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Effect of pore fluid chemistry on the mechanical behavior of a divalent compacted bentonite, an experimental and constitutive study

Geomechanics for Energy and the Environment

Al-Masri, Roa'A'; Sanchez, Camilo; Deng, Youjun; Do Nascimento Guimaraes, Leonardo; Greathouse, Jeffery A.; Matteo, Edward N.; Sanchez, Marcelo

Ongoing research in isolating high-level nuclear waste and spent fuel has highlighted compacted bentonite as a suitable material for engineered barrier systems in deep geological repositories due to its extraordinary swelling and retention properties. This research focuses on the chemo-mechanical behavior of compacted bentonite exposed to different pore fluids with different concentrations and loading conditions. The study involves swelling pressure and compressibility experiments along with mineralogy analysis employing X-ray diffraction (XRD) and Cation exchange. The tests were conducted on BCV (a Mg/Ca- bentonite) compacted at a dry density of 1.48 ± .02 Mg/m3. An advanced chemical-mechanical constitutive model for unsaturated highly expansive clays was adopted to simulate the material response and better understand its behavior. The model is able to account for the main phenomena at both macro and microstructural levels and the interactions between them. The model successfully replicated experimental observations. The XRD analyses support the macroscopic observation, indicating that salinity impacts crystalline swelling as demonstrated by the reduction of basal spacing from 19.27 Å to 15.68 Å when the osmotic suction increases from 0 MPa to 33 MPa. The results suggested that the osmotic pressure generated by the concentration in the pore fluids promotes a reduction in swelling pressures, swelling strains, and crystalline swelling of clay minerals. Also, it affects the pre-consolidation stress and the compressibility of the compacted samples. In conclusion, it was also observed that both solution type and solution concentration impact the clay swelling pressure.

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RANGERS: Methodology for Design and Performance Assessment of Engineered Barrier Systems in a Salt Repository for HLW/SNF: Synthesis Report

Simo, Eric; Gafoor, Ajmal; Herold, Philipp; Leon Vargas, Paola; Lommerzheim, Andree; Keller, Andreas; Seidel, David; Kuhlman, Kristopher L.; Matteo, Edward N.; Lopez, Carlos M.; Fukuyama, David E.; Jayne, Richard S.; Mills, Melissa M.

Salt formations have long been recognized as a highly favorable host rock for the final disposal of high-level radioactive waste (HLW) in deep geological repositories. Their unique properties, including exceptional impermeability, self-healing capabilities, and thermal conductivity, make them a reliable natural barrier for the deep disposal of radioactive waste. This report focuses on the development and application of a methodology for assessing the integrity and per formance of the Engineered Barrier System (EBS) within salt-based repositories, a critical component of the multi-barrier system ensuring safe radioactive waste disposal.

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RANGERS: Methodology Report on Design and Performance Assessment of Engineered Barrier Systems in a Salt Repository for HLW/SNF

Simo, Eric; Herold, Philipp; Lommerzheim, Andree; Keller, Andreas; Matteo, Edward N.; Jayne, Richard S.; Kuhlman, Kristopher L.; Mills, Melissa M.

Salt formations are one of the potential host rocks for the final disposal of high-level radioactive waste (HLW) in deep geological repositories, both in Germany and the United States. The safe isolation of radioactive waste in these repositories relies on a multi-barrier system, combining engineered and natural barriers. The natural barrier is provided by the salt rock itself, known for its self-sealing properties and long-term stability. The engineered barrier, on the other hand, comprises sealing components strategically placed within the repository to enhance its containment capabilities. In both Germany and the United States, long-term safety assessments require demonstrating the integrity of the natural barrier for a period of up to 1 million years. Concurrently, the engineered barrier system (EBS) must maintain its structural and functional integrity until the long-term sealing, such as the granular salt backfill material, has re-consolidated to its final low porosity and permeability. Based on extensive expertise and experience with engineered barriers in salt formations, BGE TECHNOLOGY GmbH and Sandia National Laboratories have partnered to develop a robust methodology for the integrity and performance assessment of EBS in HLW repositories through the RANGERS project. This collaborative effort aims to establish a unified approach to geotechnical engineering, repository design, integrity and performance evaluation of EBS in salt repositories.

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RANGERS: Modeling Report on Integrity and Performance Assessment of Engineered Barrier Systems in a Salt Repository for HLW/SNF

Simo, Eric; Herold, Philipp; Lommerzheim, Andree; Keller, Andreas; Matteo, Edward N.; Lopez, Carlos M.; Fukuyama, David E.; Jayne, Richard S.; Kuhlman, Kristopher L.; Mills, Melissa M.

The Engineered Barrier System (EBS) plays an important role in ensuring the long-term safety and containment of high-level waste (HLW) and spent nuclear fuel (SNF) in deep geological repositories in salt formation. As part of a multi-barrier system, the EBS works alongside the natural barrier, which is the salt formation itself and the technical barrier comprising the disposal casks. The primary function of the EBS is to maintain containment during a defined period until the backfill used in the repository made of crushed salt, develops its sealing capacity through compaction. Over the time, the backfill eventually compacts to a state of low porosity and permeability, acting as a long-term seal. However, until this process is complete, the EBS must retain its structural and functional integrity. Regulatory guidelines in Germany currently require the EBS to remain effective for up to next ice age, that is expected in 50,000 years. The significant hydro-geological and topographic changes expected during an ice age could make it impossible to accurately predict the hydro-chemical conditions within the repository system at that time. In response to these challenges, BGE TECHNOLOGY GmbH (BGE TEC) and Sandia National Laboratories (SNL) have jointly developed a comprehensive methodology for the design and safety assessment of engineered barrier systems within the scope of the RANGERS project. This methodology is tailored for repositories in salt formations. The developed methodology provides a structured approach for designing and assessing the performance of the EBS in salt-based repositories. It begins with defining a sealing concept based on the geological characteristics of the selected site and the overall repository design. The entire repository system, comprising the geological site, repository infrastructure, and EBS, is then subjected to a Features, Events, and Processes (FEP) analysis, focusing solely on those FEPs that affect the EBS. The derived FEPs help identify the loads and stresses acting on the EBS, which serve as the foundation for conducting an integrity assessment. This analysis helps predict the EBS’s evolution and performance over the regulatory time frame, feeding into integrated performance assessment simulations.

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Brine Availability Test in Salt (BATS) FY24 Update

Kuhlman, Kristopher L.; Mills, Melissa M.; Jayne, Richard S.; Matteo, Edward N.; Herrick, Courtney G.; Choens, Robert C.; Paul, Matthew J.; Stauffer, Phiip H.; Guiltinan, Eric; Rahn, Thom; Otto, Shawn; Davis, Jon; Eldridge, Daniel L.; Rutqvist, Jonny; Wu, Yuxin; Hu, Mengsu; Chen, Hang; Wang, Jiannan

This report summarizes fiscal year 2024 (FY24) activities centered around a series of field tests in bedded salt at the Waste Isolation Pilot Plant (WIPP) funded by the Office of Spent Fuel and Waste Science and Technology in the Spent Fuel and Waste Disposition (SFWD) program of the US Department of Energy’s Office of Nuclear Energy (DOE-NE). High-level Purpose of Experiments: The Brine Availability Test in Salt (BATS) field tests are revealing both brine occurrence (i.e., where, and how much) and brine migration (i.e., how easily it moves) in the excavation damaged zone (EDZ). This understanding is foundational to develop a safety case for a future heat-generating waste repository in salt, and to starting up a generic repository program in salt to buy down risk. BATS seeks to predict how much brine can flow into both ambient and heated excavations (e.g., boreholes or rooms) in salt. This work is educating and empowering new repository scientists on two fronts: “design and execution of field tests” and “prediction and modeling of coupled processes.” DOE-NE capabilities in salt have grown and been tested through international modeling and benchmarking exercises (e.g., DECOVALEX, RANGERS, KOMPASS, and MEASURES; see Mills et al., 2024). The hands-on expertise we are building is a necessary step towards large-scale disposal demonstrations and eventual implementation.

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Natural carbonation of portland cement with synthetic zeolite Y as a supplementary cementitious material

Construction and Building Materials

Rimsza, Jessica M.; Mills, Melissa M.; Walder, Brennan J.; Fritzsching, Keith; Jove-Colon, Carlos; Bullard, Jeffrey W.; Lapeyre, Jonathan; Mcenroe, Theresa; Matteo, Edward N.; Tuinukuafe, Atolo A.

Risks associated with carbonation are a key limitation to greater replacement levels of ordinary portland cement (OPC) by supplementary cementitious materials (SCMs). The addition of pozzolanic SCMs in OPC alters the hydrate assemblage by forming phases like calcium-(alumina)-silicate-hydrate (C-(A)-S-H). The objective of the present study was to elucidate how such changes in hydrate assemblage influence the chemical mechanisms of carbonation in a realistic OPC system. Here, we show that synthetic zeolite Y (faujasite) is a highly reactive pozzolan in OPC that reduces the calcium content of hydration products via prompt consumption of calcium hydroxide from the evolving phase assemblage prior to CO2 exposure. Suppression of portlandite at moderate to high zeolite Y content led to a more damaging mechanism of carbonation by disrupting the formation of a passivating carbonate layer. Without this layer, carbonation depth and CO2 uptake are increased. Binders containing 12–18% zeolite Y by volume consumed all the calcium hydroxide from OPC during hydration and reduced the Ca/(Si+Al) ratio of the amorphous products to near 0.67. In these cases, higher carbonation depths were observed after exposure to ambient air with decalcification of C-(A)-S-H as the main source of CO2 buffering. Binders with either 0% or 4% zeolite Y contained calcium hydroxide in the hydrated microstructure, had higher Ca/(Si+Al) ratios, and formed a calcite-rich passivation layer that halted deep carbonation. Although the carbonated layer in the samples with 12% and 18% zeolite Y contained 70% and 76% less calcite than the OPC respectively, their higher carbonation depths resulted in total CO2 uptakes that were 12x greater than the OPC sample. Passivation layer formation in samples with calcium hydroxide explains this finding and was further supported by thermodynamic modeling. High Si/Al zeolite additives to OPC should be balanced with the calcium content for optimal carbonation resistance.

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Structural and Spectroscopic Properties of Butanediol-Modified Boehmite Materials

Journal of Physical Chemistry C

Greathouse, Jeffery A.; Weck, Philippe F.; Bell, Nelson S.; Kruichak-Duhigg, Jessica N.; Matteo, Edward N.

Glycoboehmite (GB) materials are synthesized by a solvothermal reaction to form layered aluminum oxyhydroxide (boehmite) modified by intercalated butanediol molecules. These hybrid materials offer a platform to design materials with potentially novel sorption, wetting, and catalytic properties. Several synthetic methods have been used, resulting in different structural and spectroscopic properties, but atomistic detail is needed to determine the interlayer structure to explore the synthetic control of GB materials. Here, we use classical molecular dynamics (MD) simulations to compare the structural properties of GB interlayers containing chemisorbed butanediol molecules as a function of diol loading. Accompanying quantum (density functional theory, DFT) static calculations and MD simulations are used to validate the classical model and compute the infrared spectra of various models. Classical MD results reveal the existence of two unique interlayer environments at higher butanediol loading, corresponding to smaller (cross-linked) and expanded interlayers. DFT-computed infrared spectra reveal the sensitivity of the aluminol O-H stretch frequencies to the interlayer environment, consistent with the spectrum of the synthesized material. Insight from these simulations will aid in the characterization of the newly synthesized GB materials.

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Model Development for Thermal-Hydrology Simulations of a Full-Scale Heater Experiment in Opalinus Clay

Nuclear Technology

Hadgu, Teklu; Matteo, Edward N.; Dewers, Thomas

Disposal of commercial spent nuclear fuel in a geologic repository is studied. In situ heater experiments in underground research laboratories provide a realistic representation of subsurface behavior under disposal conditions. This study describes process model development and modeling analysis for a full-scale heater experiment in opalinus clay host rock. The results of thermal-hydrology simulation, solving coupled nonisothermal multiphase flow, and comparison with experimental data are presented. The modeling results closely match the experimental data.

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Brine Availability Test in Salt (BATS) FY23 Update

Kuhlman, Kristopher L.; Mills, Melissa M.; Jayne, Richard S.; Matteo, Edward N.; Herrick, Courtney G.; Nemer, Martin; Xiong, Yongliang; Choens, Robert C.; Paul, Matthew J.; Downs, Christine; Stauffer, Philip; Boukhalfa, Hakim; Guiltinan, Eric; Rahn, Thom; Otto, Shawn; Davis, Jon; Eldridge, Daniel; Stansberry, Aidan; Rutqvist, Johnny; Wu, Yuxin; Tounsi, Hafssa; Hu, Mengsu; Uhlemann, Sebastian; Wang, Jiannan

This report summarizes the fiscal year 2023 (FY23) status of the second phase of a series of borehole heater tests in salt at the Waste Isolation Pilot Plant (WIPP) funded by the Disposal Research and Development (R&D) program of the Spent Fuel & Waste Science and Technology (SFWST) office at the US Department of Energy’s Office of Nuclear Energy’s (DOE-NE) Office in the Spent Fuel and Waste Disposition (SFWD) program.

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M4 Summary of EBS International Activity

Hadgu, Teklu; Matteo, Edward N.

Thermal-Hydrologic (TH) modeling of DECOVALEX 2023, Task C has continued in FY23. This report summarizes progress in TH modeling of Step 1c, with calibration modeling and the addition of shotcrete. The work involves 3-D modeling of the full-scale emplacement experiment at the Mont Terri Underground Rock Laboratory (Nagra, 2019). While Step 1 is focused on modeling the heating phase of the FE experiment with changes in pore pressure in the Opalinus clay resulting from heating, Step 1c is focused on calibration of models using available data.

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Salt International Collaborations FY23 Update

Kuhlman, Kristopher L.; Matteo, Edward N.; Mills, Melissa M.; Jayne, Richard S.; Coulibaly, Jibril B.; Reedlunn, Benjamin; Bays, Nathan R.

This report summarizes the international collaborations conducted by Sandia funded by the US Department of Energy Office (DOE) of Nuclear Energy (DOE-NE) Spent Fuel and Waste Science & Technology (SFWST) as part of the Sandia National Laboratories Salt R&D and Salt International work packages. This report satisfies the level-three milestone M3SF-23SN010303062. Several stand-alone sections make up this summary report, each completed by the participants. The sections discuss granular salt reconsolidation (KOMPASS), engineered barriers (RANGERS), numerical model comparison (DECOVALEX) and an NEA Salt Club working group on the development of scenarios as part of the performance assessment development process. Finally, we summarize events related to the US/German Workshop on Repository Research, Design and Operations.

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Advanced reactors spent fuel and waste streams disposition strategies

Matteo, Edward N.; Price, Laura L.; Pulido, Ramon; Weck, Philippe F.; Taconi, Anna M.; Mariner, Paul E.; Hadgu, Teklu; Park, Heeho D.; Greathouse, Jeffery A.; Sassani, David C.; Alsaed, Halim

This report describes research and development (R&D) activities conducted during Fiscal Year 2023 (FY23) in the Advanced Fuels and Advanced Reactor Waste Streams Strategies work package in the Spent Fuel Waste Science and Technology (SFWST) Campaign supported by the United States (U.S.) Department of Energy (DOE). This report is focused on evaluating and cataloguing Advanced Reactor Spent Nuclear Fuel (AR SNF) and Advanced Reactor Waste Streams (ARWS) and creating Back-end Nuclear Fuel Cycle (BENFC) strategies for their disposition. The R&D team for this report is comprised of researchers from Sandia National Laboratories and Enviro Nuclear Services, LLC.

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Results 1–25 of 248
Results 1–25 of 248
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