Jove Colon, Carlos F.; Weck, Philippe F.; Hammond, Glenn E.; Kuhlman, Kristopher L.; Zheng, Liange; Rutqvist, Jonny; Kim, Kunhwi; Houseworth, James; Caporuscio, Florie A.; Cheshire, Michael; Palaich, Sarah; Norskog, Katherine E.; Zavarin, Mavrik; Wolery, Thomas J.; Jerden, James L.; Copple, Jacqueline M.; Cruse, Terry; Ebert, William L.
Deep geological disposal of nuclear waste in clay/shale/argillaceous rock formations has received much consideration given its desirable attributes such as isolation properties (low permeability), geochemically reduced conditions, slow diffusion, sorbtive mineralogy, and geologically widespread (Jové Colón et al., 2014). There is a wealth of gained scientific expertise on the behavior of clay/shale/ argillaceous rock given its focus in international nuclear waste repository programs that includes underground research laboratories (URLs) in Switzerland, France, Belgium, and Japan. Jové Colón et al. (2014) have described some of these investigative efforts in clay rock ranging from site characterization to research on the engineered barrier system (EBS). Evaluations of disposal options that include nuclear waste disposition in clay/shale/argillaceous rock have determined that this host media can accommodate a wide range of waste types. R&D work within the Used Fuel Disposition Campaign (UFDC) assessing thermal effects and fluid-mineral interactions for the disposition of heat-generating waste have so far demonstrated the feasibility for the EBS and clay host rock to withstand high thermal loads. This report represents the continuation of disposal R&D efforts on the advancement and refinement of coupled Thermal-Hydrological-Mechanical-Chemical (THMC), hydrothermal experiments on clay interactions, used fuel degradation (source term), and thermodynamic modeling and database development. The development and implementation of a clay/shale/argillite reference case described in Jové Colón et al. (2014) for FY15 will be documented in another report (Mariner et al. 2015) – only a brief description will be given here. This clay reference case implementation is the result of integration efforts between the GDSA PA and disposal in argillite work packages. The assessment of sacrificial zones in the EBS is being addressed through experimental work along with 1D reactive-transport and reaction path modeling. The focus of these investigations into the nature of sacrificial zones is to evaluate the chemical effects of heterogeneous chemical reactions at EBS interfaces. The difference in barrier material types and the extent of chemical reactions within these interfacial domains generates changes in mineral abundances. These mineralogical alterations also result in volume changes that, although small, could affect the interface bulk porosity. As in previous deliverables, this report is structured according to various national laboratory contributions describing R&D activities applicable to clay/shale/argillite media.
The structural, mechanical and thermodynamic properties of 1: 1 layered dioctahedral kaolinite clay, with ideal Al2Si2O5(OH)4 stoichiometry, were investigated using density functional theory corrected for dispersion interactions (DFT-D2). The bulk moduli of 56.2 and 56.0 GPa predicted at 298 K using the Vinet and Birch-Murnaghan equations of state, respectively, are in good agreement with the recent experimental value of 59.7 GPa reported for well-crystallized samples. The isobaric heat capacity computed for uniaxial deformation of kaolinite along the stacking direction reproduces calorimetric data within 0.7-3.0% from room temperature up to its thermal stability limit.
Jove Colon, Carlos F.; Weck, Philippe F.; Sassani, David H.; Zheng, Liange; Rutqvist, Jonny; Steefel, Carl I.; Kim, Kunhwi; Nakagawa, Seiji; Houseworth, James; Birkholzer, Jens; Caporuscio, Florie A.; Cheshire, Michael; Rearick, Michael S.; Mccarney, Mary K.; Zavarin, Mavrik; Benedicto, Ana; Kersting, Annie B.; Sutton, Mark; Jerden, James; Frey, Kurt E.; Copple, Jacqueline M.; Ebert, William
Radioactive waste disposal in shale/argillite rock formations has been widely considered given its desirable isolation properties (low permeability), geochemically reduced conditions, anomalous groundwater pressures, and widespread geologic occurrence. Clay/shale rock formations are characterized by their high content of clay minerals such as smectites and illites where diffusive transport and chemisorption phenomena predominate. These, in addition to low permeability, are key attributes of shale to impede radionuclide mobility. Shale host-media has been comprehensively studied in international nuclear waste repository programs as part of underground research laboratories (URLs) programs in Switzerland, France, Belgium, and Japan. These investigations, in some cases a decade or more long, have produced a large but fundamental body of information spanning from site characterization data (geological, hydrogeological, geochemical, geomechanical) to controlled experiments on the engineered barrier system (EBS) (barrier clay and seals materials). Evaluation of nuclear waste disposal in shale formations in the USA was conducted in the late 70’s and mid 80’s. Most of these studies evaluated the potential for shale to host a nuclear waste repository but not at the programmatic level of URLs in international repository programs. This report covers various R&D work and capabilities relevant to disposal of heat-generating nuclear waste in shale/argillite media. Integration and cross-fertilization of these capabilities will be utilized in the development and implementation of the shale/argillite reference case planned for FY15. Disposal R&D activities under the UFDC in the past few years have produced state-of-the-art modeling capabilities for coupled Thermal-Hydrological-Mechanical-Chemical (THMC), used fuel degradation (source term), and thermodynamic modeling and database development to evaluate generic disposal concepts. The THMC models have been developed for shale repository leveraging in large part on the information garnered in URLs and laboratory data to test and demonstrate model prediction capability and to accurately represent behavior of the EBS and the natural (barrier) system (NS). In addition, experimental work to improve our understanding of clay barrier interactions and TM couplings at high temperatures are key to evaluate thermal effects as a result of relatively high heat loads from waste and the extent of sacrificial zones in the EBS. To assess the latter, experiments and modeling approaches have provided important information on the stability and fate of barrier materials under high heat loads. This information is central to the assessment of thermal limits and the implementation of the reference case when constraining EBS properties and the repository layout (e.g., waste package and drift spacing). This report is comprised of various parts, each one describing various R&D activities applicable to shale/argillite media. For example, progress made on modeling and experimental approaches to analyze physical and chemical interactions affecting clay in the EBS, NS, and used nuclear fuel (source term) in support of R&D objectives. It also describes the development of a reference case for shale/argillite media. The accomplishments of these activities are summarized as follows: Development of a reference case for shale/argillite; Investigation of Reactive Transport and Coupled THM Processes in EBS: FY14; Update on Experimental Activities on Buffer/Backfill Interactions at elevated Pressure and Temperature; and Thermodynamic Database Development: Evaluation Strategy, Modeling Tools, First-Principles Modeling of Clay, and Sorption Database Assessment;ANL Mixed Potential Model For Used Fuel Degradation: Application to Argillite and Crystalline Rock Environments.
Within the Used Fuel Disposition Campaign (UFDC) of the United States Department of Energy Office of Nuclear Energy (DOE-NE), we have investigated used fuel (UF) degradation and radionuclide mobilization (UFD&RM) and implemented/produced a set of models encompassing radiolytic processes, UF matrix degradation, instant release fractions (IRF) of key radionuclides, and first-principles atomistic models for UO2 and its potential corrosion products. The goals of this collaborative effort (among three different national laboratories: Argonne National Laboratory [ANL]; Pacific Northwest National Laboratory [PNNLJ; and Sandia National Laboratories [SNL]) are to enhance the understanding of UF degradation processes and the technical bases for safety analyses in a range of generic disposal environments. In addition to these modeling efforts, integrated experimental studies are being conducted at both ANL and PNNL to evaluate and validate (and ultimately expand) process models for radiolytic phenomena and UF matrix degradation in various geologic disposal conditions. Integration and coupling of these process models into a generic performance assessment model (GPAM) is one focus of SNL efforts within the generic analyses of the Engineered Barrier System (EBS) for various repository environments. As discussed below, the present work has produced a set of models for implementation into the GPAM as an initial step towards an enhanced coupled model of source-term processes.