei due to the presence of ruthenium oxide and (2) chromium oxide aiding high rates of nucleation. Results indicate that the spinel crystal size can be controlled using chromium oxide and/or noble metal concentrations in the melt, even in complex mixtures like HLW glasses. Small crystals tend to settle slowly, so they are acceptable in the melter without a risk of failure. Allowing higher concentrations of spinel-forming waste components in the waste glass enables glass compositions with higher waste loading, thus increasing plant operational flexibility. An additional benefit to the presence of chromium oxide in the glass composition is the potential for the oxide to protect melter walls against corrosion.

Lonergan, Charmayne E.↗

DEVELOPMENT OF AN APPROACH FOR DOWNBLENDING AND DISPOSITION OF IRRADIATED GRAPHITE FUEL

The IGR reactor, a pulse-type test experimental reactor, reached full power in 1961. The reactor contains a center axial experimental ampoule that is subjected to a large pulse of neutrons (neutron flux maximum density of 7×1016 n/cm2·s, peak power 10GW) when the reactor is operated. The fuel form for the IGR reactor is graphite cubes and rods impregnated with highly enriched (90%) uranyl-dinitrate (UO2(NO3)2·6H2O). This fuel is eligible for return to Russia for reprocessing under the Russian Research Reactor Fuel Return program. However due to some technical and licensing issues it was decided to immobilize this fuel in Kazakhstan. The disposition approach thus selected for the spent HEU fuel involves down-blending of the fuel followed by cementation. Development of the process for down-blending and subsequent cementation requires a process that satisfies many criteria, including fissile content, compressive strength, permeability, and containment of radioactivity, among others. One key goal of the final product is to meet the criteria for termination of safeguards. This paper will describe the overall challenge associated with disposition of irradiated HEU graphite spent fuel, the identification of the objectives of the disposition process, and the constraints associated with development of the process and the waste form.

Gaines, Kris↗

Determination of Reportable Radionuclides for Defense Waste Processing Facility (DWPF) Sludge Batch 9 (Macrobatch 11)

This report documents analyses and calculations performed by the Savannah River National Laboratory (SRNL) of Tank 40 sludge as part of the Waste Acceptance Product Specifications (WAPS) requirements for Sludge Batch 9 (SB9) for the Defense Waste Processing Facility (DWPF). Tank Farm sample HTF-40-17-5 was received by SRNL Shielded Cells Operations (SCO) and was prepared for radionuclide analyses in addition to various other physical and chemical characterizations. Radionuclide analyses were performed by SRNL Analytical Development (AD). Based on criteria set forth in the Department of Energy (DOE) WAPS and DWPF’s Waste Form Compliance Plan (WCP), as well as, historical lessons from previous sludge batch analyses, a list of radionuclides was developed for which the sample was analyzed. The results of these analyses were then used as input into commercially available software, RadDecay version (v) 5.01. The software was used to calculate the activity of the measured analytes in index years 2017 through 3115 in 100-year increments. Radionuclides with half-lives greater than 10 years and activities that comprised more than 0.01% of the total sludge batch activity are reportable.

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Investigation of the swelling behavior of cationic exchange resins saturated with Na{sup +} ions in a C{sub 3}S paste

Ion exchange resins (IERs) are widely used by the nuclear industry to decontaminate radioactive effluents. Spent products are usually encapsulated in cementitious materials. However, the solidified waste form can exhibit strong expansion, possibly leading to cracking, if the appropriate binder is not used. In this work, the interactions between cationic resins in the Na{sup +} form and tricalcium silicate are investigated during the early stages of hydration in order to gain a better understanding of the expansion process. It is shown that the IERs exhibit a transient swelling of small magnitude due to the decrease in the osmotic pressure of the external solution. This expansion, which occurs just after setting, is sufficient to damage the material which is poorly consolidated for several reasons: low degree of hydration, precipitation of poorly cohesive sodium-bearing C–S–H, and very heterogeneous microstructure with zones of high porosity.

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Boom clay borehole water, home of a diverse bacterial community

For over two decades, Boom Clay has been studied in the framework of geological disposal of nuclear waste thereby mainly addressing its geochemical properties. Today, also the microbiological properties and the possibility of microbes interacting with radionuclides or repository components including the waste form, in a host formation like Boom Clay are considered [2,3]. In the past, a reference composition for synthetic Boom Clay pore water (BCPW) was derived, based on interstitial water sampled from different layers within the Boom clay [1]. Similarly, the primary aim of this microbiological study was to determine the core BCPW bacterial community and identify representative water samples for future microbial directed lab experiments. In this respect, BCPW was sampled from different Boom Clay layers using the Morpheus piezometer and subsequently analysed by microscopy and molecular techniques, in search for overall shared and abundant micro-organisms. (authors)

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Preparation and evaporation of Hanford Waste treatment plant direct feed low activity waste effluent management facility simulant

The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Melter Off-Gas Condensate, LMOGC) from the off-gas system. The baseline plan for disposition of this stream during full WTP operations 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. However, during the Direct Feed LAW (DFLAW) scenario, planned disposition of this stream involves concentrating the condensate in a new evaporator at the Effluent Management Facility (EMF) and returning it to the LAW melter. The LMOGC stream will contain components, e.g. halides and sulfates, that are volatile at melter temperatures, have limited solubility in glass waste forms, and present a material corrosion concern. Because this stream will recycle within WTP, these components are expected to accumulate in the LMOGC stream, exacerbating their impact on the number of LAW glass containers that must be produced. Diverting the stream reduces the halides and sulfates in the glass and is a key objective of this program. In order to determine the disposition path, it is key to experimentally determine the fate of contaminants. To do this, testing is needed to account for the buffering chemistry of the components, determine the achievable evaporation end point, identify insoluble solids that form, determine the formation and distribution of key regulatoryimpacting constituents, and generate an aqueous stream that can be used in testing of the subsequent immobilization step. This overall program examines the potential treatment and immobilization of the LMOGC stream to enable alternative disposal. The objective of this task was to (1) prepare a simulant of the LAW Melter Off-gas Condensate expected during DFLAW operations, (2) demonstrate evaporation in order to predict the final composition of the effluents from the EMF evaporator to aid in planning for their disposition, and (3) generate concentrated evaporator bottoms for use in immobilization testing.

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