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Reduced diffusion and enhanced retention of multiple radionuclides from pore structure characterization of barrier materials for enhanced repository performance

Fluid flow and chemical transport in porous media are the macroscopic consequences of pore structure, which integrates geometry (e.g., pore size and surface area, pore-size distribution) and topology (e.g., pore connectivity). Low-permeability geological media whose pores are poorly interconnected will exhibit the characteristics of anomalous diffusion and sample size-dependent effective porosity, which will strongly impact long-term net diffusion and retention of radionuclides in geological repository settings involving different host rocks and barrier materials. A suite of innovative and complementary experimental approaches is utilized to study the microscopic pore structure and macroscopic fluid flow & chemical transport for a range of host rocks and barrier materials, in addition to standard clay minerals and reference rocks. With a particular focus on quantifying the presence and magnitude of “isolated” pores for a reduced effective porosity in low-permeability geomedia, the integrated methodologies for basic properties and pore structure characterization of these geomedia include X-ray diffraction, thin section petrography, grain size distribution, water immersion porosimetry after vacuum-pulling for full saturation, mercury intrusion porosimetry, nitrogen physisorption, scanning electron microscopy, X-ray computed tomography, and (ultra-)small angle neutron (X-ray) scattering. In addition, custom-designed gas diffusion, tracer recipe involving a range of anionic and cationic chemicals with subsequent analyses by laser ablation and inductively coupled plasma-mass spectrometry, along with batch sorption, column transport, and imbibition tests were conducted for coupled effects of pore structure and chemical retention/transport. From the perspectives of pore structure in conjunction with multiple and complementary approaches to examining a range of sample sizes under different observational scales, we find that the poor pore connectivity is prevalent in low-permeability media (mudstone and crystalline rock) that is related to geological processes (e.g., compaction, diagenesis and thermal maturation). For example, the deep and organic matter-rich mudstones have a much smaller effective porosity than the total porosity (as a result of poor pore connectivity) and associated diffusion coefficient, and the effective porosity & diffusion coefficients are also dependent upon the sample sizes used in the measurement. Similarly, most of the pore space in the shallow mudstone is also controlled by pore-throat diameters in the 5-50 nm range of intergranular pore types from its fine-grained nature, but with an overall good pore connectivity. However, the nm-sized pore space (physically pore-network architecture) and strong sorption capacities (chemical retention from clay minerals) of both shallow and deep mudstones lead to the synergistic retention of cationic radionuclides and their utilities as effective host rocks and barrier materials. Our unique approaches of studying how the micro-scale pore structure affect macro-scale fluid flow, diffusion & retention, and chemical transport produce improved mechanistic understanding, and realistic quantification, of diffusion and retention of typical radionuclides in a range of generic host rocks and barrier materials (clay/shale, salt, crystalline rock, and tuff), with the overall results leading to scientifically-based understanding of enhanced isolation (from both diffusion and retention) of radionuclides and improved confidence on the long-term performance of geological repository to store high-level radioactive wastes. In addition to the training of 25 undergraduates, graduates, and postdocs of UTA, the scientists (organizations) involved in performing this work (e.g., discussion, sample sharing, and operation of SANS and SAXS instruments) include Ed Matteo, Yifeng Wang, and Kristopher Kuhlman (Sandia National Laboratories), Jens Birkholzer, Liange Zheng, Tim Kneafsey, and Sharon Borglin (Lawrence Berkeley National Laboratory), Mavrik Zavarin (Lawrence Livermore National Laboratory), Yukio Tachi and Yuta Fukatsu (Japan Atomic Energy Agency), Mieke de Craen (Euridice, Belgium), Markus Bleuel (NIST), Wei-Ren Chen, Gergely Nagy, Changwoo Do, William Heller, Larry Anovitz, and Kenneth Littrell (ORNL), as well as Jan Illvsky, Ivan Kuzmenko, Ju-Sang Park and Jon Almers (ANL). Key deliverables include a total of 13 peer-reviewed journal articles (nine published and three under review), 23 presentations at scientific conferences (AAPG, AAPG Southwest Section, AGU, Asian Clay Conference, GSA, GSA South-Central Section, IHLRWM, InterPore, International Conference on Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphere, International Conference on Coupled Processes in Fractured Geological Media: Observation, Modeling and Application), and academic institutions (UTA, New Mexico State University; University of Poitiers, France; University of Helsinki, Finland; Uppsala University, Sweden; Istanbul Technical University, Turkey) and other organizations (Andra, France; Posiva Oy, Finland).

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GDSA Repository Systems Analysis Investigations in FY 2024

The Disposal Research and Development (R&D) Program of the US Department of Energy (DOE) office of Nuclear Energy (NE-8) Spent Fuel and Waste Science and Technology (SFWST) Campaign is to conduct R&D on disposal of spent nuclear fuel (SNF) and high-level waste (HLW). The goal of the Geologic Disposal Safety Assessment (GDSA) within this project is to develop a disposal system modeling and analysis capability that supports the integrated modeling of coupled processes controlling disposal system performance of deep geologic repositories, including uncertainty. This report describes specific activities in the Fiscal Year (FY) 2024 associated with the GDSA Repository Systems Analysis (RSA) work package. The overall objective of the GDSA RSA work package is to develop generic deep geologic repository concepts and repository system performance models in crystalline, argillite, salt, and unsaturated alluvium potential host-rock environments, and to simulate and analyze these generic repository concepts and models using GDSA Framework toolkit, and other tools as needed.

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Effects of time-dependent deformation of shale on the integrity of a geological nuclear waste repository

Safety assessment of geological nuclear waste repositories is essential for the permanent disposal of spent nuclear fuels and high-level radioactive waste. The long-term integrity of the host rock as well as the engineered barrier system (e.g., bentonite buffer) surrounding nuclear waste canisters is of particular importance as decay heat from nuclear waste canisters, which will last over thousands of years, significantly disturbs the thermo-hydromechanical (THM) state of the repository. In this study, THM coupled simulations were carried out to investigate the effect of time-dependent deformation (i.e., creep) of shale on the long-term integrity of a generic subsurface nuclear waste repository. The Norton-Bailey creep model, which is also known as the Lemaitre-Menzel-Schreiner model, was employed to simulate the power-law type creep that is observed in shales. The TOUGH-FLAC simulator was employed for the THM coupled modeling of the repository. The objective of this study is to assess the effect of creep in different shales (i.e., high creep shale vs. low creep shale) on long-term stress and permeability changes in the repository. Results show potential advantages of constructing repositories in the high creep shale, as deviatoric stress levels in the formation decreased to zero in 100 years since the emplacement of nuclear waste canisters and the permeability also decreased to the undamaged, intrinsic levels in 10,000 years. Also, mean effective stress levels in the bentonite buffer increased by 100% in the high creep shale case relative to the low creep shale case at 10,000 years due to creep-induced contraction of the nuclear waste disposal tunnel. However, in earlier periods (e.g., 1000 years), the stress levels in the bentonite buffer were twice smaller in the high creep shale case than in the low creep shale case, which shows a tradeoff between the intermediate- (~1000 years) and long-term (>10,000 years) compaction levels in the bentonite buffer depending on the creep characteristics of the host shale.

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Insert Modeling in UNF ST&DARDS

The Used Nuclear Fuel-Storage, Transportation & Disposal Analysis Resource and Data System (UNF-ST&DARDS) is a software tool that integrates a used nuclear fuel (UNF) or spent nuclear fuel (SNF) relational database and key analysis capabilities to simplify and automate numerous UNF management and fuel cycle–related activities. UNF-ST&DARDS is being developed for the US Department of Energy’s Office of Nuclear Energy Spent Fuel and Waste Disposition program. UNF-ST&DARDS provides an integrated framework that uses advanced modeling and simulation to predict the behavior of SNF over the timescales associated with permanent disposal in a geologic repository. After leaving the spent fuel pool, SNF is transferred to dry storage in a dual-purpose canister (DPC). DPCs are considered “dual purpose” because they are designed for both storage and transportation, removing the need to transfer the fuel to a separate transportation cask. However, much research has been conducted investigating the feasibility of directly disposing of DPCs in geologic repositories. Direct disposal of DPCs could reduce worker exposure during repackaging, reducing the amount of low-level waste from the discarded DPCs and potentially saving billions of dollars. Therefore, direct disposal of as-loaded DPCs is desirable if it can be done safely.

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Continuous removal of fission products from molten-salt-fueled reactors

A method based on separation of volatilized molten salt (MS) components, including by mass, is being developed to extract fission products (FPs) from operating molten-salt reactors. The initial application of this method is for accelerator-driven subcritical reactors fueled by (fluorinated molten salt) spent nuclear fuel (UNF) from any past, present, or future reactor. The actinides remain in the subcritical reactor to produce profitable energy and be transmuted while the extracted FPs can be buried without long-lived actinides such that a geologic repository is not necessarily needed to close the nuclear fuel cycle. By removing neutron-absorbing FPs and operating sub-critically, where the restrictive link between operation and criticality is broken, it is possible to envision complete burnup of the UNF fuel. The game-changing feature of continuously processing the molten salt inside the reactor while the reactor operates eliminates the need for a separate reprocessing plant. This feature also simultaneously improves the neutronics of the reactor, increasing the burnup of the fuel and extending its useful life for generating energy. Nuclear nonproliferation and need for geologic repositories are addressed by keeping actinides inside the reactor containment until they are consumed. (authors)

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A History of Hanford Tank Waste, Implications for Waste Treatment and Disposal

More than 40 years of plutonium processing have left almost 56 million gallons of mixed radioactive waste sequestered in 177 underground tanks on the Hanford Site. Three different processing technologies were employed for plutonium purification in addition to uranium scavenging and fission product removal from the tank waste. All of these chemical processes have contributed to a complex waste stream that varies from tank to tank that presents downstream processing challenges to render the waste into a safe form for long-term storage. The current disposition pathway for Hanford tank waste is vitrification. To maximize waste loading and minimize the number of high-level waste canisters stored in a geologic repository, pretreatment of the waste is required. Both pretreatment and vitrification operations are impacted by the waste composition.

Separations, filtration, ion exchange↗

Active sulfur cycling in the terrestrial deep subsurface

The deep terrestrial subsurface remains an environment where there is limited understanding of the extant microbial metabolisms. At Olkiluoto, Finland, a deep geological repository is under construction for the final storage of spent nuclear fuel. It is therefore critical to evaluate the potential impact microbial metabolism, including sulfide generation, could have upon the safety of the repository. As such, we investigated a deep groundwater where sulfate is present, but groundwater geochemistry suggests limited microbial sulfate-reducing activity. Examination of the microbial community at the genome-level revealed microorganisms with the metabolic capacity for both oxidative and reductive sulfur transformations. Deltaproteobacteria are shown to have the genetic capacity for sulfate reduction and possibly sulfur disproportionation, while Rhizobiaceae, Rhodocyclaceae, Sideroxydans, and Sulfurimonas oxidize reduced sulfur compounds. Further examination of the proteome confirmed an active sulfur cycle, serving for microbial energy generation and growth. Our results reveal that this sulfide-poor groundwater harbors an active microbial community of sulfate-reducing and sulfide-oxidizing bacteria, together mediating a sulfur cycle that remained undetected by geochemical monitoring alone. The ability of sulfide-oxidizing bacteria to limit the accumulation of sulfide was further demonstrated in groundwater incubations and highlights a potential sink for sulfide that could be beneficial for geological repository safety.

58 GEOSCIENCES↗

Structure and thermodynamics of calcium rare earth silicate oxyapatites, Ca 2 RE 8 (SiO 4 ) 6 O 2 (RE = Pr, Tb, Ho, Tm)

Calcium rare earth silicate oxyapatites, (Ca 2 RE 8 (SiO 4 ) 6 O 2 ), are of interest as components of glass-ceramic nuclear waste forms. To assess their long-term behavior in a geologic repository, it is essential to determine their structure and thermodynamic stability at relevant conditions. Here, in this work, we performed detailed structural and thermodynamic investigations on Ca 2 Pr 8 (SiO 4 ) 6 O 2 , Ca 2 Tb 8 (SiO 4 ) 6 O 2 , Ca 2 Ho 8 (SiO 4 ) 6 O 2 , and Ca 2 Tm 8 (SiO 4 ) 6 O 2 by high energy synchrotron powder X-ray diffraction combined with Rietveld analysis and high temperature oxide melt drop solution calorimetry. Enthalpies of formation from constituent oxides (ΔH f,ox ) were determined to be -765.1 ± 22.8 kJ/mol for Ca 2 Pr 8 (SiO 4 ) 6 O 2 ; -638.9 ± 20.5 kJ/mol for Ca 2 Tb 8 (SiO 4 ) 6 O 2 ; -643.3 ± 10.3 kJ/mol for Ca 2 Ho 8 (SiO 4 ) 6 O 2 ; and -403.2 ± 5.1 kJ/mol for Ca 2 Tm 8 (SiO 4 ) 6 O 2 . These thermodynamic parameters were used in assessing the thermochemical stability of these phases in the presence of water vapor from room temperature to 600 K, as encountered in the subsurface environments of a geological repository.

36 MATERIALS SCIENCE↗

Corrosion of 316 SS in direct contact with Zircaloy-4 in repository relevant conditions

The effects of interfacial contact between 316 stainless steel (316 SS) waste canister and spent fuel cladding material (Zircaloy-4) in case of water intrusion into a deep geological repository are investigated. Hydrothermal corrosion experiments of 316 SS and Zircaloy-4 in direct contact were performed at elevated temperatures in MilliQ water and simulated Mont Terri groundwater. Hematite, magnetite, chromite, and baddeleyite form as secondary phases. pH of the Mont Terri solution increases with corrosion duration and magnetite forms preferentially instead of hematite. Thermodynamic modeling shows that iron oxidation in 316 SS controls the pH and redox potential of the aqueous environment and is in good agreement with experimental Mont Terri results, showing that experimental Mont Terri results trend to equilibrium. All oxides except hematite are predicted to exist at thermodynamic equilibrium based on calculations, implying that experimentally formed hematite will be reduced or transformed to magnetite at equilibrium. The thermodynamically predicted chromite was observed to form only at the interface where 316 SS was in contact with Zircaloy-4 at 250°C, showing that contact with Zircaloy-4 seems to accelerate the 316 SS corrosion to thermodynamic equilibrium. Finally, Mont Terri groundwater readily trends towards thermodynamic equilibrium, leading to a pH and redox buffered system that is dominated by iron in solution coming from the accelerated corrosion of 316 SS caused by Zircaloy-4 contact.

316 stainless steel↗

GDSA Repository Systems Analysis Investigations (FY2020)

The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy Office of Nuclear Energy, Office of Spent Fuel and Waste Disposition (SFWD), has been conducting research and development on generic deep geologic disposal systems (i.e., geologic repositories). This report describes specific activities in the Fiscal Year (FY) 2020 associated with the Geologic Disposal Safety Assessment (GDSA) Repository Systems Analysis (RSA) work package within the SFWST Campaign. The overall objective of the GDSA RSA work package is to develop generic deep geologic repository concepts and system performance assessment (PA) models in several host-rock environments, and to simulate and analyze these generic repository concepts and models using the GDSA Framework toolkit, and other tools as needed.

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GDSA Repository Systems Analysis Investigations in FY2021

The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy Office of Nuclear Energy, Office of Spent Fuel and Waste Disposition (SFWD), has been conducting research and development on generic deep geologic disposal systems (i.e., geologic repositories). This report describes specific activities in the Fiscal Year (FY) 2021 associated with the Geologic Disposal Safety Assessment (GDSA) Repository Systems Analysis (RSA) work package within the SFWST Campaign. The overall objective of the GDSA RSA work package is to develop generic deep geologic repository concepts and system performance assessment (PA) models in several host-rock environments, and to simulate and analyze these generic repository concepts and models using the GDSA Framework toolkit, and other tools as needed.

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GDSA Repository Systems Analysis Investigations in FY2022

The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy Office of Nuclear Energy, Office of Spent Fuel and Waste Disposition (SFWD), has been conducting research and development on generic deep geologic disposal systems (i.e., geologic repositories). This report describes specific activities in the Fiscal Year (FY) 2022 associated with the Geologic Disposal Safety Assessment (GDSA) Repository Systems Analysis (RSA) work package within the SFWST Campaign. The overall objective of the GDSA RSA work package is to develop generic deep geologic repository concepts and system performance assessment (PA) models in several host-rock environments, and to simulate and analyze these generic repository concepts and models using the GDSA Framework toolkit, and other tools as needed.

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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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Recent Advances in Corrosion Science Applicable To Disposal of High-Level Nuclear Waste

High level radioactive waste is accumulating at temporary storage locations around the world and will eventually be placed in deep geological repositories. Many different types of geological formation are under consideration, but all will eventually allow water to contact the metallic waste containers considering that the period of performance required to allow sufficient decay of dangerous radionuclides is on the order of 105 – 106 years. Corrosion of the containers and waste forms in the aqueous repository environment is therefore a concern. This review describes the recent advances of the field of materials corrosion based on the work of the Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD) to address the issues associated with the long-term performance assessment and the design of materials with improved performance, where performance is defined as resistance to aqueous corrosion. Glass, crystalline ceramics, and metals are discussed separately, and then the near field interactions of these different materials classes are addressed. Recommendations for future directions are provided.

Frankel, Gerald↗

Surrogate Model Development of Spent Fuel Degradation for Repository Performance Assessment

In model simulations of deep geologic repositories, UO 2 fuel matrix degradation typically begins as soon as the waste package breaches and groundwater contacts the fuel surface. The initial degradation rate depends on the timing of these events, burnup of the fuel, temperature, and concentrations of dissolved reactants. Estimating the initial rate of degradation is fairly straightforward, but as UO 2 corrosion products precipitate on the fuel surface and the movement of dissolved species between the fuel surface and environment is impeded by the precipitated solids, the rate is more difficult to quantify. At that point, calculating the degradation rate becomes a reactive-transport problem in which a large number of equations must be solved by iteration for a large number of grid cells at each time step. The consequence is that repository simulations, which are already expensive, become much more expensive, especially when hundreds or thousands of waste packages breach. The Fuel Matrix Degradation (FMD) model is the process model of the Spent Fuel and Waste Science and Technology (SFWST) campaign of the US Department of Energy (DOE). It calculates spent fuel degradation rates as a function of radiolysis, redox reactions, electrochemical reactions, alteration layer growth, and diffusion of reactants through the alteration layer. Like other similar fuel degradation process models, it is a complicated model requiring a large number of calculations and iterations at each time step.

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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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Effects of anisotropic shale creep on the stress and permeability evolution of a geological nuclear waste repository

To ensure long-term safety and performance, geological nuclear waste repositories require low-permeability barriers such as bentonite buffers and/or shale host rock. Shale is not only known for its low permeability but also for its trend to undergo time-dependent deformation (i.e., creep), which could heal damage, but the effects of shale creep on the long-term performance of nuclear waste repositories have not been clearly understood. In particular, the anisotropic nature of shale (i.e., bedding) could have a significant effect on its creep behavior, and consequently, on the long-term performance of nuclear waste repositories. In this research, numerical simulations were carried out with the objective of showing the effects of anisotropic shale creep on the stress and permeability evolution of a generic geological nuclear waste repository in shale. The TOUGH-FLAC simulator, a thermo-hydromechanically (THM) coupled numerical code, was used for the simulations. To achieve the objective, comparisons were performed between the results of anisotropic shale creep simulations and those of different simulation cases, namely, no creep (i.e., elastic), isotropic creep, and long-term creep shale cases. Results of the comparisons show that the elastic and isotropic creep shale cases respectively led to the overestimation and underestimation of stress and permeability in the repository, whereas the long-term creep shale case, which accumulated greater creep in later periods than in earlier periods, helped to keep large shear and tensile stresses from developing while maintaining compressive spherical stress, resulting in consistently low permeability levels. These results indicate that performance assessments with elastic and isotropic creep formation models will provide the upper and lower bound estimates of stress and permeability, while more reasonable estimates will be given by an anisotropic creep formation model, and that shale with long-term creep characteristics will be beneficial in many aspects of the safety and performance of nuclear waste repositories.

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