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Flowsheet Development for the University of Tokyo YAYOI (UTY) Fuel

The Savannah River National Laboratory (SRNL) was requested by H-Canyon Engineering to determine the flowsheet parameters needed to dissolve and store the YAYOI Material Test Reactor (MTR) uranium fuel safely and efficiently. In response to this request, a literature review of existing SRNL MTR dissolution flowsheets and general fuel dissolution literature in the nuclear fuel processing industry was performed to evaluate chemical dissolution parameters required to dissolve the YAYOI fuel and the tin-plated carbon steel product cans (PC). Based on past dissolutions of similar fuel in the H-Canyon and open literature reviews on chemical dissolution of spent nuclear fuel (SNF), the following conclusions and flowsheet recommendations were made.

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Small-Scale Drying: FY2020 Interim Report

This report documents the interim experimental status of small-scale drying tests currently being performed at Pacific Northwest National Laboratory. These small-scale drying tests are to develop the technical bases for sensors, techniques, and approaches that will be used to address the challenges faced when determining moisture content from gas samples taken at the North Anna Nuclear Generating Station for the High Burnup Demonstration Project. Specifically, the purpose of these tests is to support Sandia National Laboratories gas sample methods and analyses through a series of small-scale experiments. Key focus areas include performing tests to: • Correlate sample bottle measurements to in-cask conditions • Estimate the amount of trapped and absorbed water on cask features and surfaces that can contribute to water vapor • Assess the accuracy of the hygrometer used in the measurements under similar conditions • Identify additional methods for measuring humidity in casks easily and accurately using lessons-learned from Sandia National Laboratories, including direct gravimetric and isotopic tracer techniques. To address these topics this report outlines a series of five tests and any data collected to date that were planned for FY 2020 that include 1) humidity measurement method development, 2) gas bottle sampling tests, 3) surface drying tests on cladding, 4) small-scale drying of cladding, and 5) small-scale drying of guide-tube/dashpots. This interim report documents the experimental background, design and progress of these small-scale drying tests. Further data gathered will be summarized in the FY 2021 report.

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Developing an Analytical Framework for Cumulative Effects

The extended dry storage scenario for spent nuclear fuel (SNF) in the United States introduces the possibility of more than one transportation campaign to move the SNF from its point of origin to one or more interim storage facilities before it reaches its final destination. While the structural integrity of SNF and its storage and transportation systems are often evaluated under single event loading conditions, the reality is that a single SNF system will experience multiple structural loading events during its life cycle, the number and severity of which will depend on its individual circumstances. SNF systems will also be subjected to environmental exposure that will affect their temperature and the potential for cracks to develop in the SNF canister walls. Considered separately, many different events and scenarios might be strong enough to challenge the integrity of SNF cladding and the storage and transportations canisters that contain SNF. But considered together, over the full life cycle of an SNF system, there is the possibility that individual low-magnitude events could cause enough incremental damage to components of the SNF system to challenge its structural integrity if the time span is long enough or if the life cycle includes a sufficient number of loading events. The concern is that the cumulative effect of relatively small mechanical loads, thermal stresses, or cracking can add up to conditions that could compromise SNF or its containment structures. This report is a first step in establishing an analysis framework for evaluating these cumulative effects.

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GOTHIC Aerosol Source Depletion Studies

Pacific Northwest National Laboratory has continued work to develop an aerosol-laden flow modeling capability with the Generation of Thermal Hydraulic Information in Containment (GOTHIC TM ) computer code to perform simulations for thermal hydraulic conditions and aerosol transport and deposition in spent fuel casks. This report describes our recent work to expand our model that was originally developed in 2019 to allow for thermal characterization, carrier gas flow determination, and tracking of particulate behavior throughout the entire canister volume. This was achieved through conversion of decay heat source in all fuel tubes within the model from heaters to thermal conductors in GOTHIC as well as remeshing the internal volume of the canister. These model improvements allowed for simulations of base case scenarios for comparison of similar efforts by our collaborators with alternative tools at Sandia and Oak Ridge. Several characteristics of the GOTHIC code were elucidated by this effort and were documented for consideration in how the code is used for this effort moving forward. For instance, treatment of particle size distributions, initial spatial distributions, mesh gradients, and minimum volume concentrations were identified as important issues for consideration. Ultimately, the current version of the code is capable of tracking temperatures, flow rates, and particle behavior throughout the canister internal volume. This report presents predicted depletion times and preferred deposition patterns within the canister. Additionally, this report documents code performance and insights for further model development and use for comparisons to other codes and for predicting system behavior in experiments being performed and planned by our collaborators.

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Non-Neutron Transmutation of Used Nuclear Fuel (Final Report)

The primary goal of this study is to develop a national facility concept for transmuting long-lived fission products (LLFP) to substantially reduce the disposal impact by minimizing the need for a geologic-timescale repository. As a charter for this study, the national transmutation facility was required to reduce the radiotoxicity and decay heat of LLFP isotopes by at least 90% relative to their values at discharge from a commercial LWR, while consuming less than 10% of the reactor's energy. The identified LLFP isotopes are Se-79, Zr-93, Tc-99, I-129, Sn-126, and Cs-135, whose radiotoxicity is about 99% of the total radiotoxicity of all fission products at 1,000 years. Approximately ~72 kg of LLFPs is discharged every year from a 1,000 MWe commercial or advanced nuclear reactor. First, LLFP transmutation options with non-neutron beams (photons and protons) were explored. The study concluded that LLFP transmutation is feasible with high-energy, high-intensity photons or protons, but impractical on an engineering scale due to low transmutation rates and the high energy requirements to produce the desired photon or proton beams. As alternatives, LLFP transmutation options with neutrons from fission, fusion, and spallation reactions were additionally explored. The transmutation options using advanced critical reactors are attractive only for selective LLFP isotopes because the production rates of several LLFP isotopes (Zr-93, Sn-126, and Cs-135) from fission reactions are larger than the transmutation rates. The transmutation options with only spallation neutrons are favorable to transmute all LLFP isotopes, but as a tradeoff, the net transmutation rates are reduced. The national transmutation facility concept was developed following an exploration of transmutation options using various incident particles. The proposed national LLFP transmutation comprises a dedicated molten-salt reactor (MSR), a proton accelerator, and a spallation neutron-based transmuter. The MSR power was set at 300 MWt and 120 MWe, with the thermal power approximately 10% of that of a commercial 1,000 MWe PWR. The electricity generated by the MSR powers the accelerator and transmuter. The accelerator produces 1 GeV, 30 mA protons, which are introduced into the spallation neutron-based transmuter. The spallation neutron-based transmuter consists of a central spallation target and LLFP target pins merged in a heavy water tank. The six LLFP isotopes are separated into two groups. Tc-99, I-129, and Se-79, having larger neutron cross sections, belong to group A, while Zr-93, Sn126, and Cs-135, having smaller neutron cross sections, belong to group B. Then, for effective transmutation, LLFPs in groups A and B are transmuted in the dedicated MSR and in a spallation neutron-based transmuter, respectively. The estimated capital cost of the national transmutation facility is approximately $\$$3.1B, and its annual O&M cost is expected to be ~$\$$182M. Radiotoxicity and decay heat of LLFPs were calculated and compared with those of the original LLFPs. It was assumed that the targets were made with elementwise LLFP rather than isotopic LLFP, owing to the potentially high cost of isotopic separation from used nuclear fuels. The decay heat of LLFPs can be reduced by more than 90% using a single national transmutation facility. However, radiotoxicity decreases by 79–84%, which does not meet the transmutation performance requirement, primarily because Cs-135 is produced rather than depleted. Thus, to meet the design requirement, Cs-135 should be separated from other Cs isotopes and irradiated in a spallation neutron-based transmuter. Then, radiotoxicity decreases by ~92%.

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Determination and Comparison of Parameters from Cyclic Voltammetry of LaCl 3 in Eutectic LiCl-KCl

Electrochemical measurements of LaCl 3 were obtained in eutectic LiCl-KCl at 773 K. Cyclic voltammetry data were acquired using a tungsten electrode LaCl 3 amounts in the molten salt in the range of 0.5 to 3.0 wt%. Both cyclic voltammetry and Tafel analyses of the data resulted in calculation of values for the charge transfer coefficient (0.262), diffusion coefficient (1.67 × 10 -5 cm 2 s -1 ), exchange current density (0.0148 to 0.0473 A cm -2 ), and charge transfer resistance (0.404 to 1.99 Ω) related to lanthanum ions in the molten salt. Calculated values were compared to those available in the literature. The values of parameters found in literature varied significantly in comparison to those in the present study due to dissimilar experimental conditions, e.g., electrode material, temperature, and LaCl 3 concentration.

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Water Sorption/Desorption Characteristics of Eutectic LiCl-KCl Salt-Occluded Zeolites

Molten salt consisting primarily of eutectic LiCl-KCl is currently being used in electrorefiners in the Fuel Conditioning Facility at Idaho National Laboratory. Options are currently being evaluated for storing this salt outside of the argon atmosphere hot cell. The hygroscopic nature of eutectic LiCl-KCl makes is susceptible to deliquescence in air followed by extreme corrosion of metallic cannisters. In this study, the effect of occluding the salt into a zeolite on water sorption/desorption was tested. Two zeolites were investigated: Na-Y and zeolite 4A. Na-Y was ineffective at occluding a high percentage of the salt at either 10 or 20wt% loading. Zeolite-4A was effective at occluding the salt with high efficiency at both loading levels. Weight gain in salt occluded zeolite-4A (SOZ) from water sorption at 20% relative humidity and 40°C was 17wt% for 10% SOZ and 10wt% for 20% SOZ. In both cases, neither deliquescence nor corrosion occurred over a period of 31 days. After hydration, most of the water could be driven off by heating the hydrated salt occluded zeolite to 530°C. However, some HCl forms during dehydration due to salt hydrolysis. Over a wide range of temperatures (320–700°C) and ramp rates (5, 10, and 20°C min -1 ), HCl formation was no more than 0.6% of the Cl - in the original salt.

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Damaged Fuel in the United States

Over the years of commercial nuclear power plant operations in the United States (U.S.), many fuel assemblies have lost the capability to perform all of their desired functions. These assemblies have lost the capability to be handled, stored, or transported to meet regulations resulting in them being classified as damaged fuel. The causes of these failed assemblies are diverse and plant-specific. The majority of these failed assemblies are contained in a damaged fuel can that will be used in conjunction with a storage and/or transportation system. The storage and transportation systems have a limit on how many slots can be filled with damaged fuel cans. A damaged fuel can is generally a stainless steel container that confines damaged SNF and is closed on its end by screened openings. These screened openings allow gaseous and liquid media to escape but minimize the dispersal of gross particulate material. Out of an abundance of caution a few reactors have loaded high burnup fuel into damaged fuel cans. Damaged fuel is not licensed for storage or transport in the U.S., because the regulations for storage and transport do not specify exactly how to classify damaged fuel. Instead the regulations license/certify packages that specify approved contents. Damaged fuel must be included in the approved contents to be a viable option. In many cases damaged SNF is encapsulated in a damaged fuel can to ensure it can confine gross fuel particles, debris, and or damaged assemblies to a known volume within a loaded cask. This damaged fuel can may then be utilized in the same way as an assembly in a storage and transportation design system. Some storage cask systems utilize top and bottom plugs to confine debris in damaged fuel. The most recent domestic documentation on damaged SNF was performed by the U.S. Energy Information Administration (EIA) and used data from U.S. reactors concluding in June 30th 2013 to produce Form GC-859, “Nuclear Fuel Data Survey”. Based on this form there were 136,821 boiling water reactor (BWR) spent nuclear fuel (SNF) assemblies and 104,647 pressurized water reactor (PWR) SNF assemblies for a total of 241,468 SNF assemblies in the U.S. Out of these 241,468 SNF assemblies, 4,521 assemblies were classified as failed. Some assemblies were also disassembled and the fuel rods or pieces of fuel rods were combined together to make a consolidated assembly. A consolidated assembly may include damaged fuel, or it could have been consolidated as part of a demonstration project. The GC-859 data includes 2,550 consolidated assemblies containing between 0 and 264 whole fuel rods. These consolidated assemblies could be placed in single assembly canisters and stored in the spent fuel pool. For dry storage and transportation, a single assembly canister is generally placed in a damaged fuel can. In addition to the consolidated assemblies, 2,391 uncanistered fuel rod pieces exist, which were removed from 494 assemblies.

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Fueling Nuclear Research at MFC: The Environmental Backbone of Nuclear Operations

The National Environmental Policy Act (NEPA) review guidelines are an essential part of the approval process of any construction or modification being done at Idaho National Laboratory (INL). The Material and Fuels Complex (MFC) Environmental team is responsible for writing and reviewing Environmental Impact Statements (EISs), Environmental Assessments (EAs), Environmental Compliance Permits (ECPs), Air Permitting Applicability Determinations (APADs), and other NEPA compliance documentation. This documentation allows for innovation in MFC research by permitting the introduction of new laboratory equipment, research facilities, and materials for researchers to use in their experiments. Without the work of the Environmental team, nuclear research and operations at MFC would not be possible.

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EBR-II Driver Fuel Cladding Hull Analytical Data

Sharing EBR-II driver fuel cladding hull data with General Atomics under NDA No. 20NDA155. Data share is needed to advance discussions regarding process technologies to decontaminate separated cladding hulls

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DOE Standard Canister Loading Methodology Poster

Over 250 different types of spent nuclear fuel (SNF) are managed by the U.S. Department of Energy (DOE) at the Idaho National Laboratory (INL). The current configuration of SNF at INL is not transportable off-site. In the Yucca Mountain Repository License Application, the SNF was to be loaded into DOE Standard Canisters which are capable of storage, transportation, and eventual disposal using the proper overpacks. The DOE Standard Canister will allow INL to place the SNF in a Road-Ready configuration in preparation for transportation off-site. The focus of this work is development of a general loading methodology for the DOE Standard Canister. This methodology is to be general enough that it will apply to all SNF to be loaded into the DOE Standard Canister. The main sections of the methodology to be outlined are prerequisites before loading (including any issues with materials such as inserts or baskets), loading of SNF, and canister closure and quality assurance (including welding and inspection). Each subsection will analyze and provide the bases for each step.

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MULTIPHYSICS-MODELING OF FIRE-INDUCED URANIUM AEROSOL FORMATION – A-POSTERIORI BENCHMARKING OF EXPERIMENTS

The formulation and solution of a model that properly described the temperature profiles of uranium in fire conditions was prepared, verified and validated, to support a-posteriori benchmarking of historical experiments. Data from the multi-physics model combined with data regression from the experiments provides a useful tool for exploring sources of potential bias in historical experiments. The approaches used are augmented by visual observations and photographic evidence allowing for correlations between various phenomena, independent of whether or not that specific phenomena are part of the validated model. In this manner, the validated model is a tool for a-posteriori benchmarking, and not a model designed to replicate the experimental output exactly for any specific experiment. For experiments like the Clark (2015) experiments, this integrated model (including chemistry) demonstrated that the largest bias was associated in the metallurgy of the coupons. The model developed does serve as a basis for defending which of the historical alloys tested are the most appropriate for any other alloy being considered (e.g., one that has not yet been tested). The model identifies key reactions that impact uranium chemistry and can significantly bias experimental results. Through use of the model and energy balances, data from historical experiments by Elder and Tinkle (1980) were regressed and benchmarked. This study identifies that all uranium alloys are not equal and that there are distinct differences between the dominant alloys representing distinct metallurgical phases.

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