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Report prepared for NDEP
The unsaturated zone alluvium reference case is one of several geologic systems under consideration by the U.S. Department of Energy Office of Nuclear Energy for hosting repositories for spent nuclear fuel and associated waste (Sevougian et al., 2019). As noted by Mariner et al. (2018), the generic alluvial basin offers positive attributes that merit its consideration as a reference case by the Spent Fuel and Waste Science and Technology (SFWST) campaign. Hundreds of alluvial basins and sub-basins are scattered across the arid western United States (Figure 1-1). Precipitation and infiltration rates are relatively low with high evapotranspiration, resulting in deep regional water tables. Deep regional water tables allow for significant vertical separation between proposed repository depths and groundwater and thus longer transport paths from a hypothetical repository to an aquifer. Accumulations of alluvial sediments within these basins are typically on the order of hundreds of meters, and locally may exceed 1,000 m in thickness, as is the case for the Deming sub-basin in southern New Mexico. In alluvial basins, alluvium creates a thick geologic host medium that serves as the natural barrier system (NBS) in the conceptual model framework of a geologic disposal system and isolates the waste packages from receptors in the biosphere. Further, alluvial basin fill is typically comprised of stacked playa and lacustrine deposits along the basin axis (Perry et al., 2018). Characterized by low permeability, these layers protect the biosphere above the repository and the groundwater resources below the repository by limiting flow and transport of radionuclides.
The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Fuel Cycle Technology (FCT) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). Two high priorities for SFWST disposal R&D are design concept development and disposal system modeling. These priorities are directly addressed in the SFWST ''Geologic Disposal Safety Assessment'' (GDSA) control account, which is charged with developing a geologic repository system modeling and analysis capability, and the associated software, ''GDSA Framework'', for evaluating disposal system performance for nuclear waste in geologic media. ''GDSA Framework'' is supported by SFWST Campaign and its predecessor the Used Fuel Disposition (UFD) campaign. This report fulfills the GDSA Uncertainty and Sensitivity Analysis Methods work package (SF-20SN01030403) level 3 milestone — ''Advances in Uncertainty and Sensitivity Analysis Methods and Applications in GDSA Framework'' (M3SF-20SN010304032). It presents high level objectives and strategy for development of uncertainty and sensitivity analysis tools, demonstrates uncertainty quantification (UQ) and sensitivity analysis (SA) tools in GDSA Framework in FY20, and describes additional UQ/SA tools whose future implementation would enhance the UQ/SA capability of ''GDSA Framework''. This work was closely coordinated with the other Sandia National Laboratory GDSA work packages: the GDSA Framework Development work package (SF- 2051\101030404), the GDSA Repository Systems Analysis work package (SF-2051\101030405), and the GDSA PFLOTRAN Development work package (SF-20SN01030406). This report builds on developments reported in previous ''GDSA Framework'' milestones, particularly M2SF- 19SNO1030403.
The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Fuel Cycle Technology (FCT) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). Two high priorities for SFWST disposal R&D are design concept development and disposal system modeling. These priorities are directly addressed in the SFWST Geologic Disposal Safety Assessment (GDSA) control account, which is charged with developing a geologic repository system modeling and analysis capability, and the associated software, GDSA Framework, for evaluating disposal system performance for nuclear waste in geologic media. GDSA Framework is supported by SFWST Campaign and its predecessor the Used Fuel Disposition (UFD) campaign. This report fulfills the GDSA Uncertainty and Sensitivity Analysis Methods work package (SF-21SN01030404) level 3 milestone, Uncertainty and Sensitivity Analysis Methods and Applications in GDSA Framework (FY2021) (M3SF-21SN010304042). It presents high level objectives and strategy for development of uncertainty and sensitivity analysis tools, demonstrates uncertainty quantification (UQ) and sensitivity analysis (SA) tools in GDSA Framework in FY21, and describes additional UQ/SA tools whose future implementation would enhance the UQ/SA capability of GDSA Framework. This work was closely coordinated with the other Sandia National Laboratory GDSA work packages: the GDSA Framework Development work package (SF-21SN01030405), the GDSA Repository Systems Analysis work package (SF-21SN01030406), and the GDSA PFLOTRAN Development work package (SF-21SN01030407). This report builds on developments reported in previous GDSA Framework milestones, particularly M3SF 20SN010304032.
The Spent Fuel and Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Fuel Cycle Technology (FCT) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). Two high priorities for SFWST disposal R&D are design concept development and disposal system modeling. These priorities are directly addressed in the SFWST Geologic Disposal Safety Assessment (GDSA) control account, which is charged with developing a geologic repository system modeling and analysis capability, and the associated software, GDSA Framework, for evaluating disposal system performance for nuclear waste in geologic media. GDSA Framework is supported by SFWST Campaign and its predecessor the Used Fuel Disposition (UFD) campaign.
The liquid effluent from the Savannah River Plutonium Processing Facility (SRPPF) Aqueous Recovery Processes will be solidified into a stable form that is acceptable by Waste Isolation Pilot Plant (WIPP) for disposal. The current Aqueous Recovery flow sheet proposes to solidify the liquid effluent using a grout formula that was developed and tested for the former Waste Solidification Building process. This Portland cement based mixture results in a high pH (~13) leachate from the solidified waste form which is not acceptable to WIPP in the large quantities expected from production at SRPPF. Various cementitious materials were previously evaluated as alternative grout formulations to Portland cement and a MgO-based mix was identified as a promising alternative. A magnesium oxysulfate (MOS) cement formulation comprised of reactive magnesium oxide (MgO), anhydrous magnesium sulfate (MgSO 4 ), and sand, as a non-reactive heat sink provided good mixability, similar density to the original Portland-cement based mix, and a leachate pH of 9.4, within the assumed WIPP brine pH range. However, the MOS formulation exhibited an appreciable amount of heat generation, which resulted in premature setting of a large-scale test.
The Spent Fuel and Waste Science and Technology Campaign (SFWST) of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE) is conducting research and development on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). Two priorities for SFWST are design concept development and disposal system modeling. These priorities are directly addressed in the Geologic Disposal Safety Assessment (GDSA) control account, which is charged with developing a geologic repository system modeling and analysis capability, and the associated software, GDSA Framework, for evaluating disposal system performance for nuclear waste in geologic media. This report describes specific activities in the Fiscal Year (FY) 2025 associated with the GDSA Uncertainty and Sensitivity Analysis Methods work package. This report fulfills the GDSA Uncertainty and Sensitivity Analysis Methods work package (SF-25SN01030407) level 3 milestone, Uncertainty and Sensitivity Analysis Methods and Applications in GDSA Framework (FY2025) (M3SF-25SN010304072). This work was closely coordinated with the other Sandia National Laboratory GDSA work packages: the GDSA Framework Development work package (SF-25SN01030408), the GDSA Repository Systems Analysis work package (SF-25SN01030409), and the GDSA PFLOTRAN Development work package (SF-25SN01030410). This report builds on developments reported in previous GDSA Framework milestones, particularly M3SF-24SN010304072.
The Spent Fuel and Waste Science and Technology Campaign (SFWST) of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE) is conducting research and development on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). Two priorities for SFWST are design concept development and disposal system modeling. These priorities are directly addressed in the Geologic Disposal Safety Assessment (GDSA) control account, which is charged with developing a geologic repository system modeling and analysis capability, and the associated software, GDSA Framework, for evaluating disposal system performance for nuclear waste in geologic media.
At the U.S. Department of Energy's Hanford Site, liquid-phase waste was discharged using surface disposal features such as ponds, trenches, and cribs. These practices distributed contaminants in the subsurface, some of which are currently in the vadose zone above the groundwater. At the 200-DV-1 operable unit (OU) at the Hanford Site, a key feature is a perched-water zone. This perched-water zone contains several million liters of water contaminated with high concentrations of uranium, technetium-99 (Tc-99), and nitrate that serves as a continuing source of contamination to the underlying aquifer. Currently, a pumping system is used to remove contaminant mass from the perched-water zone. However, water extraction will become more challenging as the perched unit dewaters. As a result, residual contaminants remaining after pumping is no longer effective needs to be addressed with post-extraction mitigation approaches, appropriate monitoring, and selection of suitable remediation endpoints. Thus, a remedy evaluation needs to include the unique conditions of this perched-water zone. As part of the initial evaluation, a set of technologies have been preliminarily identified as potentially applicable to the perched-water zone, including in situ remediation technologies to sequester uranium and Tc-99 and to degrade nitrate. While there is sufficient information available for direct consideration of some of the reviewed technologies in a feasibility study, five in situ remediation technologies were identified as needing additional information on their effectiveness under the geochemical and contaminant conditions of the perched-water zone. (authors)
Microbially induced corrosion (MIC) is an emerging topic that has huge environmental impacts, such as long-term evaluation of microbial interactions with radioactive waste glass, environmental cleanup and disposal of radioactive material, and weathering effects of microbes. Time-of-flight secondary ion mass spectrometry (ToF-SIMS), a powerful mass spectral imaging technique with high surface sensitivity, mass resolution, and mass accuracy, can be used to study biofilm effects on different substrates. Understanding how to prepare biofilms on MIC susceptible substrates is critical for proper analysis via ToF-SIMS. We present here a step-by-step protocol for preparing bacterial biofilms for ToF-SIMS analysis, comparing three biofilm preparation techniques: no desalination, centrifugal spinning (CS), and water submersion (WS). Comparisons of two desalinating methods, CS and WS, show a decrease in the media peaks up to 99% using CS and 55% using WS, respectively. Proper desalination methods also can increase biological signals by over four times for fatty acids using WS, for example. ToF-SIMS spectral results show chemical compositional changes of the glass exposed in a Paenibacillus polymyxa SCE2 biofilm, indicating its capability to probe microbiologically induced corrosion of solid surfaces. This represents the proper desalination technique to use without significantly altering biofilm structure and substrate for ToF-SIMS analysis. ToF-SIMS spectral results showed chemical compositional changes of the glass exposed by a Paenibacillus bacterial biofilm over 3-month inoculation. Finally, possible MIC products include various phosphate phase molecules not observed in any control samples with the highest percent increases when experimental samples were compared with biofilm control samples.
This project addressed the main challenges associated with the disposal of electrorefiner salt: maximization of fission products in a final waste form and the associated processing costs. Since over half of the mass of the ER salt is chlorine in the form of non-radioactive chloride ions, our approach for achieving dechlorination is through the formation of HCl gas during the exchange of the metal ions into ultrastable H-Y (USHY) zeolite. The zeolite containing the fission products was then sintered into a chemically durable waste form.
Abstract There is a growing need for disposal of high‐level nuclear waste. To reduce uncertainty associated with brine availability to repository excavations in salt formations, a collaboration between Sandia, Los Alamos, and Lawrence Berkeley National Laboratories is performing a series of borehole‐scale coupled process tests. Here, we report on the first round of the Brine Availability Test in Salt (BATS) project, a “shakedown” experiment called Phase 1s. Experimental testing included placing a resistive heater, a 260‐W radiative heater, and a 750‐W radiative heater within previously drilled horizontal boreholes at the Waste Isolation Pilot Plant (WIPP) while monitoring temperature and water inflow. The experiments successfully achieved the targeted temperature of 120 °C when using the 750‐W radiative heater. Simulations using FEHM (Finite Element Heat and Mass transfer code) and TOUGH‐FLAC (Transport Of Unsaturated Groundwater and Heat–Fast Lagrangian Analysis of Continua) were able to accurately predict the coupled thermo–hydro–mechanical–chemical response of salt, matching the observed temperature and brine production. Due to the extremely low permeability of salt, these systems take many years to reach steady state when perturbed by mining activities. Long‐term numerical simulations are used to develop the initial pressure and saturation conditions. The inclusion of a damaged rock zone with higher permeability around the borehole also affects the saturation and pressure distributions and plays an important role in dissipating the potential for thermal pressurization. Knowledge gained from this round of experimentation and simulation will be used to conduct the next BATS project experiment in new boreholes at WIPP.
The chemical durability of borosilicate glass used to confine nuclear wastes is known to vary nonlinearly with their composition, making glass dissolution rate predictions difficult. Here, we focus on the effect of Al, an important oxide of these materials. The initial and residual glass dissolution rates were investigated through experiments conducted at 90 °C and pH 9. Our results show that low Al content glasses dissolve initially faster than glasses with higher Al content, but quickly achieve a lower residual rate due to the rapid formation of a more passivating gel. Nevertheless, the high Al content gel will eventually achieve passivation with a slower reorganization. The strengthening effect of Al on the Si-O bond hydrolysis will result in more stable gels, suggesting that slightly higher Al content in the gel will improve nuclear high-level waste glass durability in geological disposal conditions.
This contribution provides a thorough examination of the structural characteristics of pyrochlore-type lanthanide titanates and zirconates Ln2Ti2O7 and Ln2Zr2O7, across various length scales. This paper also examines their processing, interesting physical properties (electrical, magnetic, and thermal characteristics), and responses to high pressure and ion irradiation. Brief sections on the elemental oxides' crystal chemistry, pertinent phase diagrams, and energetics of defect formation are also provided. Pyrochlore-type Ln2Ti2O7 and Ln2Zr2O7 stand out as truly multifunctional materials. Moreover, they have emerged as fascinating materials due to magnetic geometrical frustration, arising from the ordering of magnetic Ln3+ and non-magnetic Ti4+ (or Zr4+) cations into separate, interpenetrating lattices of corner-sharing tetrahedra. This results in a diverse array of exotic magnetic ground states, such as spin-ice (e.g., Dy2Ti2O7 or Ho2Ti2O7) or quantum spin ice (e.g., Tb2Ti2O7), observed at both low and room temperatures. They also exhibit varied electrical and electrochemical characteristics. Some members such as Gd2Zr2O7, function as fast ion conductors with a conductivity (σ) of ≈10−2 S·cm−1 at 800 °C and activation energy (Ea) ranging from 0.85 to 1.52 eV, depending on the degree of structural disorder. Others, such as Gd2TiMoO7, are mixed ionic-electronic conductors with σ ≈ 25 S·cm−1 at 1000 °C, making them promising candidate materials for applications in energy conversion and storage devices and oxygen separation membranes. Their exceptionally low thermal conductivity (e.g., κ ∼ 1.1–1.7 W·m−1·K−1 between 700 and 1200 °C for Ln2Zr2O7), close to the glass-like lower limit of highly disordered solids, positions them as valuable materials for thermal barrier coatings. They can also effectively accommodate actinides (e.g., Pu, Np, Cm, Am) in solid solutions and sustain prolonged exposure to radiation due to alpha-decay events, while preserving the integrity of the periodic atomic structure. Proposed as major components in actinide-bearing ceramics, they contribute to the long-term immobilization and disposal of long-lived waste radionuclides from nuclear programs. Some of these properties are displayed simultaneously, opening avenues for new applications. Despite the wealth of data available in the literature, this review highlights the need for a better understanding of order/disorder processes in pyrochlore-type materials and the influence of the structural length scale on their physical and chemical properties. Recent experimental evidence has revealed that pyrochlore short-range structure is far more complex than originally thought. Moreover, pyrochlore local structure is now believed to include short-range, lower symmetry, ordered domains, such as the orthorhombic weberite-type of structure. Notably, short- and long-range structures appear decoupled across different length scales and temperature regimes, and these differences persist even in well-ordered samples. We believe that the pyrochlore structure offers a unique opportunity for examining the interplay between chemical composition, defect chemistry, and properties. In Memoriam: Rodney C. Ewing, Fondly Remembered.
In this issue, highlights of our contributions to mission operations include descriptions of the following. • How exact and scrupulous planning in concert with sophisticated science enabled a first-ever direct measurement of a radionuclide with a half-life as short as six days. The work, which included operations at the Los Alamos Neutron Science Centers (LANSCE) Weapons Neutron Research Facility and the Isotope Production Facility’s hot cell facility, is a boon for both astrophysics and weapons science. • An introduction to Christie Davis and her role in ensuring the Lab’s execution of simultaneous excellence. • A look at progress by AOT’s Target and Experimental Support Team in reclaiming long-dormant space in a radiological controlled area for new work improving target systems for the Lujan Center. • A story showcasing a cross-organizational effort to minimize the directorate’s legacy and environmental footprint. Staff from across the Lab joined together to ensure the safe and efficient disposal of Rocky Flats legacy waste stored in a transportainer at the Target Fabrication Facility. • How the Lab’s Utilities and Infrastructure experts collaborated with stakeholders in our directorate to safety execute preventive maintenance on the LANSCE mesa’s large electrical substation. The Safe Conduct of Research principles provided a common framework for the planning and process. • A description of the resources called upon and the procedures undertaken by MPA to inventory the division’s time-sensitive chemicals, including the careful and conscientious response of an alert team member when something seemed amiss.
The goal of this Case Study was to evaluate the performance of air classification of logging residues toward meeting conversion CMAs for carbon and ash contents, as compared to the static status quo Base Case system in which the residues are first dried and then ground in a hammer mill with a 6 mm screen and fines < 1.18 mm are removed. Also considered were moisture and ash impacts on throughput and Overall Operating Effectiveness (OOE), as well as delivered feedstock cost and minimum fuel selling price (MFSP). Laboratory data on the impacts of fan speed and moisture content on the separation efficiency of soil ash, needles and bark from white wood were received from FCIC Subtask 5.2. Average throughput and energy consumption data were obtained from the Bioenergy Feedstock National User Facility (BFNUF) for the same air classifier. These data were utilized to develop the necessary response surface equations to perform throughput analysis using discrete event simulation. Because the Base Case status quo system utilizes drying prior to grinding, we modeled the Case Study with drying prior to air classification and subsequent grinding of the separated white wood to isolate the individual quality and cost impacts of air classification relative to the Base Case system. Key takeaways from this Case Study are that air classification improves the quality of the final material, but increases the production cost, especially when lights are disposed; this becomes a tradeoff between increased conversion yield and the extra cost. Removing material should be done as early in the process as possible. Each operation that occurs prior to removing the material increases the cost of the disposed material and leads to wasted energy expenditures. As processes are included or modified, the impact on monetary and energy cost should be included in the decision process. Identifying alternative uses and the associated value for material that is separated from the feedstock stream will have a significant impact on the delivered cost of the material. Although there was an increase in production cost by adding air classification, there was a resulting benefit to the MFSP when meeting or exceeding all of the conversion CMAs; this was an important finding that should be explored further with FCIC Subtask 8.3 and potentially FCIC Task 6.
The University of Tennessee, Knoxville and Oak Ridge National Laboratory have completed proof-of principle testing on an advanced sulfur-based zirconium and aluminum chlorination process for the recovery of Zr or Al from spent fuel claddings and purification of the products. This process could be used to recover hafnium-free nuclear-grade zirconium for reuse or disposal as low-level waste. Testing showed that even non-optimized reaction protocols could produce zirconium product streams from simulated irradiated fuel with purities >90%. The chlorination process was tested on representative fission product species that would be found in Advanced Test Reactor fuel (ATR). First, fission product generation was determined through modeling and simulation of the ATR. The generation of fission products was used to selected contaminants and potentially volatile fission product simulants for laboratory testing. The goal is to identify which species may react with the sulfur-chlorine reagents and be transported into the advanced chlorination off-gas.
A new powdered-carbon treatment process is being developed for the elimination of the present problems, associated with the disposal of biologically active sewage waste solids, and with water reuse. This counter-current flow process produces an activated carbon, which is obtained from the pyrolysis of the sewage solids, and utilizes this material to remove the adulterating materials from the water. Additional advantages of the process are the elimination of odors, the removal of heavy metals, and the potential for energy conservation.