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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 811 records · Page 45

Electrolytic Oxide Reduction of Plutonium Oxide Surrogates

Our research team has investigated electrolytic oxide reduction (EOR) as an improved metal production process versus the currently employed multiple cycle direct oxide reduction (MCDOR) process for the conversion of plutonium oxide to plutonium metal. Inherent advantages in safety, waste generation, efficiency, and operational ease make EOR an attractive alternative to traditional metal production practices. Phase I of the project consisted of the construction of a prototype electrochemical cell, and proof of concept experiments towards the reduction of SnO 2 and CeO 2 compounds. Phase II of the project was focused on the optimization of the cerium system in preparation for future plutonium EOR experiments. We observed the electrolytic reduction of cerium oxide resulting in mixed degrees of success, and discovered this was a result of parasitic side reactions and partial reduction. We employed cyclic voltammetry (CV) to identify the products of these side reactions and characterize partially reduced species. We also observed that, when metal was successfully produced by EOR, a large amount of passed charge was required. We concluded that this observation was due to several inefficiencies of the process relating to the reduction mechanism (e.g. inefficient use of cathodically produced calcium). We used our CV results to guide our optimization of the EOR of CeO 2 by refining our electrochemical method, cell geometry, and materials of construction. Finally, we developed a next generation cell, worked to establish a new molten salt electrochemical capability in the Plutonium Facility, and completed a strategy for plutonium experiments. Our electrochemical method to produce plutonium metal clearly supports the core mission of the laboratory. Furthermore, this project has allowed for the development of capabilities that will provide valuable data to programs interested in characterization and detection, as well as science of signatures. Additionally, establishing this capability in the plutonium facility will facilitate future safeguard studies that can assist with safeguard development in molten salt reprocessing flowsheets, and molten salt reactor designs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dense Plasma Focus Diagnostic Suite for the Surrogate Static Test

A Neutron Diagnosed Subcritical Experiment (NDSE) has been proposed to measure the reactivity of a subcritical ($k_{eff} <$ 1:0) plutonium experiment. This experiment requires a short, high-intensity neutron pulse delivered to the target material with precise timing. A feasibility study for the NDSE is being conducted jointly by National Security Technologies, LLC, and Los Alamos National Laboratory at Area 11 of the Nevada National Security Site. The goals of this study include characterizing and developing the proposed neutron pulse source, the fast photon detection system, and the shielding system to suppress scattering backgrounds.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Surrogate Model Development of Spent Fuel Degradation for Repository Performance Assessment

In model simulations of deep geologic repositories, UO 2 fuel matrix degradation typically begins as soon as the waste package breaches and groundwater contacts the fuel surface. The initial degradation rate depends on the timing of these events, burnup of the fuel, temperature, and concentrations of dissolved reactants. Estimating the initial rate of degradation is fairly straightforward, but as UO 2 corrosion products precipitate on the fuel surface and the movement of dissolved species between the fuel surface and environment is impeded by the precipitated solids, the rate is more difficult to quantify. At that point, calculating the degradation rate becomes a reactive-transport problem in which a large number of equations must be solved by iteration for a large number of grid cells at each time step. The consequence is that repository simulations, which are already expensive, become much more expensive, especially when hundreds or thousands of waste packages breach. The Fuel Matrix Degradation (FMD) model is the process model of the Spent Fuel and Waste Science and Technology (SFWST) campaign of the US Department of Energy (DOE). It calculates spent fuel degradation rates as a function of radiolysis, redox reactions, electrochemical reactions, alteration layer growth, and diffusion of reactants through the alteration layer. Like other similar fuel degradation process models, it is a complicated model requiring a large number of calculations and iterations at each time step.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Surrogate Suspension-Resuspension Study

The objective of this study was to conduct a series of tests looking at the deposition and resuspension of aerosol particles deposited onto multiple representative substrate surfaces for a range of particle sizes under varying environmental conditions. The benefit of this study is to provide additional insight into the understanding of early time resuspension from different mechanisms and compare to existing literature. The resuspension methods utilized in this study were full-scale and the substrates were representative of real- world ground level conditions. Multiple experiments were conducted to assess the impact on resuspension from the varying substrates and mechanisms. The results of this study show variations in the size distribution of aerosol as a function of height from the source resuspension factors. Additionally, the aerosolized mass concentration and resuspension factor were evaluated. The maximum resuspension factor was found to be on the order of 10 -4 m -1 which is higher than most resuspension factors found in literature but represents idealized conditions due to the well constrained experimental setup.

36 MATERIALS SCIENCE↗

Surrogate multi-fidelity data and model fusion for scientific discovery and uncertainty quantification in Earth System Models

This whitepaper addresses the Earth and Environmental Systems Sciences Division (EESSD)’s predictability challenges in modeling the integrated water cycle and data-model integration. Specifically, it focuses on reducing and characterizing the uncertainty in the representation of process models for unresolved physics, either due to model resolution or limited by the physical under standing or computational efficiency, and the use of observational data for in-situ process parameter optimization within ESM. The described methods may also be used to determine the nature of responses (e.g. strength and direction), and hence to identify critical processes that drive the overall ESM responses to perturbation in the forcing

54 ENVIRONMENTAL SCIENCES↗

Measurement of radiolytic hydrogen generation and impact of drying treatments on reactor exposed and surrogate aluminum materials

Technical challenges associated with dry storage of Aluminum-clad Spent Nuclear Fuel (ASNF) include a need to better understand the potential extent of gaseous molecular hydrogen (H 2 ) production through radiolytic degradation of the aluminum (oxy)hydroxide films present on ASNF. The characterization of radiolytic gas generation from ASNF (oxy)hydroxide layers has been identified as a key knowledge gap which poses a technical challenge to the long-term storage of ASNF. Task 2 of the action plan for the extended (>50 years) dry storage of ASNF addresses this gap. Previous radiolysis studies performed under Task 2 established baseline estimates of H 2 generation rates from the attendant hydrated oxides. The results confirmed that net radiolytic H 2 production has a dependency on absorbed gamma dose, as well as relative humidity and cover gas composition (air, nitrogen, and argon). Further experiments revealed that the physisorbed water on the samples may significantly impact the radiolytic H 2 yield. This phenomenon complicates the determination of H 2 generation rates for hydrated oxides, which may lead to inaccurate modeling predictions of the long-term H 2 yields in sealed storage systems containing ASNF, particularly when compared to spent fuel casks which have undergone some drying process intended to remove physically- and chemically-bound water. This report describes the testing methods utilized and the hydrogen generation results obtained in an investigation of the effects of gamma irradiation on aluminum materials for a variety of (oxy)hydroxide surface compositions and drying conditions. The testing methods included small-area aluminum material testing in ampules, and large-area aluminum material testing in steel vessels. Test material preparation, irradiation, and radiolytic H 2 measurement methods are summarized. The measured H 2 concentrations, which reflect the variable initial hydrated inventory and drying treatments, are compared to one another as well as to previously published data, to identify the primary factors affecting radiolytic H 2 generation rates and potential equilibrium H 2 concentrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗