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At least 289 records · Page 16

Solubility of An(OH) 3 am and An(OH) 3 cr in the presence of Citrate and EDTA

The solubility of An(III), which pertains to Pu(III), Am(III), and Cm(III), in brine is an important contributor in WIPP (Waste Isolation Pilot Plant) performance assessment (PA) models to calculate the potential release of transuranic elements in the near-field environment of the WIPP repository. Americium, although present in much smaller quantities than plutonium (~ 336 kg on year 2033 is potentially WIPP-bound primarily as Am-241), has a significant impact on release due to its higher activity during the earlier times of repository history (~26% initially, decreasing to 17% and ~0% at 1000 and 10,000 years after emplacement) (SOTERM, 2019). Lanthanide analogues such as Nd 3+ possess physical and chemical characteristics that allow them to be used to examine the chemical behavior of trivalent actinides (Lucchini, et al., 2007).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Waste Control Specialists Technical Review Team Report

1. Modeling of Drum 68660 and the WCS Drums: A calibrated model of Los Alamos National Laboratory (LANL) Drum 68660 indicates that pressurization of the drum by restriction of drum venting could have led to the thermal runaway reaction at the Waste Isolation Pilot Plant (WIPP) in 2014, supporting the hypothesis that the contents of the drum were not fundamentally different from the overall remediated nitrate salt (RNS) waste stream. 2. Nitric Acid Reactions and Aging of the Waste: The stability of the WCS RNS waste with respect to autocatalytic thermal runaway due to nitric acid chemistry should increase over time as the nitric acid is depleted from chemical reactions in the drum. However, this cannot be confirmed because of the lack of long-term experimental data on the impact of aging on the reactivity of RNS waste. The calibrated model indicates that the waste drums retain most of their reactive components, metal nitrate salts and sWheat Scoop ® , even after eight years. 3. Pressure Effects and Runaway Reactions: The calibrated model indicates that if the drums and standard waste boxes (SWBs) are not allowed to pressurize during transport or storage and they are stored at historical WIPP repository temperatures, then an autocatalytic thermal runaway event is not expected to occur. Since the cause of Drum 68660 pressurization is not known, decision makers are not able to tailor mitigating strategies to the initiating event. Consequently, mitigating strategies must consider all feasible internal and external events that could lead to the pressurization of the drums. 4. Temperature Effects and Runaway Reactions: Temperature also has a strong influence on the stability of the waste. The calibrated model indicates that cooling the drums or SWBs can reduce the possibility of autocatalytic thermal runaway reactions. Simulations suggest that for a drum with a plugged vent, the probability of thermal runaway may be reduced or eliminated if wastes are maintained at or below 43 °F through active cooling measures from the initiation of transport until emplacement at WIPP.

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Neptunium (V) Solubility in the Presence and Absence of WIPP Relevant Ligands

CRA (Compliance Recertification Application)-2024 will update the oxidation state specific model used to calculate actinide solubility in the WIPP (Waste Isolation Pilot Plant). The pentavalent Np(V) ion is the most stable ion in solution within the An(V) series. This valence stability of Np(V) in aqueous solution makes Np a useful representative element for studying the aqueous complex chemistry of all An(V), but in the predicted WIPP scenario, this is the only TRU component that increases in the inventory with time as it is the main daughter product of 241 Am decay (alpha, n) so its relative importance increases throughout the 10,000-year performance period of the WIPP, it is only used to represent itself. This work is focused on confirming organic, borate and carbonate effects on solubility of Np(V) in WIPP simulated brines and 5 M NaCl and reassessing the predicted model speciation to strengthen the overall WIPP An(V) model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of Borate and Organics on U(VI) Solubility in WIPP Brine

The solubility of uranium (VI) in Waste Isolation Pilot Plant (WIPP)-relevant brine was determined to support ongoing WIPP recertification activities. This research was performed by the Los Alamos National Laboratory Carlsbad Operations (LANL-CO) Actinide Chemistry and Repository Science Program (ACRSP). The WIPP Actinide Source Term Program (ASTP) did not develop a model for the solubility of actinides in the VI oxidation state. The solubility of UO 2 2+ , in the absence of WIPP specific data, is presently set to be equal to a conservatively high 1 mM within the WIPP Performance Assessment (PA) for all expected WIPP conditions (SOTERM, 2019) as selected at the recommendation of the Environment Protection Agency (EPA) (EPA, 2005). According to the current WIPP chemistry model assumptions and conditions, the expected pC H+ is about 9.5 and controlled by MgO buffering CO 3 2- . The goal of this study is to perform screening experiments that account for the contributions of organics and borate on uranium solubility. In this report, the solubility of U(VI) was determined at pC H+ 9 WIPP brine in the absence or presence of borate and organics at under-saturation approach. Experiments were equilibrated for about 135 days. Organic compounds present in WIPP waste can form strong complexes with actinides and can affect the oxidation states of actinides. The organic compounds addressed in WIPP performance assessment include EDTA (Ethylenediaminetetraacetic Acid), oxalate, citrate, and acetate (SOTERM, 2019). These data quantify the effects of WIPP-relevant concentrations of borate and organics effects on the solubility of U(VI) to challenge the predictions of the WIPP actinide model and inform decisions and recommendations made in the upcoming recertification of the WIPP (CRA-2024). The experiments performed were done according to the U.S. Department of Energy (DOE) approved Test Plan entitled “Experimental Strategy to Challenge Actinide Solubility Predictions” and designated LCO-ACP-26. All data reported were obtained under the LANL-CO Quality Assurance Program, which is compliant with the DOE Carlsbad Field Office, Quality Assurance Program Document (CBFO/QAPD) (QAPD, 2017).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Plutonium Oxidation State Distribution under WIPP Relevant Conditions (Rev. 2)

The oxidation state of plutonium in the Waste Isolation Pilot Plant (WIPP) environment has been a topic of interest since the initial compliance certification application. Plutonium (Pu) was initially expected to be present primarily as Pu(IV), but since the presence of Pu(III) could not be ruled out, it was also included in performance assessment (PA) calculations. The redox of the other variant actinides, uranium (U) and neptunium (Np), are also coupled to the plutonium redox. This led to a position in performance assessment calculations that is commonly referred to as “50/50”. In which half of the PA realizations assume solubility is dominated by the low oxidation state [U(IV), Np(IV), Pu(III)] and the other half assume solubility is dominated by the higher oxidation state [U(VI), Np(V), Pu(IV)]. Recently, a joint group of WIPP project participants from Los Alamos National Laboratory (LANL), Sandia National Laboratories (SNL), and the Department of Energy’s Carlsbad Field Office (DOE-CBFO) agreed on a new path forward for the oxidation state model in PA which will decouple the redox active actinides and will instead consider their redox as a function of E h . This will take the current binary approach and turn it into a system with four possible redox states.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Chemical and Cement Components 2021 Inventory Estimates for Additional Panels National Environmental Policy Act Analysis

This standard analysis report provides the estimates for the chemical (oxyanions and complexing agents) and cement components with a data collection cut-off date of December 31, 2021. These estimates will be included in a response to an inventory data request developed for the U.S. Department of Energy (DOE) performance assessment (PA) for the National Environmental Policy Act (NEPA) analysis on additional panels for the Waste Isolation Pilot Plant (WIPP).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Packaging Capacity Calculation: Pu Oxide Packaging Options with the 2 Quart SAVY Container

This calculation supports programmatic efforts to Dilute and Dispose Pu. Metal is to be oxidized at LANL, then transported to SRS for dilution at SRS. Ultimately, the diluted oxide will be disposed of at the Waste Isolation Pilot Plant (WIPP). Currently 3013 containers are used to package the oxide, which are placed in to 9975 Type B shipping containers. The Oxide Packaging Technology Maturation Plan determined that a transition to the used of 2-qt SAVY containers placed in 9977 would increase efficiency in shipping and handling and increase programmatic flexibility. The 2-quart SAVY container meets DOE M 441.1 and TA-55 Documented Safety Analysis requirements for handling and storage of Pu oxide at LANL.

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Overview of Virtual Test Bed FY23 Activities

The National Reactor Innovation Center (NRIC) was created for accelerating the deployment of novel reactor concepts. This will be achieved by providing both physical and virtual spaces for building and testing various components, systems, and complete pilot plants. The Virtual Test Bed (VTB) represents the virtual arm. It is being developed in collaboration with Department of Energy’s (DOE) Nuclear Energy Advanced Modeling and Simulation (NEAMS) program.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Verification Testing of OLI Systems Mixed Solvent Electrolyte Model for the Na-K-Mg-Ca-H-Cl-SO 4 -OH-HCO 3 -CO 3 -CO 2 -H 2 ) System to High Ionic Strength at 25°C

This technical report summarizes model verification results and summary statistics for 41 evaporite mineral solubility cases evaluated by Savannah River National Laboratory using OLI Systems’ aqueous electrolyte thermodynamic modeling software. The 41 verification cases containing a total of 60 solubility curves comprise mineral solubility data from low to high ionic strength at 25°C for the eight-component system Na-K-Mg-Ca-H-Cl-SO 4 -OH-HCO 3 -CO 3 -CO 2 -H 2 O as reported by Harvie et al. (1984). Thermodynamic calculations were executed using OLI Systems’ Stream Analyzer computation module within the OLI Studio software platform (Ver. 11.0, Rev. 11.0.1.9). The Mixed Solvent Electrolyte (MSE) thermodynamic framework was chosen for this investigation because of its superiority in modeling high ionic-strength inorganic salt solutions and actinide redox chemistry and solubility, both of which are relevant to the geological repository conditions at the Waste Isolation Pilot Plant in Carlsbad, New Mexico. Mineral solubility data in various inorganic salt solutions were digitized and extracted from figures generated by Harvie et al. (1984). For each of the 60 solubility curves, a case-specific chemistry model and input file were generated in OLI Studio using OLI Stream Analyzer and the MSE (H 3 O + ion) public databank provided by OLI Systems. Model simulation results were exported to Microsoft Excel to calculate summary statistics and to generate graphs comparing the OLI model predictions to the solubility data. Summary statistics include residuals (model – data) and concordance (accuracy × precision, where precision is indicated by the Pearson correlation coefficient and accuracy accounts for bias and scale differential). Private databanks were not developed, and activity coefficient model regressions were not performed to improve OLI model fits to the data. Of the 41 model verification plots, 83% have a mean of the percent residuals less than or equal to 25%. Similarly, 75% display a concordance greater than or equal to 0.75. Only seven of the 41 verification plots fail to show good agreement between the model and data. Of these seven, three are relevant to the WIPP repository because they involve the Mg-OH-Cl-SO 4 -CO 3 aqueous system. The remaining four address salt solubilities at the pH extremes (strong acid and strong base). It should be noted that in two of the three Mg-OH-Cl-SO 4 -CO 3 system cases, the regressed Harvie et al. (1984) solubility curve also deviated from the data. Lack of agreement between the OLI model-predicted solubility curves and the data is attributable to one or more of the following: specific solid species are not included in the OLI MSE databank; there is significant variation among the different solubility datasets chosen by Harvie et al. (1984); the OLI MSE model’s thermodynamic parameters were determined using different solubility datasets; and the activity coefficient parameters for certain relevant ion-ion and ion-molecule pairs have not been optimized via data regression. Two recommendations for future work are to (1) evaluate solubility data for the Mg-OH-Cl-SO 4 -CO 3 system at high ionic strength and, if necessary, develop a private OLI MSE database that includes missing species and, where necessary, regressed standard state properties and interaction parameters; (2) perform similar verification testing of the OLI model for actinide solubility data.

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Solidification of REDC Organics For Disposal As Solid Waste

The Radiochemical Engineering Development Center (REDC) generates various liquid organic wastes from processing irradiated targets to recover heavy elements. In the past, these organics were discharged to the Oak Ridge National Laboratory (ORNL) liquid low-level waste (LLLW) system, along with the aqueous waste. Because of a reduction in aqueous LLLW from other ORNL generators and an increase in the radionuclide concentration, particularly 238 Pu, in the REDC organic waste stream, the organics can no longer be discharged to the LLLW system. The plan is to solidify the liquid organic waste for disposal as solid waste. Solidifying the organic liquids using PM-199 Organoclay ® would produce solid waste forms with no free liquid, which should qualify for disposal at the Waste Isolation Pilot Plant. Granular Organoclay can be added to the organic waste solutions until there is a dry layer on top of the liquid and then allowed to cure for a few hours to produce a solid wasteform.

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Design and Assessments of Liquid Metal Systems for a Fusion Power Reactor

This three-year research program at UCLA builds on the Fusion Engineering System Study (FESS) and has the major goal of identifying and accessing the most critical MHD/Mass & Heat Transfer phenomena associated with LM MHD flows in fusion breeding/cooling applications. The computed results and their analyses provide a strong basis to overcome present design limitations and will eventually lead to feasible, more effective solutions for LM systems of a fusion power reactor, such as breeding blankets and LM plasma facing components (PFCs). The project focuses on three research thrusts: Identification and characterization of the most important generic issues common to LM breeders (hereinafter called “Blanket”: ~47% of the resources); Design, implementation and assessments of two LM breeding-blanket concepts, DCLL and HCLL, for particular fusion devices, such as the US Fusion Nuclear Science Facility (FNSF) or the Fusion Pilot Plant (FPP) (hereinafter called “System Studies”: ~40% of the resources); Design and analysis of LM (Li) divertor concepts for FNSF or FPP, including scoping and detailed 2D and 3D computations (hereinafter called “LM PFC”: ~13% of the resources).

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Scoping Thermal Response Calculations of RNS Waste During Transport to and Disposal at the WIPP

Sandia National Laboratories (SNL) was contracted by the United States Department of Energy Environmental Management (DOE-EM), Los Alamos Field Office to perform mechanical and thermal scoping calculations as part of a study seeking to understand the ignitability risk of the Remediated Nitrate Salts (RNS) waste drums during transportation from the Waste Control Specialists (WCS) facility to Waste Isolation Pilot Plant (WIPP) and permanent disposal of the waste at WIPP. The scoping thermal simulations described in this report pertain to thermal calculations performed with a packaging system consisting of one Standard Waste Box (SWB) loaded with drums placed inside a Standard Large Box 2 (SLB2). During transportation, the SLB2 is inside Transuranic Package Transporter Model III (TRUPACT-III), which provides the third layer of the packaging. Once at the WIPP, it is assumed the SLB2 is extracted from the TRUPACT-III and maintained above ground, and then subsequently placed underground for permanent disposal. In these proposed configurations, the space between the SLB2 and the SWB is always filled by a layer of insulation consisting of air-filled glass microbubbles except for the bottom which rests directly on the SLB2. The thermal scoping calculations described in this report specifically address whether the introduction of external heat inputs, combined with the contributions from the internally generated radiolytic decay heat and chemical reactions, lead to an unstable thermal state during the time of its movement and placement in the permanent disposal location. The external heat inputs are of two forms: 1) ambient thermal irradiation (e.g., solar and ambient storage/disposal temperatures) and 2) accident-induced fire. Three scoping calculation scenarios were derived as representative, conservative scenarios: 1A) TRUPACT-III transient transportation, 1B) SLB2 48-hour outdoor storage with solar radiation, and 2) fully-engulfing fire during SLB2 handling or emplacement following a steady-state analysis in a 38 °C environment. All the simulated scenarios are conservative relative to the operational conditions expected for handling the waste package during transportation and placement in the WIPP underground disposal unit. The predictions obtained from simulating the three exposure scenarios revealed that adding the SLB2 and the air-filled glass microbubbles to the transport and storage/disposal configurations provides additional thermal protection of the drums beyond what the SWB provides alone, both during long-term above ground insolation and underground during a fire accident. Under the current transportation/storage/disposal concepts, the degree of protection provided by the packaging concept is sufficient to prevent the waste from being ignitable. The simulation results demonstrate that there is adequate margin to safely transport and place the RNS waste from WCS to the WIPP under the current operational concept.

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Annual Transuranic Waste Inventory Report – 2020 (Data Cutoff Date 12/31/2019)

The purpose of this Annual Transuranic Waste Inventory Report (ATWIR) – 2020 is to document the inventory estimate of transuranic (TRU) waste reported by the TRU waste generator sites as of December 31, 2019. This report also notes major changes to the inventory used for the ATWIR-2019 that had a data cutoff date of December 31, 2018. This updated inventory information is available to the U.S. Department of Energy (DOE) TRU waste complex, Waste Isolation Pilot Plant (WIPP) stakeholders, and regulators. The TRU waste inventory information is used for strategic planning, and supports the DOE Carlsbad Field Office (CBFO) input into documents (e.g., WIPP Documented Safety Analysis and National Environmental Policy Act analyses), planned changes, and other design changes as needed for the WIPP project.

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Annual Transuranic Waste Inventory Report – 2021 (Data Cutoff Date 12/31/2020)

The purpose of this Annual Transuranic Waste Inventory Report (ATWIR) – 2021 is to document the inventory estimate of transuranic (TRU) waste reported by the TRU waste generator sites as of December 31, 2020. This report also notes major changes to the inventory used for the ATWIR-2020 that had a data cutoff date of December 31, 2019. This updated inventory information is available to the U.S. Department of Energy (DOE) TRU waste complex, Waste Isolation Pilot Plant (WIPP) stakeholders, and regulators. The TRU waste inventory information is used for strategic planning, and supports the DOE Carlsbad Field Office (CBFO) input into documents (e.g., WIPP Documented Safety Analysis and National Environmental Policy Act analyses), planned changes, and other design changes as needed for the WIPP project.

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Annual Transuranic Waste Inventory Report – 2022 (Data Cutoff Date 12/31/2021)

The purpose of this Annual Transuranic Waste Inventory Report (ATWIR) – 2022 is to document the inventory estimate of transuranic (TRU) waste reported by the TRU waste generator sites as of December 31, 2021. This report also notes major changes to the inventory since the ATWIR-2021, which had a data cutoff date of December 31, 2020. This updated inventory information is available to the U.S. Department of Energy (DOE) TRU waste complex, Waste Isolation Pilot Plant (WIPP) stakeholders, and regulators. The TRU waste inventory information is used for strategic planning, and supports the DOE Carlsbad Field Office (CBFO) input into documents (e.g., WIPP Documented Safety Analysis and National Environmental Policy Act evaluations), performance assessments, planned changes, and other design changes as needed for the WIPP project.

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Brine Availability Test in Salt (BATS) FY23 Update

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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The Compelling Need for a Mid-Scale Stellarator Facility

In the pursuit of the goal of commercial fusion as an abundant and safe source of energy, the stellarator is a leading concept with compelling attractiveness and demonstrated performance. A new mid-size stellarator is needed to retire risks and innovate towards a high performance, economically attractive, stellarator Fusion Pilot Plant. In this presentation we, as a community of US researchers from Universities, National Laboratories, and Private Industry, involved in studying the stellarator concept, lay out the programmatic and technical motivation for a new and modern mid-size stellarator research facility. A new mid-scale stellarator is needed to realize the potential predicted by a solid body of theory and simulation along with advances in computational tools for optimization and non-linear turbulence modeling. Notably, it is possible to combine the advantages of the stellarator (steady state, no current drive, no disruptions) with the good confinement regularly achieved in tokamaks. The top priorities for experimental work, and the motivation for a mid-scale stellarator experiment are: turbulence control, non-resonant divertor, MHD stability at large beta, confinement of fast particles, and coil simplification. A new mid-size quasi-symmetric stellarator, built as a user facility, would complement existing research at Wendelstein 7-X and LHD and strongly augment private industry. It would provide a program of innovative research, concept validation, theoretical advancement, and workforce development. Growing support and interest for stellarators by the fusion community and private industry affirms this rationale.

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