Publications

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This report describes research and development (R&D) activities conducted during fiscal year 2019 (FY19) specifically related to the Engineered Barrier System (EBS) R&D Work Package in the Spent Fuel and Waste Science and Technology (SFWST) Campaign supported by the United States (U.S.) Department of Eneregy (DOE). The R&D activities focus on understanding EBS component evolution and interactions within the EBS, as well as interactions between the host media and the EBS. A primary goal is to advance the development of process models that can be implemented directly within the Genreric Disposal System Analysis (GDSA) platform or that can contribute to the safety case in some manner such as building confidence, providing further insight into the processes being modeled, establishing better constraints on barrier performance, etc.The FY19 EBS activities involved not only modeling and analysis work, but experimental work as well. The report documents the FY19 progress made in seven different research areas as follows: (1) thermal analysis for the disposal of dual purpose canisters (DPCs) in sedimentary host rock using the semianalytical method, (2) tetravalent uranium solubility and speciation, (3) modeling of high temperature, thermal-hydrologic-mechanical-chemical (THMC) coupled processes, (4) integration of coupled thermalhydrologic- chemical (THC) model with GDSA using a Reduced-Order Model, (5) studying chemical controls on montmorillonite structure and swelling pressure, (6) transmission x-ray microscope for in-situ nanotomography of bentonite and shale, and (7) in-situ electrochemical testing of uranium dioxide under anoxic conditions. The R&D team consisted of subject matter experts from Sandia National Laboratories, Lawrence Berkeley National Laboratory (LBNL), Los Alamos National Laboratory (LANL), Pacific Northwest National Laboratory (PNNL), the Bureau de Recherches Géologiques et Minières (BRGM), the University of California Berkeley, and Mississippi State University. In addition, the EBS R&D work leverages international collaborations to ensure that the DOE program is active and abreast of the latest advances in nuclear waste disposal. For example, the FY19 work on modeling coupled THMC processes at high temperatures relied on the bentonite properties from the Full-scale Engineered Barrier EXperiment (FEBEX) Field Test conducted at the Grimsel Test Site in Switzerland. Overall, significant progress has been made in FY19 towards developing the modeling tools and experimental capabilities needed to investigate the performance of EBS materials and the associated interactions in the drift and the surrounding near-field environment under a variety of conditions including high temperature regimes.

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The Waste Isolation Pilot Plant (WIPP) is a geologic repository for defense-related nuclear waste. If left undisturbed, the virtually impermeable rock salt surrounding the repository will isolate the nuclear waste from the biosphere. If humans accidentally intrude into the repository in the future, then the likelihood of a radionuclide release to the biosphere will depend significantly on the porosity and permeability of the repository itself. Room ceilings and walls at the WIPP tend to collapse over time, causing rubble piles to form on floors of empty rooms. The surrounding rock formation will gradually compact these rubble piles until they eventually become solid salt, but the length of time for a rubble pile to reach a certain porosity and permeability is unknown. This report details the first efforts to build models to predict the porosity and permeability evolution of an empty room as it closes. Conventional geomechanical numerical methods would struggle to model empty room collapse and rubble pile consolidation, so three different meshless methods, the Immersed Isogeometric Analysis Meshfree, Reproducing Kernel Particle Method (RKPM), and the Conformal Reproducing Kernel method, were assessed. First, the meshless methods and the finite element method each simulated gradual room closure, without ceiling or wall collapse. All three methods produced equivalent room closure predictions with comparable computational speed. Second, the Immersed Isogeometric Analysis Meshfree method and RKPM simulated two-dimensional empty room collapse and rubble pile consolidation. Both methods successfully simulated large viscoplastic deformations, fracture, and rubble pile rearrangement to produce qualitatively realistic results. In addition to geomechanical simulations, the flow channels in damaged salt and crushed salt were measured using micro-computed tomography, and input into a computational fluid dynamics simulation to predict the salt's permeability. Although room for improvement exists, the current simulation approaches appear promising.

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The failure of subsurface seals (i.e., wellbores, shaft and drift seals in a deep geologic nuclear waste repository) has important implications for US Energy Security. The performance of these cementitious seals is controlled by a combination of chemical and mechanical forces, which are coupled processes that occur over multiple length scales. The goal of this work is to improve fundamental understanding of cement-geomaterial interfaces and develop tools and methodologies to characterize and predict performance of subsurface seals. This project utilized a combined experimental and modeling approach to better understand failure at cement-geomaterial interfaces. Cutting-edge experimental methods and characterization methods were used to understand evolution of the material properties during chemo-mechanical alteration of cement-geomaterial interfaces. Software tools were developed to model chemo-mechanical coupling and predict the complex interplay between reactive transport and solid mechanics. Novel, fit-for-purpose materials were developed and tested using fundamental understanding of failure processes at cement- geomaterial interfaces. ACKNOWLEDGEMENTS The authors wish to acknowledge the Earth Sciences Research Foundation for their generous support over the last three years. In particular, we thank Erik Webb for his numerous suggestions, comments, feedback, and encouragement over the course of the project. There many who helped bring this project to fruition, including: Dave Borns, Steve Bauer, Pania Newell, Heeho Park, and Doug Blankenship. There are many support personnel who we thank for their valuable contributions to the logistics and business of management side of the project, including: Tracy Woolever, Libby Sanzero, and Nancy Vermillion.

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Microscale defects (microannuli) at the steel-cement and rock-cement interfaces are a major cause of failure in the integrity of wellbore systems. Microscale defects/microcracks as small as 30 μm are sufficient to create a significant leakage pathway for fluids. In this paper, the authors propose the use of nanomodified methyl methacrylate (NM-MMA) polymer as a seal material for 30-μm microcracks. Four materials were evaluated for their ability to serve as an effective seal material to seal 30-μm microcracks: microfine cement, epoxy, methyl methacrylate (MMA), and NM-MMA incorporating 0.5% by weight aluminum nanoparticles (ANPs). The seal materials' bond strengths with shale were investigated using push-out tests. In addition, the ability to flow fluid through the microcracks was investigated using sagittal microscopic images. Viscosity, surface tension, and contact angle measurements explain the superior ability of MMA seal materials to flow into very thin microcracks compared with other materials. Post-test analysis shows MMA repair materials are capable of completely filling the microcracks. In addition, incorporating ANPs in MMA resulted in significant improvement in seal material ductility. Dynamic mechanical analysis (DMA) showed that incorporating ANPs in MMA reduced the creep compliance and improved creep recovery of NM-MMA. X-ray diffraction (XRD) analysis shows that incorporating ANPs in MMA resin increases the degree of polymer crystallization, resulting in significant improvement in seal material ductility.

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In wellbores, cement plays an important role in wellbore integrity. As wells age and are stressed during their life cycle, the cement sheath may deform, altering its permeability and, perhaps compromising its integrity. In this study, we use flow measurements (calculated permeability) to provide real-time insight into damage incurred during triaxial deformation of neat cement. Cracks may be induced during deformation and their linkage may be sensed in the flow measurements. Conversely, cracks and pores may be closed during deformation, arresting fluid flow. We subjected room temperature specimens of neat Portland cement to confining pressures (0.7, 2.1, 13.8 MPa) and measured heliu m flow continuously during triaxial deformation. Axial displacement across a specimen was periodically halted to perhaps assure steady flow rate throughout the sample. We observed the apparent permeability to decrease from 0.8 to 0.7 to 0.2 μD with the imposed confining pressure increase. Each specimen, when subjected to differential stress, exhibited a slight decrease in apparent permeability, implying disconnects of flow paths. For the two lower confining pressures, apparent permeability began to increase just prior to macroscopic failure, suggesting microcrack linkage. For the 2.1 MPa confining pressure test, apparent permeability increased by a factor of three at macrofracture, and for the 0.7 MPa confining pressure test, apparent permeability increased by a factor of thirty at macrofracture. At 13.8 MPa confining pressure, apparent permeability only decreases during triaxial loading, implying that poroelastic compaction restricts flow pathways and connectivity of appropriately oriented cracks for axial flow decreases during deformation. Failure by macrofracture did not occur in this sample. Optical and scanning electron microscopy of deformed specimens indicate that pores and microcracks interact in complex manners, similar microcrack densities are observed in both 0.7 and 13.8 MPa test specimens, and pores represent both microcrack origination and localization sites. Larger pores (entrapped air voids) are sheared, flattened, and sites of crack opening. Micron-scale capillary porosity, determined using SEM image processing, is similar for all specimens. The results from these few experiments indicate that microfracturing of cement during triaxial deformation results in permeabilit y increases at low confining pressures. At the greater pressure, although microfracturing is observed, compaction and lack of microfracture interconnectivity have a greater effect on flow pathways, resulting in a permeability decrease during deformation.

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Our results show that a pseudo-boehmite precursor material can be chemically modified with divalent cationic species, for example, Nickel, to create an effective getter for anionic species. The viability of this novel class of materials is established by a variety of characterization methods, including surface area measurements, scanning electron microscopy, elemental analysis, and sorption capacity measurements. We will present the results of sorption capacity and surface area measurements that show the high sorption capacity of this novel class of getter materials. Our study shows that the divalent cation modification can increase the sorption capacity by as much as a factor of two.

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This document is a summary of the R&D activities associated with the Engineered Barrier Systems Work Package. Multiple facets of Engineered Barrier Systems (EBS) research were examined in the course of FY18 activities. This report is focused on delvering an update on the status and progress of modelling tools and experimental methods, both of which are essential to understanding and predicting long-term repository performance as part of the safety case. Specifically, the work described herein aims to improve understanding of EBS component evolution and interactions. Utlimately, the EBS Work Package is working towards producing process models for distinct processes that can either be incorporated into performance assessment (PA), or provide critical information for implementing better contraints on barrier performance The main objective of this work is that the models being developed and refined will either be implemented directly into the Genreric Disposal System Analysis platform (GDSA), or can otherwise be indirectly linked to the performance assessment by providing improved bounding conditions. In either the case, the expectation is that validated modelling tools will be developed that provide critical input to the safety case. This report covers a range of topics — modelling topics include: thermal-hydrologic-mechnicalchemical coupling (THMC) in buffer materials, comparisons of modelling approaches to optimize computational efficiency, thermal analysis for EBS/repository design, benchmarking of thermal analysis tools, and a preliminary study of buffer re-saturation processess. Experimental work reported, includes: chemical evolution and sorption behavior of clay-based buffer materials and high-pressure, high temperature studies of EBS material interactions. The work leverages international collaborations to ensure that the DOE program is active and abreast of the latest advances in nuclear waste disposal. This includes participation in the HotBENT Field Test, aimed at understanding near-field effects on EBS materials at temperatures above 100 °C, and the analysis of data and characterization of samples from the FEBEX Field Test. Both the FEBEX and HotBENT Field Tests utilize/utilized the Grimsel Test Site in Switzerland, which is situated in a granite host rock. These tests offer the opportunity to understand near field evolution of bentonite buffer at in situ conditions for either a relatively long timescale (18 years for FEBEX) or temperature above 100 °C (HotBENT). Overall, this report provides in depth descriptions of tools and capabilities to investigate nearfield performance of EBS materials (esp. bentonite buffer), as well as tools for drift-scale thermal and thermal-hydrologic analysis critical to EBS and repository design. For a more detailed description of work contained herein, please see Section 10 ("Conclusions") of this document.

Predicting chemical-mechanical fracture initiation and propagation in materials is a critical problem, with broad relevance to a host of geoscience applications including subsurface storage and waste disposal, geothermal energy development, and oil and gas extraction. In this project, we have developed molecular simulation and coarse- graining techniques to obtain an atomistic-level understanding of the chemical- mechanical mechanisms that control subcritical crack propagation in materials under tension and impact the fracture toughness. We have applied these techniques to the fracture of fused quartz in vacuum, in distilled water, and in two salt solutions - 1M NaC1, 1M NaOH - that form relatively acidic and basic solutions respectively. We have also established the capability to conduct double-compression double-cleavage experiments in an environmental chamber to observe material fracture in aqueous solution. Both simulations and experiments indicate that fractures propagate fastest in NaC1 solutions, slower in distilled water, and even slower in air.

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This project plan gives a high-level description of the US Department of Energy Office of Nuclear Energy (DOE-NE) Spent Fuel and Waste Disposition (SFWD) campaign in situ borehole heater test project being planned for the Waste Isolation Pilot Plant (WIPP) site This plan provides an overview of the schedule and responsibilities of the parties involved. This project is a collaborative effort by Sandia, Los Alamos, and Lawrence Berkeley National Laboratories to execute a series of small-diameter borehole heater tests in salt for the DOE-NE SFWD campaign. Design of a heater test in salt at WIPP has evolved over several years. The current design was completed in fiscal year 2017 (FY17), an equipment shakedown experiment is underway in April FY18, and the test implementation will begin in summer of FY18. The project comprises a suite of modular tests, which consist of a group of nearby boreholes in the wall of drifts at WIPP. Each test is centered around a packer-isolated heated borehole (5" diameter) containing equipment for water-vapor collection and brine sampling, surrounded by smaller-diameter (2" diameter) satellite observation boreholes. Observation boreholes will contain temperature sensors, tracer release points, electrical resistivity tomography (ERT) sensors, fiber optic sensing, and acoustic emission (AE) measurements, and sonic velocity sources and sensors. These satellite boreholes will also be used for plugging/sealing tests. The first two tests to be implemented will have the packer-isolated borehole heated to 120°C, with one observation borehole used to monitor changes. Follow-on tests will be designed using information gathered from the first two tests, will be conducted at other temperatures, will use multiple observation boreholes, and may include other measurement types and test designs.

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