This report describes research and development (R&D) activities conducted during Fiscal Year 2022 (FY22) specifically related to the Engineered Barrier System (EBS) R&D Work Package in the Spent Fuel Waste Science and Technology (SFWST) Campaign supported by the United States (U.S.) Department of Energy (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. The R&D team represented in this report consists of individuals from Sandia National Laboratories, Lawrence Berkeley National Laboratory (LBNL), Los Alamos National Laboratory (LANL), and Vanderbilt University. EBS R&D work also leverages international collaborations to ensure that the DOE program is active and abreast of the latest advances in nuclear waste disposal.
Cryogenic plasma focused ion beam (PFIB) electron microscopy analysis is applied to visualizing ex situ (surface industrial) and in situ (subsurface geologic) carbonation products, to advance understanding of carbonation kinetics. Ex situ carbonation is investigated using NIST fly ash standard #2689 exposed to aqueous sodium bicarbonate solutions for brief periods of time. In situ carbonation pathways are investigated using volcanic flood basalt samples from Schaef et al. (2010) exposed to aqueous CO2 solutions by them. The fly ash reaction products at room temperature show small amounts of incipient carbonation, with calcite apparently forming via surface nucleation. Reaction products at 75° C show beginning stages of an iron carbonate phase, e.g., siderite or ankerite, common phases in subsurface carbon sequestration environments. This may suggest an alternative to calcite in carbonation low calcium-bearing fly ashes. Flood basalt carbonation reactions show distinct zonation with high calcium and calcium-magnesium bearing zones alternating with high iron-bearing zones. The calcium-magnesium zones are notable with occurrence of localized pore space. Oscillatory zoning in carbonate minerals is distinctly associated with far-from-equilibrium conditions where local chemical environments fluctuate via a coupling of reaction with transport. The high porosity zones may reflect a precursor phase (e.g., aragonite) with higher molar volume that then “ripens” to the high-Mg calcite phase-plus-porosity. These observations reveal that carbonation can proceed with evolving local chemical environments, formation and disappearance of metastable phases, and evolving reactive surface areas. Together this work shows that future application of cryo-PFIB in carbonation studies would provide advanced understanding of kinetic mechanisms for optimizing industrial-scale and commercial-scale applications.
Thermal-Hydrologic-Mechanical (THM) modeling of DECOVALEX 2023, Task C has continued. In FY2022 the simulations have progressed to Step 1, which is on 3-D modeling of the full-scale emplacement experiment at the Mont Terri Underground Rock Laboratory (Nagra, 2019). This report summarizes progress in Thermal-Hydrologic (TH) modeling of Step 1. THM modeling will be documented in future reports.
Dewers, Thomas D.; Reda-Taha, Mahmoud R.; Stormont, John C.; Pyrak-Nolte, Laura J.; Ahmadian, Mohsen A.; Chapman, David C.
Borehole cement is used across the range of energy technologies to stabilize casing, to serve as a barrier to behind-casing fluid movement. Cement debonding and other flaws, both at cement interfaces and within the cement itself, can create leakage pathways that can threaten safety to personnel, and wellbore performance, with economic and regulatory consequences. A primary method to assess cement health and wellbore integrity is via acoustic methods. This project was designed with three aims: demonstrate a significant improvement in the interpretation of cement acoustic behavior, both during curing, and in interpreting effects of flaws and evolving interfaces; develop sensor technologies to improve signal-noise ratios and cement acoustic responses; and lastly, provide a borehole demonstration of at least one of these technologies. We have accomplished the first two objectives, and the third, delayed by pandemic health concerns, is proceeding as of this writing via a technology partner with the University of Texas Advanced Energy Consortium.
This report describes research and development (R&D) activities conducted during fiscal year 2021 (FY21) 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 Energy (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 Generic 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.
Calcium-silicate-hydrate (C–S–H) represents a key microstructural phase that governs the mechanical properties of concrete at a large scale. Defects in the C–S–H phase are also responsible for the poor ductility and low tensile strength of concrete. Manipulating the microstructure of C–S–H can lead to new cementitious materials with improved structural performance. This paper presents an experimental investigation aiming to characterize a new synthetic polymer-modified synthetic calcium-silicate-hydrate (C–S–H)/styrene-butadiene rubber (SBR) binder. The new C–S–H/SBR binder is produced by calcining calcium carbonate and mixing this with fumed silica (SiO2), deionized water and SBR. Mechanical, physical, chemical and microstructural characterization was conducted to measure the properties of new hardened C–S–H binder. Results from the experimental investigation demonstrate the ability to engineer a new C–S–H binder with low elastic modulus and improved toughness and bond strength by controlling the SBR content and method of C–S–H synthesis. The new binder suggests the possible development of a new family of low-modulus silica-polymer binders that might fit many engineering applications such as cementing oil and gas wells.
Trujillo, Natasha; Rose-Coss, Dylan; Heath, Jason; Dewers, Thomas D.; Ampomah, William; Mozley, Peter S.; Cather, Martha
Leakage pathways through caprock lithologies for underground storage of CO2 and/or enhanced oil recovery (EOR) include intrusion into nano-pore mudstones, flow within fractures and faults, and larger-scale sedimentary heterogeneity (e.g., stacked channel deposits). To assess multiscale sealing integrity of the caprock system that overlies the Morrow B sandstone reservoir, Farnsworth Unit (FWU), Texas, USA, we combine pore-to-core observations, laboratory testing, well logging results, and noble gas analysis. A cluster analysis combining gamma ray, compressional slowness, and other logs was combined with caliper responses and triaxial rock mechanics testing to define eleven lithologic classes across the upper Morrow shale and Thirteen Finger limestone caprock units, with estimations of dynamic elastic moduli and fracture breakdown pressures (minimum horizontal stress gradients) for each class. Mercury porosimetry determinations of CO2 column heights in sealing formations yield values exceeding reservoir height. Noble gas profiles provide a “geologic time-integrated” assessment of fluid flow across the reservoir-caprock system, with Morrow B reservoir measurements consistent with decades-long EOR water-flooding, and upper Morrow shale and lower Thirteen Finger limestone values being consistent with long-term geohydrologic isolation. Together, these data suggest an excellent sealing capacity for the FWU and provide limits for injection pressure increases accompanying carbon storage activities.
This report summarizes the FY21 Activities for EBS International Collaborations Work Package. The international collaborations work packages aim to leverage knowledge, expertise, and tools from the international nuclear waste community, as deemed relevant according to SFWST “roadmap” priorities. This report describes research and development (R&D) activities conducted during fiscal year 2021(FY21) 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 Energy (DOE). It fulfills the SFWST Campaign deliverable M4SF- 21SN010308062. The R&D activities described in this report 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 Generic 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. Sandia National Laboratories is participating in THM modeling in the international projects EBS Task Force and DECOVALEX 2023. EBS Task Force, Task 11 is on modeling of laboratory-scale High Temperature Column Test conducted at Lawrence Berkeley National Laboratory. DECOVALEX 2023, Task C is on THM modeling of the full-scale emplacement experiment (FE experiment) at the Mont Terri Underground Rock Laboratory, Switzerland. This report summarizes Sandia’s progress in the modeling studies of DECOVALEX 2023, Task C. Modeling studies related to the High Temperature Column Test will be documented in future reports.
Vemuganti, S.; Stormont, J.C.; Pyrak-Nolte, L.J.; Dewers, Thomas D.; Reda Taha, M.M.
Cement is widely used in wellbores to stabilize the steel casing used in wellbore operations for oil and gas production, enhanced geothermal systems and carbon sequestration, and to limit fluid movement between sub-surface strata. Flaws such as microcracks in wellbore cement can lead to leakage along the wellbore compromising wellbore integrity. There is an increasing need for methods to monitor cement crack propagation in wellbore environments. In this study, we develop and report the first cementitious sensors capable of exhibiting high frequency acoustic bandgaps (ABGs) using carbon nanotubes (CNTs). Computational simulations of a sensor unit cell are used to design cement-multi walled carbon nanotubes (MWCNTs) sensors that show a wide bandgap. When the cement-MWCNTs sensors is embedded in cement specimens, bandgaps were measured experimentally under 300 kHz and under 600 kHz, consistent with the computationally predicted bandgaps in the range of 290–360 kHz, 410–460 kHz and 515–585 kHz. These bandgap features were absent in homogeneous cement specimens. X-ray tomographic reconstructions showed microscopic debonding at cement-MWCNTs sensor interface. Frequency response analysis of a three-dimensional computational model indicated a shift of frequency of minimum transmission due to the interface debonding, but no perturbation of bandgap response was observed. The cement-MWCNTs sensors developed in this study show the potential of a packed CNT inclusion material in cementitious matrix to create ABGs in a cement matrix.
This report describes research and development (R&D) activities conducted during fiscal year 2020 (FY20) 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 Energy (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 Generic 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 FY20 EBS activities involved not only modeling and analysis work, but experimental work as well. Despite delays to some planned activities due to COVID-19 precautions, progress was made during FY20 in multiple research areas and documented in this report as follows: (1) EBS Task Force: Task 9/FEBEX Modeling Final Report: Thermo-Hydrological Modeling with PFLOTRAN, (2) preliminary sensitivity analysis for the FEBEX in-situ heater test, (3) cement-carbonate rock interaction under saturated conditions: from laboratory to modeling, (4) hydrothermal experiments, (5) progress on investigating the high temperature behavior of the uranyl-carbonate complexes, (6) in-situ and electrochemical work for model validation, (7) investigation of the impact of high temperature on EBS bentonite with THMC modeling, (8) sorption and diffusion experiments on bentonite, (9) chemical controls on montmorillonite structure and swelling pressure, (10) microscopic origins of coupled transport processes in bentonite, (11) understanding the THMC evolution of bentonite in FEBEX-DP—coupled THMC modeling, (12) modeling in support of HotBENT, an experiment studying the effects of high temperatures on clay buffers/near-field, and (13) high temperature heating and hydration column test on bentonite.
This report outlines Sandia National Laboratories modeling studies applied to Stage 1 and Stage 2 of the Full-scale Engineered Barriers Experiment in Crystalline Host Rock (FEBEX) in situ test for the SKB EBS Task Force Task 9. The FEBEX test was a full-scale test conducted over ~18 years at the Grimsel, Switzerland Underground Research Laboratory (URL) managed by NAGRA. It involved emplacing simulated waste packages, in the form of welded cylindrical heaters, inside a tunnel in crystalline granitic rock and surrounded by a bentonite barrier and cement plug. Sensors emplaced within the bentonite monitored the wetting-up, heating, and drying out of the bentonite barrier, and the large resulting data set provides an excellent opportunity for validation of multiphysics Thermal-Hydrological (TH), Thermal-Hydrologic-Chemical (THC), and Thermal-Hydrological-Mechanical (THM) modeling approaches for underground nuclear waste storage and the performance of engineered bentonite barriers. The present status of the EBS Task Force is finalizing Task 9, which follows years of modeling studies of the FEBEX test, by many notable modeling teams (Gens et al., 2009; Sanchez et al. 2010; 2012; Samper et al., 2018). These modeling studies generally use two-dimensional axisymmetric meshes, ignoring threedimensional effects, gravity and asymmetric wetting and dry out of the bentonite engineered barrier. This study investigates these effects with use of the PFLOTRAN THC code with massively parallel computational methods in modeling FEBEX Stage 1 and Stage 2 results. The PFLOTRAN numerical code is an open source, state-of-the-art, massively parallel subsurface flow and reactive transport code operating in a high-performance computing environment (Hammond et al., 2014). Section 2 describes the applied partial differential equations describing mass, momentum and energy balance used in this study, considerations derived by assuming phase equilibrium between gas and liquid phases, constitutive equations for granite, cement plug, and bentonite domains, and specific approaches for use inthe PFLOTRAN code. Section 3 describes the geometry, meshing, and model set-up. Section 4 describes modeling results, Section 5 compares modeling results to field testing data, and Section 6 gives conclusions. The Appendix provides detailed information required by the EBSTask Force for final reporting.
Geomechanics experiments were used to assess mechanical alteration of Boise Sandstone promoted by reactions with supercritical carbon dioxide (scCO2) and water vapor. During geologic carbon storage, scCO2 is injected into subsurface reservoirs, forming buoyant plumes. At brine-plume interfaces, scCO2 can dissolve into native brines, and water from brines can partition into scCO2, forming hydrous scCO2. This study investigates the effect of hydrous scCO2 on the strength of Boise Sandstone. Samples are first exposed to recirculating hydrous scCO2 for 24 h at 70 °C and 13.8 MPa scCO2 pressure. Samples are reacted with scCO2 with added water contents up to 500 mL. After scCO2 exposure, samples are deformed at room temperature under confining pressures of 3.4, 6.9, and 10.3 MPa. The results demonstrate that hydrous scCO2 induces chemical reactions in Boise Sandstone, with ions migrating from the solid into the hydrous scCO2 phase. At the longer time-scales, these reactions could lead to mechanical weakening in the samples; however, on the scale of our experiments, the strength changes are within sample variability. Because the solubility of water in scCO2 is extremely low (0.008 mol H2O per 1 mol CO2), the mineral dissolution of Boise Sandstone was under 0.002 wt.%. Additionally, mineral grains and pore throats in Boise Sandstone are cemented with quartz, which is not susceptible to dissolution at these conditions. Our results indicate that humidity in scCO2 plumes is unlikely to sustain chemical reactions and induce long term strength changes in quartz cemented sandstones due to resistant mineralogies and low water solubility.
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.
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.
Measuring the size and orientation of borehole breakouts is one of the primary methods for determining the orientation and magnitudes of the in situ stresses in the subsurface. To better understand the effects of anisotropy on borehole breakouts, experiments were conducted on Mancos Shale, a finely laminated mudrock. A novel testing configuration was developed to conduct borehole breakout experiments in a standard triaxial vessel and load frame. Samples were prepared at three different orientations and deformed under 6.9 to 20.7 MPa confining pressure. The results show a variation of peak strength and breakout geometry depending on the lamination orientation. Samples deformed parallel to laminations failed at a higher maximum compressive stress than samples deformed perpendicular to laminations, which were stronger than inclined samples. These relationships are quantified by a cosine-based failure envelope. Observed breakout shapes in perpendicular samples are V-shaped and symmetric around the borehole, which advance as a series of fractures of increasing size into the sidewalls. In inclined samples, fractures form along weaker laminations planes and grow in an en echelon pattern towards the axial stress direction. In parallel samples, long fractures grow from the wellbore towards the axial stress direction. The observed geometries highlight potential sources of error in calculating in situ stresses from borehole breakouts.
Pore structure is an important parameter to quantify the reservoir rock adsorption capability and diffusivity, both of which are fundamental reservoir properties to evaluate the gas production and carbon sequestration potential for coalbed methane (CBM) and shale gas reservoirs. In this study, we applied small-angle neutron scattering (SANS) to characterize the total and accessible pore structures for two coal and two shale samples. We carried out in situ SANS measurements to probe the accessible pore structure differences under argon, deuterated methane (CD 4 ), and CO 2 penetrations. The results show that the total porosity ranges between 0.25 and 5.8% for the four samples. Less than 50% of the total pores are accessible to CD 4 for the two coals, while more than 75% of the pores were found to be accessible for the two shales. This result suggests that organic matter pores tend to be disconnected compared to mineral matter pores. Argon pressurization can induce pore contraction because of the mechanical compression of the solid skeleton in both the coal and shale samples. Hydrostatic compression has a higher effect on the nanopores of coal and shale with a higher accessible porosity. Both methane and CO 2 injection can reduce the accessible nanopore volume due to a combination of mechanical compression, sorption-induced matrix swelling, and adsorbed molecule occupation. CO 2 has higher effects on sorption-induced matrix swelling and pore filling compared to methane for both the coal and shale samples. Gas densification and pore filling could occur at higher pressures and smaller pore sizes. In addition, the compression and adsorption could create nanopores in the San Juan coal and Marcellus shale drilled core but could have an opposite effect in the other samples, namely, the processes could damage the nanopores in the Hazleton coal and Marcellus shale outcrop.
The success of geological carbon storage (GCS) depends on the sealing properties of caprocks, typically mudrocks, and their laminated variety – shales. In this study, we examined mineralogical changes in carbonate-rich Mancos Shale and corresponding changes in micro-mechanical properties following the reaction with carbon dioxide (CO2). Mineralogical changes of Mancos Shale depended on the pressure of CO2 during its exposure to the CO2-brine mixtures for up to 8 weeks. Dedolomitization was observed in the reactors pressurized with 100 psi of CO2, combined with the precipitation of gypsum. In the reactor pressurized with 2500 psi of CO2, the complete dissolution of calcite, partial dissolution of dolomite, and precipitation of magnesite and anhydrite were observed. Localized mechanical weakening was observed only for dolomite-muscovite-illite-rich laminae following whole shale puck alteration at 2500 psi of CO2, and a decrease of up to 50 ± 20% in scratch toughness was observed. The quartz-calcite-rich laminae did not exhibit a measurable difference in scratch toughness before and after reaction in CO2-rich brine. The predicted changes in mineralogy, porosity, density, and hardness of Mancos Shale are limited, according to the geochemical models describing alteration of shale by CO2-rich brine lasting for 5000 years. This study illustrates a coupled and localized chemical-mechanical response of caprock to the injection of CO2.
Bedrock fracture is a key element of rock erosion and subsequent surface processes. Here, we test the hypothesis that rock's susceptibility to subcritical cracking, a specific type of fracturing, significantly drives and limits rock erosion. We measured 10Be-derived erosion rates, compressive strength, and crack characteristics on 20 outcrops of different rock units (quartzite, granite, and two metasandstones) in the northern Blue Ridge Mountains of Virginia (USA). We also measured the subcritical cracking index (n), Charles's law velocity constant (A), and fracture toughness (KIC) of samples from four of the same outcrops, representative of each rock type. Erosion rates range from 1.16 ± 0.67 to 32.3 ± 7.8 m/m.y. We find strong correlations- across the four rock units-between average erosion rates and the three subcritical cracking parameters (R2 > 0.85, p < 0.05), but not compressive strength (R2 = 0.6; p > 0.1). We also find a correlative relationship between n and outcrop fracture length (R2 = 0.91; p < 0.05). The latter correlation is consistent with that of published model predictions, further indicating a mechanistic link between subcritical cracking and rock erosion. We infer that subcritical cracking parameters closely tie to erosion rates, because subcritical cracking is the dominant process of mechanical weathering, leading to positive feedbacks relating subcritical cracking rates, crack length, porosity, and water accessibility. These data are the first that directly test and support the hypothesis that subcritical cracking can set the pace of long-term rock erosion.
Espinoza, D.N.; Jung, Hojung; Major, Jonathan R.; Sun, Zhuang; Ramos, Matthew J.; Eichhubl, Peter; Balhoff, Matthew T.; Choens, R.C.; Dewers, Thomas D.
CO2 geological storage in saline aquifers results in acidification of resident brine. Chemical reactions between acidified brine and rock minerals lead to dissolution and precipitation of minerals at various time scales. Mineral dissolution and precipitation are often neglected in assessing the mechanical integrity of target storage formations, yet, changes in rock strength and deformational behavior can impact trapping mechanisms. This study shows the impact of exposure to CO2-charged brine on shear strength and stiffness of various outcrop rocks evaluated through triaxial testing. The tested rocks were exposed to CO2-charged brine over geological time at a naturally occurring near-surface seepage along the Little Grand Wash Fault and Salt Wash Grabens, which include the Crystal Geyser site near the town of Green River, Utah. Prior work suggests that this site provides a near-surface structural analog for possible fault-controlled CO2 leakage over time scales that exceed expected injection time scales (10–100 years). Results show mechanical alteration in various aspects: (1) CO2-charged brine alteration at near-surface conditions results in mineral dissolution/precipitation and reduction of shear strength and brittleness of Entrada sandstone and Summerville siltstone samples, and (2) carbonate precipitation in fractured Mancos shale leads to matrix stiffening and fracture mineralization resulting in overall stiffer and likely tighter shale. Additional discrete element simulations coupled with a bonded-particle-model confirm the role of cement bond size alteration as one of the main controls for rock chemo-mechanical alteration in sandstones. The chemo-mechanical alteration path that mimics cement dissolution (under stressed subsurface conditions) results in vertical compaction and lateral stress relaxation. Overall, results show that rock exposure to CO2-charged brine can impart distinct petrophysical and geomechanical changes according to rock lithology and location with respect to major CO2 conduits. While mineral dissolution in the storage rock may result in undesired reservoir strains and changes of stresses, mineral precipitation downstream from a leakage path can help seal potentially induced fractures.
Desirable outcomes for geologic carbon storage include maximizing storage efficiency, preserving injectivity, and avoiding unwanted consequences such as caprock or wellbore leakage or induced seismicity during and post injection. To achieve these outcomes, three control measures are evident including pore pressure, injectate chemistry, and knowledge and prudent use of geologic heterogeneity. Field, experimental, and modeling examples are presented that demonstrate controllable GCS via these three measures. Observed changes in reservoir response accompanying CO2 injection at the Cranfield (Mississippi, USA) site, along with lab testing, show potential for use of injectate chemistry as a means to alter fracture permeability (with concomitant improvements for sweep and storage efficiency). Further control of reservoir sweep attends brine extraction from reservoirs, with benefit for pressure control, mitigation of reservoir and wellbore damage, and water use. State-of-the-art validated models predict the extent of damage and deformation associated with pore pressure hazards in reservoirs, timing and location of networks of fractures, and development of localized leakage pathways. Experimentally validated geomechanics models show where wellbore failure is likely to occur during injection, and efficiency of repair methods. Use of heterogeneity as a control measure includes where best to inject, and where to avoid attempts at storage. An example is use of waste zones or leaky seals to both reduce pore pressure hazards and enhance residual CO2 trapping.
A novel experimental geometry is combined with acoustic emission monitoring capability to measure crack growth and damage accumulation during laboratory simulations of borehole breakout. Three different experiments are conducted in this study using Sierra White Granite. In the first experiment, the sample is deformed at a constant 17.2 MPa confining pressure without pore fluids; in the second experiment, the sample is held at a constant effective pressure of 17.2 MPa with a constant pore pressure; and in the third experiment, pore pressure is modified to induce failure at otherwise constant stress. The results demonstrate that effective pressure and stress path have controlling influence on breakout initiation and damage accumulation in laboratory simulations of wellbore behavior. Excellent agreement between the dry test and constant pore pressure test verify the application of the effective pressure law to borehole deformation. Located AE events coincide with post-test observations of damage and fracture locations. Comparison of AE behavior between the experiments with pore pressure show that breakouts develop prior to peak stress, and continued loading drives damage further into the formation and generates shear fractures.
Results of axisymmetric compression tests on weak, porous Castlegate Sandstone (Cretaceous, Utah, USA), covering a range of dilational and compactional behaviors, are examined for localization behavior. Assuming isotropy, bulk and shear moduli evolve as increasing functions of mean stress and Mises equivalent shear stress respectively, and as decreasing functions of work-conjugate plastic strains. Acoustic emissions events located during testing show onset of localization and permit calculation of observed shear and low-angle compaction localization zones, or bands, as localization commences. Total strain measured experimentally partitions into: A) elastic strain with constant moduli, B) elastic strain due to stress dependence of moduli, C) elastic strain due to moduli degradation with increasing plastic strain, and D) plastic strain. The third term is the elastic-plastic coupling strain, and though often ignored, contributes significantly to pre-failure total strain for brittle and transitional tests. Constitutive parameters and localization predictions derived from experiments are compared to theoretical predictions. In the brittle regime, predictions of band angles (angle between band normal and maximum compression) demonstrate good agreement with observed shear band angles. Compaction localization was observed in the transitional regime in between shear localization and spatially pervasive compaction, over a small range of mean stresses. In contrast with predictions, detailed acoustic emissions analyses in this regime show low angle, compaction-dominated but shear-enhanced, localization.
A series of constant mean stress (CMS) and constant shear stress (CSS) tests were performed to investigate the evolution of permeability and Biot coefficient at high mean stresses in a high porosity reservoir analog (Castlegate sandstone). Permeability decreases as expected with increasing mean stress, from about 20 Darcy at the beginning of the tests to between 1.5 and 0.3 Darcy at the end of the tests (mean stresses up to 275 MPa). The application of shear stress causes permeability to drop below that of a hydrostatic test at the same mean stress. Results show a nearly constant rate decrease in the Biot coefficient as the mean stress increases during hydrostatic loading, and as the shear stress increases during CMS loading. CSS tests show a stabilization of the Biot coefficient after the application of shear stress.
Greater Aneth oil field, Utah’s largest oil producer, was discovered in 1956 and has produced over 483 million barrels of oil. Located in the Paradox Basin of southeastern Utah, Greater Aneth is a stratigraphic trap producing from the Pennsylvanian (Desmoinesian) Paradox Formation. Because Greater Aneth is a mature, major oil field in the western U.S., and has a large carbonate reservoir, it was selected to demonstrate combined enhanced oil recovery and carbon dioxide storage. The Aneth Unit in the northwestern part of the field has produced over 160 million barrels of the estimated 386 million barrels of original oil in place—a 42% recovery rate. The large amount of remaining oil made the Aneth Unit ideal to enhance oil recovery by carbon dioxide flooding and demonstrate carbon dioxide storage capacity.
A series of tests have been performed on Sierra White granite subjected to general (true triaxial) states of stress. Tests were performed under constant Lode angle conditions at Lode angles of 23.4, 16.1 and 0°. The constant Lode angle condition was maintained by holding the minimum principal stress constant while increasing the maximum and intermediate principal stress at a predetermined ratio. Tests were performed at minimum principal stresses of 5, 17 and 30 MPa. All of the specimens failed in a brittle manner, with significant dilatant volume strain accumulated, and failure showed a strong dependence on Lode angle. Specimens behaved in a nearly linear elastic manner until approximately 75% of the peak stress was reached. The angle of the failure feature (shear band) was compared to predictions developed by using the Rudnicki and Rice (1975) localization criterion. It was found that there was good agreement (within 7°) between the experimental results and theoretical predictions.
Dissolved CO2 in the subsurface resulting from geological CO2 storage may react with minerals in fractured rocks, confined aquifers, or faults, resulting in mineral precipitation and dissolution. The overall rate of reaction can be affected by coupled processes including hydrodynamics, transport, and reactions at the (sub) pore-scale. In this work pore-scale modeling of coupled fluid flow, reactive transport, and heterogeneous reactions at the mineral surface is applied to account for permeability alterations caused by precipitation-induced pore-blocking. This work is motivated by observations of CO2 seeps from a natural CO2 sequestration analog, Crystal Geyser, Utah. Observations along the surface exposure of the Little Grand Wash fault indicate the lateral migration of CO2 seep sites (i.e., alteration zones) of 10–50 m width with spacing on the order of ~100 m over time. Sandstone permeability in alteration zones is reduced by 3–4 orders of magnitude by carbonate cementation compared to unaltered zones. One granular porous medium and one fracture network systems are used to conceptually represent permeable porous media and locations of conduits controlled by fault-segment intersections and/or topography, respectively. Simulation cases accounted for a range of reaction regimes characterized by the Damköhler (Da) and Peclet (Pe) numbers. Pore-scale simulation results demonstrate that combinations of transport (Pe), geochemical conditions (Da), solution chemistry, and pore and fracture configurations contributed to match key patterns observed in the field of how calcite precipitation alters flow paths by pore plugging. This comparison of simulation results with field observations reveals mechanistic explanations of the lateral migration and enhances our understanding of subsurface processes associated with the CO2 injection. In addition, permeability and porosity relations are constructed from pore-scale simulations which account for a range of reaction regimes characterized by the Da and Pe numbers. The functional relationships obtained from pore-scale simulations can be used in a continuum scale model that may account for large-scale phenomena mimicking lateral migration of surface CO2 seeps.
We characterize geomechanical constitutive behavior of reservoir sandstones at conditions simulating the “Cranfield” Southeast Regional Carbon Sequestration Partnership injection program. From two cores of Lower Tuscaloosa Formation, three sandstone lithofacies were identified for mechanical testing based on permeability and lithology. These include: chlorite-cemented conglomeratic sandstone (Facies A); quartz-cemented fine sandstone (Facies B); and quartz- and calcite-cemented very fine sandstone (Facies C). We performed a suite of compression tests for each lithofacies at 100 °C and pore pressure of 30 MPa, including hydrostatic compression and triaxial tests at several confining pressures. Plugs were saturated with supercritical CO2-saturated brine. Chemical environment affected the mechanical response of all three lithofacies, which experience initial plastic yielding at stresses far below estimated in situ stress. Measured elastic moduli degradation defines a secondary yield surface coinciding with in situ stress for Facies B and C. Facies A shows measurable volumetric creep strain and a failure envelope below estimates of in situ stress, linked to damage of chlorite cements by acidic pore solutions. The substantial weakening of a particular lithofacies by CO2 demonstrates a possible chemical-mechanical coupling during injection at Cranfield with implications for CO2 injection, reservoir permeability stimulation, and enhanced oil recovery.
The Mount Simon Sandstone and Eau Claire Formation represent a potential reservoir-caprock system for wastewater disposal, geologic CO2 storage, and compressed air energy storage (CAES) in the Midwestern United States. A primary concern to site performance is heterogeneity in rock properties that could lead to nonideal injectivity and distribution of injected fluids (e.g., poor sweep efficiency). Using core samples from the Dallas Center domal structure, Iowa, we investigate pore characteristics that govern flow properties of major lithofacies of these formations. Methods include gas porosimetry and permeametry, mercury intrusion porosimetry, thin section petrography, and X-ray diffraction. The lithofacies exhibit highly variable intraformational and interformational distributions of pore throat and body sizes. Based on pore-throat size, there are four distinct sample groups. Micropore-throat-dominated samples are from the Eau Claire Formation, whereas the macropore-dominated, mesopore-dominated, and uniform-dominated samples are from the Mount Simon Sandstone. Complex paragenesis governs the high degree of pore and pore-throat size heterogeneity, due to an interplay of precipitation, nonuniform compaction, and later dissolution of cements. The cement dissolution event probably accounts for much of the current porosity in the unit. Mercury intrusion porosimetry data demonstrate that the heterogeneous nature of the pore networks in the Mount Simon Sandstone results in a greater than normal opportunity for reservoir capillary trapping of nonwetting fluids, as quantified by CO2 and air column heights that vary over three orders of magnitude, which should be taken into account when assessing the potential of the reservoir-caprock system for waste disposal (CO2 or produced water) and resource storage (natural gas and compressed air). Our study quantitatively demonstrates the significant impact of millimeter-scale to micron-scale porosity heterogeneity on flow and transport in reservoir sandstones.
This report details experimental testing and constitutive modeling of sandy soil deformation under quasi - static conditions. This is driven by the need to understand constitutive response of soil to target/component behavior upon impact . An experimental and constitutive modeling program was followed to determine elastic - plastic properties and a compressional failure envelope of dry soil . One hydrostatic, one unconfined compressive stress (UCS), nine axisymmetric compression (ACS) , and one uniaxial strain (US) test were conducted at room temperature . Elastic moduli, assuming isotropy, are determined from unload/reload loops and final unloading for all tests pre - failure and increase monotonically with mean stress. Very little modulus degradation was discernable from elastic results even when exposed to mean stresses above 200 MPa . The failure envelope and initial yield surface were determined from peak stresses and observed onset of plastic yielding from all test results. Soil elasto - plastic behavior is described using the Brannon et al. (2009) Kayenta constitutive model. As a validation exercise, the ACS - parameterized Kayenta model is used to predict response of the soil material under uniaxial strain loading. The resulting parameterized and validated Kayenta model is of high quality and suitable for modeling sandy soil deformation under a range of conditions, including that for impact prediction.
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.
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 oth er 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. Mo dels 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 vali date. 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 potent ial 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 mech anics, 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 (%7E900 psi) and temperatures to 90 o 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 deg rees. Creep volume strain - time relations obey simple log - time behavior through the range of porosities (%7E50 to 2% as measured); creep strain rate increases with temperature and applied stress as expected. Mercury porosimetry is used to determine characteri stic 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 t o 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 (brin e - air) flow.
This paper presents results of three models simulating the hydrological-mechanical behavior of a CO2 injection reservoir and the resulting effects on wellbore system (cement and casing) and seal repair materials. A critical aspect of designing effective wellbore seal repair materials is predicting thermo-mechanical perturbations that can compromise seal integrity. Three distinct computational models comprise the current modeling effort. The first model depicts bench-top experiments of an integrated seal system in an idealized scaled wellbore mock-up being used to test candidate seal repair materials. This model will be used to gain an understanding of the wellbore microannulus compressibility and permeability. The second is a field scale model that uses the stratigraphy, material properties, and injection history from a pilot CO2 injection operation to develop stress-strain histories for wellbore locations from 100 to 400 meters from an injection well. The results from these models are used as input to a more detailed model of a wellbore system. The 3D wellbore model examines the impacts of various loading scenarios on a wellbore system. The results from these models will be used to estimate the necessary thermal-mechanical properties needed for a successful repair material.
Multiscale characteristics of anisotropic, heterogeneous pore structure and compositional (e.g., kerogen, clay, cement, etc) distribution profoundly influence the hydro, mechanical, and chemical response of shale materials during stimulation and production. In this work the impact of these lithologic heterogeneities on physical, chemical, and mechanical properties is investigated over a micron to core scale of shale samples for Cretaceous Mancos Shale. Principal macroscopic lithofacies at a decimeter scale are petrographically examined. Thin sections (∼2-3cm) impregnated with fluorochromes are examined using laser scanning confocal microscopy and optical microscopy with different filters to characterize micro-facies (i.e., texture patterns) and using electron microprobe to identify the mineralogical distribution. Advanced multiscale image analysis for texture classification will be used to identify key features of samples which will be further analyzed using dual focused ion beam-scanning electron microscopy, aberration corrected-scanning TEM and energy dispersive X-ray spectrometry for nano-pore and organic-pore structures and mineralogies at nano scale. This characterization will be examined against experimental data including acoustic emission and nano-indentation measurements of elastic properties using focused ion-beam milled pillars. Finally, multiscale 3-D image stacks will be segmented to rigorously test the scale of a representative elementary volume based on multiple measures from image analysis and pore-scale simulations.
The Water, Energy, and Carbon Sequestration Simulation Model (WECSsim) is a national dynamic simulation model that calculates and assesses capturing, transporting, and storing CO2 in deep saline formations from all coal and natural gas-fired power plants in the U.S. An overarching capability of WECSsim is to also account for simultaneous CO2 injection and water extraction within the same geological saline formation. Extracting, treating, and using these saline waters to cool the power plant is one way to develop more value from using saline formations as CO2 storage locations. WECSsim allows for both one-to-one comparisons of a single power plant to a single saline formation along with the ability to develop a national CO2 storage supply curve and related national assessments for these formations. This report summarizes the scope, structure, and methodology of WECSsim along with a few key results. Developing WECSsim from a small scoping study to the full national-scale modeling effort took approximately 5 years. This report represents the culmination of that effort. The key findings from the WECSsim model indicate the U.S. has several decades' worth of storage for CO2 in saline formations when managed appropriately. Competition for subsurface storage capacity, intrastate flows of CO2 and water, and a supportive regulatory environment all play a key role as to the performance and cost profile across the range from a single power plant to all coal and natural gas-based plants' ability to store CO2. The overall system's cost to capture, transport, and store CO2 for the national assessment range from $74 to $208 / tonne stored ($96 to 272 / tonne avoided) for the first 25 to 50% of the 1126 power plants to between $1,585 to well beyond $2,000 / tonne stored ($2,040 to well beyond $2,000 / tonne avoided) for the remaining 75 to 100% of the plants. The latter range, while extremely large, includes all natural gas power plants in the U.S., many of which have an extremely low capacity factor and therefore relatively high system's cost to capture and store CO2.
In the supercritical CO2-water-mineral systems relevant to subsurface CO2 sequestration, interfacial processes at the supercritical fluid-mineral interface will strongly affect core- and reservoir-scale hydrologic properties. Experimental and theoretical studies have shown that water films will form on mineral surfaces in supercritical CO2, but will be thinner than those that form in vadose zone environments at any given matric potential. The theoretical model presented here allows assessment of water saturation as a function of matric potential, a critical step for evaluating relative permeabilities the CO2 sequestration environment. The experimental water adsorption studies, using Quartz Crystal Microbalance and Fourier Transform Infrared Spectroscopy methods, confirm the major conclusions of the adsorption/condensation model. Additional data provided by the FTIR study is that CO2 intercalation into clays, if it occurs, does not involve carbonate or bicarbonate formation, or significant restriction of CO2 mobility. We have shown that the water film that forms in supercritical CO2 is reactive with common rock-forming minerals, including albite, orthoclase, labradorite, and muscovite. The experimental data indicate that reactivity is a function of water film thickness; at an activity of water of 0.9, the greatest extent of reaction in scCO2 occurred in areas (step edges, surface pits) where capillary condensation thickened the water films. This suggests that dissolution/precipitation reactions may occur preferentially in small pores and pore throats, where it may have a disproportionately large effect on rock hydrologic properties. Finally, a theoretical model is presented here that describes the formation and movement of CO2 ganglia in porous media, allowing assessment of the effect of pore size and structural heterogeneity on capillary trapping efficiency. The model results also suggest possible engineering approaches for optimizing trapping capacity and for monitoring ganglion formation in the subsurface.
The state of the art in failure modeling enables assessment of crack nucleation, propagation, and progression to fragmentation due to high velocity impact. Vulnerability assessments suggest a need to track material behavior through failure, to the point of fragmentation and beyond. This eld of research is particularly challenging for structures made of porous quasi-brittle materials, such as ceramics used in modern armor systems, due to the complex material response when loading exceeds the quasi-brittle material's elastic limit. Further complications arise when incorporating the quasi-brittle material response in multi-material Eulerian hydrocode simulations. In this report, recent e orts in coupling a ceramic materials response in the post-failure regime with an Eulerian hydro code are described. Material behavior is modeled by the Kayenta material model [2] and Alegra as the host nite element code [14]. Kayenta, a three invariant phenomenological plasticity model originally developed for modeling the stress response of geologic materials, has in recent years been used with some success in the modeling of ceramic and other quasi-brittle materials to high velocity impact. Due to the granular nature of ceramic materials, Kayenta allows for signi cant pressures to develop due to dilatant plastic ow, even in shear dominated loading where traditional equations of state predict little or no pressure response. When a material's ability to carry further load is compromised, Kayenta allows the material's strength and sti ness to progressively degrade through the evolution of damage to the point of material failure. As material dilatation and damage progress, accommodations are made within Alegra to treat in a consistent manner the evolving state.
The Iowa Stored Energy Plant Agency selected a geologic structure at Dallas Center, Iowa, for evaluation of subsurface compressed air energy storage. The site was rejected due to lower-than-expected and heterogeneous permeability of the target reservoir, lower-than-desired porosity, and small reservoir volume. In an initial feasibility study, permeability and porosity distributions of flow units for the nearby Redfield gas storage field were applied as analogue values for numerical modeling of the Dallas Center Structure. These reservoir data, coupled with an optimistic reservoir volume, produced favorable results. However, it was determined that the Dallas Center Structure cannot be simplified to four zones of high, uniform permeabilities. Updated modeling using field and core data for the site provided unfavorable results for air fill-up. This report presents Sandia National Laboratories petrologic and petrophysical analysis of the Dallas Center Structure that aids in understanding why the site was not suitable for gas storage.
We develop a 2-D pore scale model of coupled fluid flow, reactive transport, and calcium carbonate (CaCO 3) precipitation and dissolution. The model is used to simulate transient experimental results of CaCO 3 precipitation and dissolution under supersaturated conditions in a microfluidic pore network (i.e., micromodel) in order to improve understanding of coupled reactive transport systems perturbed by geological CO 2 injection. In the micromodel, precipitation is induced by transverse mixing along the centerline in pore bodies. The reactive transport model includes the impact of pH upon carbonate speciation and a CaCO 3 reaction rate constant, the effect of changing reactive surface area upon the reaction, and the impact of pore blockage from CaCO 3 precipitation on diffusion and flow. Overall, the pore scale model qualitatively captured the precipitate morphology, precipitation rate, and maximum precipitation area using parameter values from the literature. In particular, we found that proper estimation of the effective diffusion coefficient (D eff) and the reactive surface area is necessary to adequately simulate precipitation and dissolution rates. In order to match the initial phase of fast precipitation, it was necessary to consider the top and bottom of the micromodel as additional reactive surfaces. In order to match a later phase when dissolution occurred, it was necessary to increase the dissolution rate compared to the precipitation rate, but the simulated precipitate area was still higher than the experimental results after ∼30 min, highlighting the need for future study. The model presented here allows us to simulate and mechanistically evaluate precipitation and dissolution of CaCO 3 observed in a micromodel pore network. This study leads to improved understanding of the fundamental physicochemical processes of CaCO 3 precipitation and dissolution under far-from-equilibrium conditions. Copyright 2012 by the American Geophysical Union.