Publications

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The amount of brine present in domal salt formation is far less than in bedded salts (e.g., 0.01 to 0.1% compared with 1 to 3%). In salt domes, shear deformation associated with diapirism has caused existing brine to coalesce, leading to flow and expulsion. Brine migration behavior was investigated in bedded salt at WIPP (Nowak and McTigue 1987, SAND87-0880), and in domal salt at Asse (Coyle et al. 1987, BMI/ONWI-624). Test methods were not standardized, and the tests involved large diameter boreholes (17 to 36 in. diameter) and large apparatus. The tested intervals were proximal to mined openings (within approximately 1 diameter) where in situ stresses are redistributed due to excavation. The tests showed that (1) brine inflow rates can range over at least 2 orders of magnitude for domal vs. bedded salt, (2) that brine inflow is strongly associated with clay and interbedded permeable layers in bedded salt, and (3) that measurement systems can readily collect very small quantities of moisture over time frames of 2 years or longer. Brine inflow rates declined slightly with time in both test series, but neither series approached a state of apparent depletion. This range of flow magnitude could be significant to repository design and performance assessment, especially if inflow rates can be predicted using stratigraphic and geomechanical inputs, and can be shown to approach zero in a predictable manner.

Deep Borehole Disposal (DBD) of radioactive waste has some clear advantages over mined repositories, including incremental construction and loading, enhanced natural barriers provided by deep continental crystalline basement, and reduced site characterization. Unfavorable features for a DBD site include upward vertical fluid potential gradients, presence of economically exploitable natural resources, presence of high permeability connection from the waste disposal zone to the shallow subsurface, and significant probability of future volcanic activity. Site characterization activities would encompass geomechanical (i.e., rock stress state, fluid pressure, and faulting), geological (i.e., both overburden and bedrock lithology), hydrological (i.e., quantity of fluid, fluid convection properties, and solute transport mechanisms), chemical (i.e., rock and fluid interaction), and socioeconomic (i.e., likelihood for human intrusion) aspects. For a planned Deep Borehole Field Test (DBFT), site features and/or physical processes would be evaluated using both direct (i.e., sampling and in-hole testing) and indirect (i.e., surface and borehole geophysical) methods for efficient and effective characterization. Surface-based characterization would be used to guide the exploratory drilling program, once a candidate DBFT site has been selected. Borehole based characterization will be used to determine the variability of system state (i.e., stress, pressure, temperature, petrology, and water chemistry) with depth, and to develop material and system parameters relevant for numerical simulation. While the site design of DBD could involve an array of disposal boreholes, it may not be necessary to characterize each borehole in detail. Characterization strategies will be developed in the DBFT that establish disposal system safety sufficient for licensing a disposal array.

While deep borehole disposal of nuclear waste should rely primarily on off-the-shelf technologies pioneered by the oil and gas and geothermal industries, the development of new science and technology will remain important. Key knowledge gaps have been outlined in the research roadmap for deep boreholes (B. Arnold et al, 2012, Research, Development, and Demonstration Roadmap for Deep Borehole Disposal, Sandia National Laboratories, SAND2012-8527P) and in a recent Deep Borehole Science Needs Workshop. Characterizing deep crystalline basement, understanding the nature and role of deep fractures, more precisely age-dating deep groundwaters, and demonstrating long-term performance of seals are all important topics of interest. Overlapping deep borehole and enhanced geothermal technology needs include: quantification of seal material performance/failure, stress measurement beyond the borehole, advanced drilling and completion tools, and better subsurface sensors. A deep borehole demonstration has the potential to trigger more focused study of deep hydrology, high temperature brine-rock interaction, and thermomechanical behavior.

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Options for disposal of the spent nuclear fuel and high level radioactive waste that are projected to exist in the United States in 2048 were studied. The options included four different disposal concepts: mined repositories in salt, clay/shale rocks, and crystalline rocks; and deep boreholes in crystalline rocks. Some of the results of this study are that all waste forms, with the exception of untreated sodium-bonded spent nuclear fuel, can be disposed of in any of the mined disposal concepts, although with varying degrees of confidence; salt allows for more flexibility in managing high-heat waste in mined repositories than other media; small waste forms are potentially attractive candidates for deep borehole disposal; and disposal of commercial SNF in existing dual-purpose canisters is potentially feasible but could pose significant challenges both in repository operations and in demonstrating confidence in long-term performance. Questions addressed by this study include: is a " 'one-size-fits-all ' repository a good strategic option for disposal?" and "do some disposal concepts perform significantly better with or without specific waste types or forms? " The study provides the bases for answering these questions by evaluating potential impacts of waste forms on the feasibility and performance of representative generic concepts for geologic disposal.

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An analysis of the Waste Isolation Pilot Plant (WIPP) colloid model constraints and parameter values was performed. The focus of this work was primarily on intrinsic colloids, mineral fragment colloids, and humic substance colloids, with a lesser focus on microbial colloids. Comments by the US Environmental Protection Agency (EPA) concerning intrinsic Th(IV) colloids and Mg-Cl-OH mineral fragment colloids were addressed in detail, assumptions and data used to constrain colloid model calculations were evaluated, and inconsistencies between data and model parameter values were identified. This work resulted in a list of specific conclusions regarding model integrity, model conservatism, and opportunities for improvement related to each of the four colloid types included in the WIPP performance assessment.

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The structures of the only known minerals containing peroxide, namely studtite [(UO 2)O 2(H 2O) 4] and metastudtite [(UO 2)O 2(H 2O) 2], have been investigated using density functional theory. The structure of metastudtite crystallizing in the orthorhombic space group Pnma (Z = 4) is reported for the first time at the atomic level and the computed lattice parameters, a = 8.45, b = 8.72, c = 6.75 Å, demonstrate that the unit cell of metastudtite is larger than previously reported dimensions (Z = 2) derived from experimental X-ray powder diffraction data. © 2012 The Royal Society of Chemistry.

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Published results of performance assessments for deep geologic disposal of high-level radioactive waste and spent nuclear fuel provide insight into those aspects of the waste form that are potentially important to the long-term performance of a repository system. Alternative waste forms, such as might result from new technologies for processing spent fuel and advances in nuclear reactor design, have the potential to affect the long-term performance of a geologic repository. This paper reviews relevant results of existing performance assessments for a range of disposal concepts and provides observations about how hypothetical modifications to waste characteristics (e.g., changes in radionuclide inventory, thermal loading, and durability of waste forms) might impact results of the performance assessment models. Disposal concepts considered include geologic repositories in both saturated and unsaturated environments. Specifically, we consider four recent performance assessments as representative of a range of disposal concepts. We examine the extent to which results of these performance assessments are affected by (i) thermal loading of the waste proposed for disposal; (ii) mechanical and chemical lifetime of the waste form; and (iii) radionuclide content of the waste. We find that peak subsurface temperature generally is a constraint that can be met through engineering solutions and that processing of wastes to reduce thermal power may enable more efficient use of repositories rather than improved repository performance. We observe that the rate of radionuclide release is often limited by geologic or chemical processes other than waste form degradation. Thus, the effects on repository performance of extending waste-form lifetime may be relatively small unless the waste form lifetime becomes sufficiently long relative to the period of repository performance. Finally, we find that changes to radionuclide content of waste (e.g., by separation or transmutation processes) do not in general correspond to proportional effects on repository performance. Rather, the effect of changes to radionuclide content depends on the relative mobility of various radionuclides through the repository system, and consequently on repository geology and geochemistry.

This report describes the progress in fiscal year 2010 in developing the Waste Integrated Performance and Safety Codes (IPSC) in support of the U.S. Department of Energy (DOE) Office of Nuclear Energy Advanced Modeling and Simulation (NEAMS) Campaign. The goal of the Waste IPSC is to develop an integrated suite of computational modeling and simulation capabilities to quantitatively assess the long-term performance of waste forms in the engineered and geologic environments of a radioactive waste storage or disposal system. The Waste IPSC will provide this simulation capability (1) for a range of disposal concepts, waste form types, engineered repository designs, and geologic settings, (2) for a range of time scales and distances, (3) with appropriate consideration of the inherent uncertainties, and (4) in accordance with robust verification, validation, and software quality requirements. Waste IPSC activities in fiscal year 2010 focused on specifying a challenge problem to demonstrate proof of concept, developing a verification and validation plan, and performing an initial gap analyses to identify candidate codes and tools to support the development and integration of the Waste IPSC. The current Waste IPSC strategy is to acquire and integrate the necessary Waste IPSC capabilities wherever feasible, and develop only those capabilities that cannot be acquired or suitably integrated, verified, or validated. This year-end progress report documents the FY10 status of acquisition, development, and integration of thermal-hydrologic-chemical-mechanical (THCM) code capabilities, frameworks, and enabling tools and infrastructure.

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This report evaluates the feasibility of high-level radioactive waste disposal in shale within the United States. The U.S. has many possible clay/shale/argillite basins with positive attributes for permanent disposal. Similar geologic formations have been extensively studied by international programs with largely positive results, over significant ranges of the most important material characteristics including permeability, rheology, and sorptive potential. This report is enabled by the advanced work of the international community to establish functional and operational requirements for disposal of a range of waste forms in shale media. We develop scoping performance analyses, based on the applicable features, events, and processes identified by international investigators, to support a generic conclusion regarding post-closure safety. Requisite assumptions for these analyses include waste characteristics, disposal concepts, and important properties of the geologic formation. We then apply lessons learned from Sandia experience on the Waste Isolation Pilot Project and the Yucca Mountain Project to develop a disposal strategy should a shale repository be considered as an alternative disposal pathway in the U.S. Disposal of high-level radioactive waste in suitable shale formations is attractive because the material is essentially impermeable and self-sealing, conditions are chemically reducing, and sorption tends to prevent radionuclide transport. Vertically and laterally extensive shale and clay formations exist in multiple locations in the contiguous 48 states. Thermal-hydrologic-mechanical calculations indicate that temperatures near emplaced waste packages can be maintained below boiling and will decay to within a few degrees of the ambient temperature within a few decades (or longer depending on the waste form). Construction effects, ventilation, and the thermal pulse will lead to clay dehydration and deformation, confined to an excavation disturbed zone within a few meters of the repository, that can be reasonably characterized. Within a few centuries after waste emplacement, overburden pressures will seal fractures, resaturate the dehydrated zones, and provide a repository setting that strongly limits radionuclide movement to diffusive transport. Coupled hydrogeochemical transport calculations indicate maximum extents of radionuclide transport on the order of tens to hundreds of meters, or less, in a million years. Under the conditions modeled, a shale repository could achieve total containment, with no releases to the environment in undisturbed scenarios. The performance analyses described here are based on the assumption that long-term standards for disposal in clay/shale would be identical in the key aspects, to those prescribed for existing repository programs such as Yucca Mountain. This generic repository evaluation for shale is the first developed in the United States. Previous repository considerations have emphasized salt formations and volcanic rock formations. Much of the experience gained from U.S. repository development, such as seal system design, coupled process simulation, and application of performance assessment methodology, is applied here to scoping analyses for a shale repository. A contemporary understanding of clay mineralogy and attendant chemical environments has allowed identification of the appropriate features, events, and processes to be incorporated into the analysis. Advanced multi-physics modeling provides key support for understanding the effects from coupled processes. The results of the assessment show that shale formations provide a technically advanced, scientifically sound disposal option for the U.S.

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