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All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Uniaxial Creep as a Control on Mercury Intrusion Capillary Pressure in Consolidating Rock Salt

The nature of geologic disposal of nuclear waste in salt formations requires validated and verified two-phase flow models of transport of brine and gas through intact, damaged, and consolidating crushed salt. Such models exist in other realms of subsurface engineering for other lithologic classes (oil and gas, carbon sequestration etc. for clastics and carbonates) but have never been experimentally validated and parameterized for salt repository scenarios or performance assessment. Models for waste release scenarios in salt back-fill require phenomenological expressions for capillary pressure and relative permeability that are expected to change with degree of consolidation, and require experimental measurement to parameterize and validate. This report describes a preliminary assessment of the influence of consolidation (i.e. volume strain or porosity) on capillary entry pressure in two phase systems using mercury injection capillary pressure (MICP). This is to both determine the potential usefulness of the mercury intrusion porosimetry method, but also to enable a better experimental design for these tests. Salt consolidation experiments are performed using novel titanium oedometers, or uniaxial compression cells often used in soil mechanics, using sieved run-of-mine salt from the Waste Isolation Pilot Plant (WIPP) as starting material. Twelve tests are performed with various starting amounts of brine pore saturation, with axial stresses up to 6.2 MPa (~900 psi) and temperatures to 90°C. This corresponds to UFD Work Package 15SN08180211 milestone “FY:15 Transport Properties of Run-of-Mine Salt Backfill – Unconsolidated to Consolidated”. Samples exposed to uniaxial compression undergo time-dependent consolidation, or creep, to various degrees. Creep volume strain-time relations obey simple log-time behavior through the range of porosities (~50 to 2% as measured); creep strain rate increases with temperature and applied stress as expected. Mercury porosimetry is used to determine characteristic capillary pressure curves from a series of consolidation tests and show characteristic saturation-capillary pressure curves that follow the common van Genuchten (1978, 1980) formulation at low stresses. Higher capillary pressure data are suspect due to the large potential for sample damage, including fluid inclusion decrepitation and pore collapse. Data are supportive of use of the Leverett “J” function (Leverett, 1941) to use for scaling characteristic curves at different degrees of consolidation, but better permeability determinations are needed to support this hypothesis. Recommendations for further and refined testing are made with the goal of developing a self- consistent set of constitutive laws for granular salt consolidation and multiphase (brine-air) flow.

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DOE OSTI2024

RANGERS: Modeling Report on Integrity and Performance Assessment of Engineered Barrier Systems in a Salt Repository for HLW/SNF

The Engineered Barrier System (EBS) plays an important role in ensuring the long-term safety and containment of high-level waste (HLW) and spent nuclear fuel (SNF) in deep geological repositories in salt formation. As part of a multi-barrier system, the EBS works alongside the natural barrier, which is the salt formation itself and the technical barrier comprising the disposal casks. The primary function of the EBS is to maintain containment during a defined period until the backfill used in the repository made of crushed salt, develops its sealing capacity through compaction. Over the time, the backfill eventually compacts to a state of low porosity and permeability, acting as a long-term seal. However, until this process is complete, the EBS must retain its structural and functional integrity. Regulatory guidelines in Germany currently require the EBS to remain effective for up to next ice age, that is expected in 50,000 years. The significant hydro-geological and topographic changes expected during an ice age could make it impossible to accurately predict the hydro-chemical conditions within the repository system at that time. In response to these challenges, BGE TECHNOLOGY GmbH (BGE TEC) and Sandia National Laboratories (SNL) have jointly developed a comprehensive methodology for the design and safety assessment of engineered barrier systems within the scope of the RANGERS project. This methodology is tailored for repositories in salt formations. The developed methodology provides a structured approach for designing and assessing the performance of the EBS in salt-based repositories. It begins with defining a sealing concept based on the geological characteristics of the selected site and the overall repository design. The entire repository system, comprising the geological site, repository infrastructure, and EBS, is then subjected to a Features, Events, and Processes (FEP) analysis, focusing solely on those FEPs that affect the EBS. The derived FEPs help identify the loads and stresses acting on the EBS, which serve as the foundation for conducting an integrity assessment. This analysis helps predict the EBS’s evolution and performance over the regulatory time frame, feeding into integrated performance assessment simulations.

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DOE OSTI2021

International collaboration in disposal research: comparative modeling of coupled processes in the DECOVALEX project

Abstract. This presentation gives an overview of an international research collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems. The creation of the international DECOVALEX project, now running for more than 25 years, was motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel. DECOVALEX emphasizes joint analysis and comparative modeling of state-of-the-art field and laboratory experiments, across a range of host rock options and repository designs. Participating research teams are from radioactive waste management organizations, national research institutes, regulatory agencies, universities, and consulting groups, providing a wide range of perspectives and solutions to these complex problems. The presentation provides examples of the research contributions made collectively in past DECOVALEX tasks and also touches on the unique modeling challenges tackled in the ongoing project phase, referred to as DECOVALEX-2023. The current phase comprises 17 partner organizations, about 50 modeling teams, and 7 modeling tasks, which cover a broad portfolio from fundamental studies on gas migration to full-scale in situ heater experiments in different host rocks to performance assessment studies. Together, these examples illustrate that the insight and scientific knowledge gained within the DECOVALEX project would not have been possible if one group had studied these complex THMC modeling challenges alone rather than within a truly collaborative setting.

Birkholzer, Jens T.↗
DOE OSTI2018

Assessment of the potential for criticality in the far field of a used nuclear fuel repository

This study aims to assess the likelihood for criticality in the far field of a repository for direct disposal of commercial light water reactor used nuclear fuel. Two models are used in combination: (1) a neutronics model to estimate the minimum critical masses of spherical, water-saturated depositions of fissile material; (2) a transport model to simulate the dissolution of waste packages arranged in an array and the subsequent transport of fissile solutes through fractured bedrock to a single accumulation location. The neutronics model shows that heavy metals from different types of used fuel present the same minimum critical mass behavior in the parameter space of initial enrichment and burnup, dictated largely by the fissile content. However, the magnitude of the minimum critical mass varies significantly within that parameter space, and secondary effects like the presence of absorbing nuclides play a minor role. Here, the transport model employs various subsurface transport scenarios, and for each scenario the mass of each isotope and the overall fissile content of the accumulation is reported from the time of canister failure up to one hundred million years at various distances from the repository edge. Taking the results of the two models in concert, it is shown that even if the accumulation of a critical mass is possible under conservative conditions, these conditions are unlikely to be present in the vicinity of a carefully engineered repository. Based on the results of each model, recommendations for risk mitigation in terms of waste characteristics and repository design are given.

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DOE OSTI2026

Analysis of the Effects of Postclosure Criticality on Repository Performance

The United States Department of Energy’s (DOE) Office of Nuclear Energy’s Disposal Research & Development Campaign seeks to better understand the technical basis, risks, and uncertainty associated with the safe and secure disposition of spent nuclear fuel (SNF) and high-level radioactive waste (HLW). Commercial nuclear power generation in the United States has resulted in thousands of metric tons of SNF, the disposal of which is the responsibility of DOE (Nuclear Waste Policy Act of 1982, as amended). Any repository licensed to dispose of SNF will be subject to requirements regarding the long-term performance of that repository. Evaluating the long-term performance of the repository may consider the consequences of the SNF achieving a critical configuration during the postclosure period. Of particular interest is the potential for this to occur in dual-purpose canisters (DPCs), which are currently licensed and being used to store and transport SNF but were not designed for permanent geologic disposal. DOE has been considering disposing of SNF in DPCs to avoid the costs and worker dose associated with repackaging the SNF currently stored in DPCs into repository-specific canisters. This report examines the consequences of postclosure criticality to provide technical support to DOE in developing a disposal plan.

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NASA NTRS1982

Analysis of space systems for the space disposal of nuclear waste follow-on study. Volume 1: Executive summary

The impact on space systems of three alternative waste mixes was evaluated as part of an effort to investigate the disposal of certain high-level nuclear wastes in space as a complement to mined geologic repositories. A brief overview of the study background, objectives, scope, approach and guidelines, and limitations is presented. The effects of variations in waste mixes on space system concepts were studied in order to provide data for determining relative total system risk benefits resulting from space disposal of the alternative waste mixes. Overall objectives of the NASA-DOE sustaining-level study program are to investigate space disposal concepts which can provide information to support future nuclear waste terminal storage programmatic decisions and to maintain a low level of research activity in this area to provide a baseline for future development should a decision be made to increase the emphasis on this option.

Source record↗
NASA NTRS2000

Modeling of Solid Waste Processing Options in BIO-Plex

BIO-Plex is a ground-based test bed currently under development by NASA for testing technologies and practices that may be utilized in future long-term life support missions. All aspects of such an Advanced Life Support (ALS) System must be considered to confidently construct a reliable system, which will not only allow the crew to survive in harsh environments, but allow the crew time to perform meaningful research. Effective handling of solid wastes is a critical aspect of the system, especially when recovery of resources contained in the waste is required. This is particularly important for ALS Systems configurations that include a Biomass Production Chamber. In these cases, significant amounts of inedible biomass waste may be produced, which can ultimately serve as a repository of necessary resources for sustaining life, notably carbon, water, and plant nutrients. Numerous biological and physicochemical solid waste processing options have been considered. Biological options include composting, aerobic digestion, and anaerobic digestion. Physicochemical options include pyrolysis, SCWO (supercritical water oxidation), various incineration configurations, microwave incineration, magnetically assisted gasification, and low temperature plasma reaction. Modeling of these options is a necessary step to assist in the design process. A previously developed top-level model of BIO-Plex implemented in MATLAB Simulink (r) for the use of systems analysis and design has been adopted for this analysis. Presently, this model only considered incineration for solid waste processing. Present work, reported here, includes the expansion of this model to include a wider array of solid waste processing options selected from the above options, bearing in mind potential, near term solid waste treatment systems. Furthermore, a trade study has also been performed among these solid waste processing technologies in an effort to determine the ideal technology for long-term life support missions.

Rodriguez, Luis F.↗
DOE OSTI2017

Purification of Zirconium Tetrachloride (ZrCl{sub 4}) from UNF Cladding - A Progress Report

Zirconium-based cladding materials that surround used nuclear fuel (UNF) rods represent a significant fraction of the total amount of high level waste that must be disposed of in long term geological repositories. The decontamination and/or recovery and reuse of these materials would significantly reduce the amount of high level waste associated with light water nuclear energy reactors and could provide a new source of hafnium free zirconium for the fabrication of new nuclear components. A step in a strategy to recycle zirconium from used cladding materials is the direct, high yield chlorination reaction that produces zirconium tetrachloride (ZrCl{sub 4}). The ZrCl{sub 4} so obtained is contaminated with other metal chloride species (FeCl{sub 3}, NbCl{sub 5}, NbOCl{sub 3}, SnCl{sub 4}, CsCl, SbCl{sub 5}, etc.) that originate from the alloying metals present initially as well as contaminants from oxide layers on the cladding, trace fission products, fuel residues, activation byproducts, and tritium. The suggested strategy to remove the metal chloride impurities is based on sublimation at atmospheric pressure combined with chemical treatments influencing volatility of the impurities.

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DOE OSTI2018

Reporting the Radionuclide Inventory of the DWPF Product

In the Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS), the radionuclides contained in the liquid high-level waste currently stored at SRS are being converted into a durable borosilicate glass. This glass in its sealed stainless-steel canister, the DWPF product, eventually must be sent to a federal repository for final disposal. In order to ensure that the DWPF product is suitable for acceptance by the U. S. Department of Energy’s (DOE) Civilian Radioactive Waste Management System (CRWMS)*, the DOE Office of Environmental Management (DOE-EM) established the Waste Acceptance Product Specifications for Vitrified High-Level Waste Forms (WAPS). DOE-EM is tentatively performing surrogate CRWMS waste acceptance functions, as the office was eliminated in 2009, for review and concurrence of technical baseline documents and waste form non conformances. The specifications are divided into five sections, dealing with the waste form (borosilicate glass) itself, the canister, the canistered waste form, quality assurance, and documentation and other administrative requirements. The DWPF is required to document its compliance with the specifications in the Waste Form Compliance Plan (WCP), the Waste Form Qualification Report (WQR), the Production Records, and the Storage and Shipping Records. The WCP provides general information about the DWPF process and product, and a general description of the methods and programs by which the DWPF will demonstrate compliance with each specification in the WAPS. The WCP was vital to DWPF startup with respect to operations planning and also assurance to DOE that the canistered waste forms would be acceptable for disposal at any future High-Level Waste (HLW) geologic repository. The WQR is a compilation of the results of the testing and analysis programs identified in the WCP. The WQR details the method of compliance with each specification, and the testing performed to demonstrate the effectiveness of each method. The WQR is published in separate volumes which each correspond to one or more of the specifications. The WQR also contains a description of the DWPF’s Glass Product Control Program. Each volume contains Part and Item designators which indicate the corresponding item(s) in the WCP. The Production Records, and the Storage and Shipping Records document that each DWPF product has been produced and stored in compliance with the WAPS. This document, Volume 4 of the WQR, responds to WAPS Specifications 1.2.2, 1.6, and 3.14 which require that the DWPF report the radionuclide inventory of each canistered waste form, and of each waste type. This volume describes the systems the DWPF uses to determine and report the radionuclide inventory of the glass product, and provides evidence that these systems allow the DWPF to satisfy the WAPS specification. This volume of the WQR has been prepared to establish that methods are available to determine and report the radionuclide inventory, and that the DWPF is ready to collect the facility-specific data necessary to provide definitive estimates of the errors associated with the use of these methods.

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DOE OSTI2019

WIPP Operational and Safety Lessons Learned from the 2014 Fire and Radiological Events - 19389

The Waste Isolation Pilot Plant (WIPP) experienced two accident events in 2014 within 9 days of each other (salt haul truck fire and a radiological release). The repository was designed in the 1980's for high level waste and started operations in late 1990's for defense related transuranic (TRU) waste. Several long-standing technical issues from competing requirements between an underground facility (mine), nuclear safety, and environmental requirements lead to design, operations, and safety weaknesses that were not resolved prior to the two accident events. Other design issues and actions during early recovery efforts were identified as lessons learned for the Safety Significant Confinement Ventilation System (SSCVS) and Utility Shaft (US) capital asset projects and for future planning efforts. The infrastructure at WIPP was significantly degraded at the time of the events with key safety related items that had been out of service or not maintained for years. The emergency response to the two accident events was less than adequate and caused concerns with stakeholders. There are many operational and safety lessons learned from these two events and their corrective actions that will be valuable for all future planning of deep geological repositories (DGR). (authors)

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DOE OSTI2018

Preliminary Long-term Safety Assessment for the Planned LLW Disposal Facility at Al-Tuwaitha, Iraq - 18142

Before 1991, Iraq had a significant nuclear program which encompassed ten nuclear sites spread out across the country. The largest nuclear site was located at the Al-Tuwaitha site near Baghdad where 18 nuclear facilities were concentrated. During the first Gulf War in 1991, all sites suffered significant damage from bombing and subsequent looting. Currently, the Ministry of Science and Technology is responsible for the ten heavily damaged nuclear sites and for the management of radioactive waste in Iraq in general. The task of decommissioning the damaged nuclear facilities and managing the resulting waste is being supported by the International Atomic Energy Agency (IAEA), the European Commission (EC), and the United States (US). In the framework of its Instrument for Nuclear Safety Cooperation (INSC), the EC has launched a cooperation project to support the planned construction of an engineered repository for short-lived low- and intermediate level waste for the safe disposal of radioactive waste resulting from the decommissioning activities, as well as for waste from the continuing use of radioisotopes in medicine and the oil and gas industry in the country. The main objectives of this project, which was awarded to a Consortium led by NUKEM Technologies Engineering Services GmbH and joined by DBE Technology GmbH of Germany and JAVYS a.s. of Slovakia, are the development of an initial conceptual level basic design and preliminary safety assessment report (PSAR) and the subsequent detailed engineering design and supporting pre-construction safety assessment report (PCSAR). The current paper focuses on the development of the PSAR. Special focus is given to the long-term calculations and difficulties associated with the limited data base in regard to site characterization as well as the expected inventory for the future repository. Because of the ongoing security concerns in Iraq, the Ministry of Science and Technology had already selected the Al-Tuwaitha Site as the best suited location for the planned surface repository at the start of the project. Although some site characterization work had already been carried out prior to the start of the project, certain data for modelling the geology and hydrology of the site are still lacking. Missing data have been compensated by conservative assumptions and the assessment of alternative scenarios. Consequently, for the development of the simplified GoldSim{sup R} computer model used to carry out the long-term calculations supporting the PSAR, existing site information was used and, as appropriate, amended or replaced by conservative assumptions. Due to the nature of the waste, data on the expected inventory are associated with large uncertainties. Although certain estimates related to the future volume of the waste exist, little to no information is available on the expected radionuclide vector and respective activities. Therefore, the long-term calculations were carried out for a generic inventory including a broad range of radionuclides that are to be expected as being important considering the kind of waste to be disposed of in the facility. Based on the results of these calculations, the maximum total capacity of the facility was estimated and converted into activity limits for individual radionuclides that will be integrated into the existing general WAC for the facility. Compliance with these WAC will then guarantee the safety of the repository in regard to potential radionuclide releases via the groundwater pathway. In parallel to the determination of activity limits for the WAC, long-term calculations were carried using different estimates for the expected total activity to determine the general suitability of the proposed technical solution of the repository for receiving the total amount of Iraqi radioactive waste principally acceptable for surface disposal. (authors)

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DOE OSTI2017

Experiments and Modeling to Support Field Test Design

Disposition of heat-generating nuclear waste (HGNW) remains a continuing technical and sociopolitical challenge. We define HGNW as the combination of both heat generating defense high level waste (DHLW) and civilian spent nuclear fuel (SNF). Numerous concepts for HGNW management have been proposed and examined internationally, including an extensive focus on geologic disposal (c.f. Brunnengräber et al., 2013). One type of proposed geologic material is salt, so chosen because of its viscoplastic deformation that causes self-repair of damage or deformation induced in the salt by waste emplacement activities (Hansen and Leigh, 2011). Salt as a repository material has been tested at several sites around the world, notably the Morsleben facility in Germany (c.f. Fahland and Heusermann, 2013; Wollrath et al., 2014; Fahland et al., 2015) and at the Waste Isolation Pilot Plant (WIPP) near Carlsbad, NM. Evaluating the technical feasibility of a HGNW repository in salt is an ongoing process involving experiments and numerical modeling of many processes at many facilities.

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DOE OSTI2016

Geological Disposal of Nuclear Waste in Tuff: Yucca Mountain (USA) [Geological Disposal in Tuff: Yucca Mountain]

For more than three decades, the US Department of Energy has investigated the potential for permanent disposal of high-level radioactive waste and spent nuclear fuel in a deep-mined repository at Yucca Mountain, Nevada (USA). A detailed license application submitted to the US Nuclear Regulatory Commission in 2008 provides full documentation of the case for permanent disposal of nuclear waste in tuff. Furthermore, the aridity of the site and great depth to the water table provide a disposal environment and a design concept unique among deep-mined repositories currently or previously proposed worldwide.

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DOE OSTI2022

DECOVALEX-2019: An international collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems

The DECOVALEX Project is an international research collaboration for advancing the understanding and modeling of coupled thermo-hydro-mechanical-chemical (THMC) processes in geological systems. DECOVALEX stands for “DEvelopment of COupled Models and VALidation against EXperiments”. The creation of this international initiative, now running for almost 30 years, was motivated by the recognition that prediction of these coupled effects is an essential part of the performance and safety assessment of geologic disposal systems for radioactive waste and spent nuclear fuel, and also for a range of other sub-surface engineering activities. DECOVALEX emphasizes joint analysis and comparative modeling of state-of-the-art field and laboratory experiments, across a range of host rock options and repository designs. Participating research teams are from radioactive waste management organizations, national research institutes, regulatory agencies, universities, and consulting groups, providing a wide range of perspectives and solutions to these complex problems. The most recent phase of the DECOVALEX Project, here referred to as DECOVALEX-2019, started in 2016 and ended in 2019. Modeling teams from 13 international partner organizations participated in the comparative evaluation of seven modeling tasks involving complex field and/or laboratory experiments. Furthermore, this Virtual Special Issue on DECOVALEX-2019 provides an in-depth overview of these collaborative research efforts and how these have advanced the state-of-the-art of understanding and modeling coupled THMC processes.

58 GEOSCIENCES↗
DOE OSTI2017

Engineering-Scale Development/Demonstration of Zirconium Recovery from Used Duel Cladding

Recognizing that the zirconium (Zr) in used nuclear fuel (UNF) cladding is the second largest mass in UNF assemblies, process development studies for the recovery and purification of Zr were initiated and have been in progress at Oak Ridge National Laboratory (ORNL) for the last several years as a major element of waste minimization for advanced nuclear fuel recycle. Together with uranium recovery and recycle, Zr recovery would divert >90% (wt.) of the UNF assemblies from emplacement in a geologic repository by converting the Zr to low-level waste or reuse/recycle.

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DOE OSTI2020

Mineral-specific heterogeneous neptunium sorption onto geological repository rocks in oxic and anoxic conditions and various temperatures

Neptunium poses challenges for radioactive wastes management due to its long half-life and ingrowth from americium decay, as well as its high mobility in water in its oxidized forms. Np(V)-bearing aqueous solutions were contacted with polished and crushed gneiss and dolerite from the Yeniseisky site, Russia, which is under consideration as a location for an underground repository, both in oxic and anoxic conditions at 20 and 90 °C. Neptunium sorption on crushed gneiss and dolerite in oxic conditions at 20 °C was quite low, but increased substantially in anoxic conditions. Autoradiography on samples treated at 20 °C revealed that sorbed Np was associated mostly with dark colored iron-bearing minerals, and solvent extraction indicated partial reduction of Np(V) to Np(IV). Sorption of Np from aqueous solutions contacted with dolerite and gneiss at 90 °C was in all cases higher than at the lower temperature. Autoradiography of polished rock samples treated in anoxic conditions at 90 °C revealed that Fe-bearing minerals had 3–4 orders of magnitude more Np sorbed on them than the quartz and feldspar grains. X-ray photoelectron spectroscopy indicated this sorbed Np was present as NpO 2 . This study supports the concept that the geologic conditions present at the planned repository site will retard Np migration.

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DOE OSTI2016

Defense Waste Processing Facility (DWPF) Durability-Composition Models and the Applicability of the Associated Reduction of Constraints (ROC) Criteria for High TiO 2 Containing Glasses

Radioactive high-level waste (HLW) at the Savannah River Site (SRS) has successfully been vitrified into borosilicate glass in the DWPF since 1996. Vitrification requires stringent product/process (P/P) constraints since the glass cannot be reworked once it has been poured into ten foot tall by two foot diameter canisters. A unique “feed forward” statistical process control (SPC) was developed for this control rather than relying on statistical quality control (SQC). In SPC, the feed composition to the DWPF melter is controlled prior to vitrification. In SQC, the glass product would be sampled after it is vitrified. Individual glass property-composition models form the basis for the “feed forward” SPC. The models transform constraints on the melt and glass properties into constraints on the feed composition going to the melter in order to determine, at the 95% confidence level, that the feed will be processable and that the durability of the resulting waste form will be acceptable to a geologic repository. The DWPF SPC system is known as the Product Composition Control System (PCCS). One of the process models within PCCS is known as the Thermodynamic Hydration Energy Reaction MOdel (THERMO™). The DWPF will soon be receiving increased concentrations of TiO 2 -, Na 2 O-, and Cs 2 O-enriched wastes from the Salt Waste Processing Facility (SWPF). The SWPF has been built to pretreat the high-curie fraction of the salt waste to be removed from the HLW tanks in the F- and H-Area Tank Farms at the SRS. In order to validate the existing TiO 2 term in THERMO™ beyond 2.0 wt% in the DWPF, new durability data were developed over the target range of 2.00 to 6.00 wt% TiO 2 and evaluated against the 1995 durability model. The durability was measured by the 7-day Product Consistency Test. This study documents the adequacy of the existing THERMO™ terms. It is recommended that the modified THERMO™ durability models and the modified property acceptable region limits for the durability constraints be incorporated in the next revision of the technical bases for PCCS and then implemented into PCCS. It is also recommended that an reduction of constraints of 4 wt% Al 2 O 3 be implemented with no restrictions on the amount of alkali in the glass for TiO 2 values ≥2 wt%. The ultimate limit on the amount of TiO 2 that can be accommodated from SWPF will be determined by the three PCCS models, the waste composition of a given sludge batch, the waste loading of the sludge batch, and the frit used for vitrification.

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DOE OSTI2020

Engineered Barrier System R&D and International Collaborations – LANL (FY20): Spent Fuel and Waste Disposition

The United States Department of Energy’s Spent Fuel and Waste Disposition (SFWD) program is investigating the design and safety function of generic nuclear geologic repositories in a variety of geologic settings (salt, argillite, and crystalline rock). Different configurations and loadings of spent nuclear fuel and waste within disposal canisters are also being investigated, some of which have the potential to generate repository temperatures higher than previously considered (i.e., temperatures >100ºC) by foreign and domestic concepts. This report expands on engineered barrier material stability in a high temperature crystalline rock repository through high temperature hydrothermal experiments. Experiments were designed to develop engineered barrier system (EBS) concepts in a hightemperature crystalline environment in 1) bentonite-Grimsel Granodiorite interactions, 2) bentonite-cement reactions, and 3) interaction between waste canister materials and bentonite. Experiment results are applied to understanding long-term repository performance in terms of radionuclide isolation. One hydrothermal experiment was completed in the rocking autoclaves at LANL in FY-20: IEBS-6 (Grimsel Granodiorite + Wyoming bentonite + cured ordinary Portland cement + Grimsel Granodiorite synthetic groundwater, 250ºC/150 bar, 8 weeks). Several other experiments were planned but were delayed due to the COVID-19 pause in laboratory work. In addition, some characterization of the reaction products of experiments conducted in FY-20 was prevented by COVID-19. Mineral phase chemistry was not measured via electron microprobe analyses for IEBS-6. Quantitative X-ray diffraction results from IEBS-6 and HBT-1 were not completed. The missing analyses and discussion of the results will be included in next year’s report. New characterization that was completed includes scanning electron microscopy of reaction products from IEBS-6, quantitative X-ray diffraction results are presented from IEBS-1 through IBES-5, preliminary scanning electron microscope images and chemical analyses for IEBS-6, X-ray diffraction of the clay fraction from all experiments, measurement/imaging of mineral growth on the surface of steel coupons. Major observations pertaining to bentonite stability in a Grimsel Granodiorite environment include the stability of Na-montmorillonite at 250°C, the formation of trace CSH phases, and the formation of bentonite colloids on experiment cooling. The addition of a cured chip of Portland cement to the bentonite-Grimsel system results in slightly higher pH values and the formation of diverse secondary mineral phases that were not observed in the previous experiments (e.g., analcime, garronite, CSH phases). The new characterization efforts related to the interaction of stainless-steel coupons and bentonite clay focused on thickness and mineralogy of phases that formed at the steel surface. In Wyoming bentonite + Grimsel Granodiorite systems, newly formed minerals at the bentonitesteel coupon interface included alteration of the outermost steel edge to Fe,Cr-oxide phases, followed by Fe-rich phyllosilicates (Fe-saponite, chlorite) and interbedded Fe,Cr,Ni-sulfide phases (pentlandite). Hydrothermal experiments were completed to assess uranium-carbonate complexation at conditions relevant to high-temperature disposal. Autoclave solubility experiments were conducted at 150 to 250ºC with a range of carbonate and uranium concentrations. The experiment results were characterized via situ UV-Visible spectroscopy and synchrotron-based in situ XAS techniques. Results show a significant decrease in the stability of uranyl-carbonate complexes at temperatures above 100ºC along with the precipitation of uranium oxides. Further, at T > 200ºC, results show that uranyl-hydroxyl complexes control solubility of uranium instead of the previously predicted uranyl-carbonate species. These results are significant for understanding the mobility of uranium in the EBS, which will likely contain carbonate-rich fluids. International research efforts focused on three main areas: 1) participation in international conferences, 2) building collaborations with foreign repository programs, and 3) the initiation of an experimental program to complement the full-scale HotBENT test at the Grimsel test site. This experiment included Wyoming bentonite + low carbon steel + Grimsel Granodiorite synthetic groundwater and was run at the planned maximum temperature of the HotBENT test (200°C). Complete characterization of reaction products was hindered by disruptions to laboratory work but will be reported in the next FY. The experimental results obtained in FY-20 continue to document the wide-ranging effects of bulk composition and pressure-temperature conditions in the mineralogical and geochemical evolution of a high-temperature repository environment. Concepts developed will be used to inform models of long-term material stability in a generic crystalline rock-hosted repository.

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