Search NASA⌕ Search

SEARCH · Search NASA

Results for “UO2 Fuel”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 145 records · Page 8

Conceptual Design of a Scaled Voloxidation Apparatus for Testing with Used Nuclear Fuel

This report details the conceptual design overview for Department of Energy (DOE) Level 2 milestone M2FT-25IN030101021 titled “Complete conceptual design of a scaled voloxidation apparatus for testing with used nuclear fuel.” Advanced voloxidation uses high temperature nitrogen dioxide (NO2) gas to oxidize uranium dioxide (UO2) material to triuanium octoxide (U3O8) and ultimately to uranium trioxide (UO3). After consideration of multiple available options and inputs, a rotating advanced voloxidation design was determined to be the best fit for the needs of a full-scale apparatus. The system, which will be deployed in hot cell 4 of the Analytical Research Laboratory (ARL), has been designed to meet the space constraints of the facility while still accommodating at least 100g of used nuclear fuel (UNF). The apparatus consists of three main unit operations, including the gas panel, the custom furnace with reaction vessel, and the liquid scrubber.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Performance and properties evolution of near-term accident tolerant fuel: Cr-doped UO 2

Chromium-doped UO 2 fuel has received significant interest due to the ability for chromium to produce pellets with large average grain size (>30 μm), which has shown to increase fission gas retention during operation. Sintering of chromium-doped UO 2 pellets was pursued with oxygen potential and sintering atmosphere controlled to tailor the final microstructure of the material. Chromium additions in this study ranged from 750 to 7800 ppm. Cr concentrations were studied pre and post sintering using Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES). Effects of chromium content on lattice parameter and microstructure were examined with X-ray diffraction (XRD) and scanning electron microscopy (SEM). Contraction of the UO 2 lattice parameter was observed, as well as enlargement of grain size with increasing chromium content up to 4900 ppm Cr 2 O 3 . In addition, SEM indicated Cr incorporation within the matrix and the formation of chromium oxide precipitates throughout the microstructure at high Cr concentrations. Evaluation of thermophysical properties of Cr-doped UO 2 pellets were conducted up to 1200 °C to illustrate their evolution with increased dopant concentration and microstructural changes. The results show that grain size is maximized at 52 μm with Cr 2 O 3 concentration equal to 4900 ppm; however, grain size decreases at higher Cr 2 O 3 concentrations. No significant changes were observed in specific heat capacity, linear thermal expansion, and coefficient of thermal expansion compared to undoped UO 2 . The thermal conductivity also decreased through the incorporation of Cr 2 O 3 dopants above 750 ppm and is shown to be ~15 % lower than reported UO 2 values.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A molecular dynamics survey of grain boundary energy in uranium dioxide and cerium dioxide

Uranium dioxide (UO 2 ) is the primary fuel material that is used in current nuclear reactors. As one of the most fundamental material parameters, grain boundary (GB) energy strongly influences many fuel properties, and the influences depend on the characters and properties of individual GBs. Using molecular dynamics simulations, a high throughput survey of GB energy in UO 2 was carried out for the purpose of elucidating the roles of GB geometry such as misorientation and inclination, as well as the bonding nature of UO 2 , in affecting GB energy. GB energies in CeO 2 were calculated as well for comparison with UO2toinvestigate the generality of GB energy anisotropy in fluorite phase oxides. The results show significant GB energy anisotropy in both UO 2 and CeO 2 that is associated with the cubic symmetry of the fluorite structure. More interestingly, the GB anisotropy is found to be dependent not only on the crystal structure but also the ionic bonding. As such, the GB energy anisotropy in fluorite oxides has significant differences compared with that in fcc metals. We report that the data obtained and the increased knowledge on GB anisotropy will facilitate GB engineering for nuclear fuels with improved properties

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Optical Vibrational Spectroscopic Investigation of Natural and Synthetic Analogs of Uranyl Oxyhydroxyhydrate Minerals

Uranyl oxy-hydroxy-hydrate minerals are common alteration products of uraninite (UO2+x) which is chemically and structurally analogous to uranium dioxide nuclear fuel. Therefore, structural and spectroscopic investigations of these alteration minerals and their analogous anthropogenic counterparts can provide insight into the environmental behavior of nuclear fuel cycle materials. Previously, we compiled available vibrational spectroscopic data for uranyl minerals in the Compendium of Uranium Raman and Infrared Experimental Spectra (CURIES) and found that only 37% of known uranyl oxy-hydroxy-hydrate minerals had spectra readily available in the literature and existing databases for inclusion therein. Furthermore, no available infrared spectra for this mineral group were included in CURIES. To expand our understanding of the spectroscopic features of uranyl oxy-hydroxy-hydrates and the structural origins thereof, we collected, and now include in CURIES, Raman and infrared spectra for an additional 12 uranyl hydroxide phases. To better understand the impact of structural and compositional variations of these phases on their spectroscopic features, we compare Raman spectra of different anion sheet topological groups and of analogous phases hosting different counter cations. We identify spectroscopic variations related to differences in equatorial bonding and structural changes as a result of cation substitution. We also prepare a uranyl hydroxide phase via hydrolysis of uranyl fluoride (UO2F2) as an analog of hydrolysis reactions that occur in nuclear fuel cycle materials; and we find that the alteration product of UO2F2, despite chemical and structural similarities to uranyl oxy-hydroxy-hydrate minerals, is readily distinguishable from related mineral phases using Raman spectroscopy. In this work, we provide new insights into the structural origins of spectroscopic features in uranyl oxy-hydroxy-hydrate minerals, improve the average Raman spectrum for this group of minerals, and thereby improve capabilities for identifying these mineral species and related anthropogenic phases using Raman spectroscopy.

Barth, Brodie [ORNL] (ORCID:0000000256142601)↗

Phase-field modeling for restructuring in the dark zone of high burnup UO 2

This report summarizes the mesoscale modeling work performed in fiscal year 2024 under the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program to capture the microstructural evolution and restructuring observed in the dark regions of high burnup UO 2 nuclear fuel. This is the first attempt to realistically simulate the restructuring behavior observed in different region of a high burnup fuel. We employ a grand-potential based phase-field model to concurrently evaluate the formation of subgrains and growth of fission bubbles within the fuel. A energy-based subgrain formation criteria is introduced to simulate the restructuring process. Effect of different initial conditions and different modeling parameters are studies systematically to capture how each of these parameters influence the characteristics of the restructured fuel. It is observed that the subgrain formation begins around existing fission gas bubbles and then proceeds towards triple junctions, grain boundaries and grain interiors. It is demonstrated that restructuring is influenced by a combination of initial dislocation densities, subgrain formation rate, and temperature. Rate of restructuring increases with increase in fuel temperature. A restructuring bias is observed within the microstructure due to variation in defect accumulation among different grains. Furthermore, bubble sizes and distribution does not have a significant effect on rate of restructuring. The predicted microstructures resembles the characteristics of the restructured regions as observed in experiments. Finally, a correlation is presented that demonstrates the evolution of the restructuring volume fraction as a function of local effective burnup. This work provides a first of its kind restructuring model for darkzone that can be used by BISON for performance prediction of high burnup UO 2 fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Charge-lattice coupling and the dynamic structure of the U–O distribution in UO 2+x

The different structures and behaviors of UO 2+x observed in crystallographic and local structure measurements were examined by extended X-ray absorption fine structure (EXAFS) measurements of pristine UO 2.0 , p + and He 2+ irradiated UO 2.0 , and, at multiple temperatures, bulk U 4 O 9 and U 3 O 7 and thin film U 4 O 9-δ on an epitaxial substrate. The disorder caused by irradiation is mostly limited to increased widths of the existing U–O/U pair distributions, with any new neighbor shells being minor. As has been previously reported, the disorder caused by oxidative addition to U 4 O 9 and U 3 O 7 is much more extensive, resulting in multisite U–O distributions and greater reduction of the U–U amplitude with different distributions in bulk and thin-film U 4 O 9 . This includes the significant spectral feature near R = 1.2 Å for all U 4 O 9 and U 3 O 7 samples fit with a U-oxo type moiety with a U–O distance around 1.7 Å. In addition to indicating that these anomalies only occur in mixed valence materials, this work confirms the continuous rearrangement of the U–O distributions from 10 to 250 K. Although these variations of the structure are not observed in crystallography, their prominence in the EXAFS indicates that the dynamic structure underlying these effects is an essential factor of these materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mesoscale modeling to inform Bison models of accident tolerant fuel concepts

U 3 Si 2 and doped UO 2 have been under investigation in recent years as potential accident-tolerant fuel concepts. In this report, lower-length scale studies of these fuel concepts carried out during Fiscal Year 2020 are detailed. U 3 Si 2 is a potential accident-tolerant fuel that shows promise due to its high thermal conductivity and higher uranium density relative to UO 2 . However, its swelling and fission gas release behavior in light water reactor (LWR) conditions is relatively unknown. To provide mechanistic insight and determine parameters for engineering-scale fuel performance modeling of pellet-form U 3 Si 2 , phase-field simulations of the growth, interconnection, and venting of intergranular fission gas bubbles were performed. The fractional coverage of the grain boundary and the fraction of bubble area that is vented were calculated as a function of time. From the simulation data, the fractional grain boundary coverage at saturation, an important parameter needed in engineering-scale modeling of swelling and fission gas release, was determined. Multiple simulations were run to determine the uncertainty in the calculated value. The effect of model assumptions and input parameters that are not well known was evaluated. Simulation results are compared to related theoretical and computational work. Based on the simulation results, a value of 0.60 for the fractional grain boundary coverage at saturation is recommended for U 3 Si 2 fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Technology Development of a High-Capacity High-Assay Low Enriched Uranium Transportation Concept

This paper discusses the technology development (TD) efforts that led to the development of a High-Capacity High-Assay Low Enriched Uranium Transportation (HALEU) transportation concept. In 2018, the Department of Energy (DOE) Office of Nuclear Technology and Research Development tasked Idaho National Laboratory (INL) to investigate strategies to transport large quantities of HALEU. To complete this task, INL collaborated with Pacific Northwest National Laboratory and Oak Ridge National Laboratory. The project was completed in 2020, and one of the project outcomes was a transportation concept that consisting of five individual Type B packages transported on a single legal-weight truck (LWT). The total payload capacity of this concept is 1,881 kg (4,149 lb) of HALEU in the form of uranium dioxide (UO2) powder. The concept utilizes an existing Type B packaging design carrying a novel fuel basket design with an incorporated flux trap. The basket can be loaded with 18 individual fuel canisters. The research collaboration investigated the U.S. certification potential of this concept. This part of the project included evaluations of criticality safety, radiological safety, thermal safety, structural integrity, and confinement under hypothetical accident scenarios of transport. The results of these evaluations demonstrated a promising potential for U.S. certification of this concept. Eventually, the described efforts led to the pursuance and issuance of a U.S. patent, thus, protecting the associated intellectual property (IP). Current short-term goals include making this IP available to private industry partners for licensing, directly supporting DOE’s objectives of accelerating commercialization of national laboratory-generated IP. If additional funding becomes available, long-term research goals could include exploring the feasibility of transporting other uranium chemical forms (e.g., UF4) with this concept, or refining operational procedures to load or unload the packagings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Destructive PIE and Safety Testing of Six AGR-2 UO 2 Capsule 3 Compacts

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s second irradiation experiment (AGR-2) was irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) from June 2010 to October 2013 (Collin 2014). The fuel compacts in this experiment held either tristructural isotropic (TRISO)-coated spherical kernels of uranium oxide (UO2) or TRISO-coated kernels containing both uranium carbide and uranium oxide phases (UCO). There were six separately monitored and controlled capsules in the AGR-2 test train. Capsule 3 held twelve compacts containing UO2-TRISO particles fabricated by BWX Technologies Nuclear Operations Group. The AGR-2 TRISO particles were fabricated in a pilot-scale fluidized-bed chemical vapor deposition (FB-CVD) furnace with a coating chamber inner diameter of 150 mm (Phillips, Barnes, and Hunn 2010), which was a change from the first irradiation experiment (AGR-1) particles that had been coated in a lab-scale FB-CVD coating system with a chamber inner diameter of 50 mm (Lowden 2006). The TRISO particles were overcoated with resinated graphite flake at Oak Ridge National Laboratory (ORNL), and the overcoated particles were pressed into one-inch-long, half-inch-diameter cylinders (Hunn, Montgomery, and Pappano 2010). Each cylindrical compact held an average of 1,543 TRISO particles with 9.6% enriched UO2 kernels that had a nominal diameter of 500 μm (Hunn, Savage, and Silva 2012). Capsule 3 compacts were irradiated to average calculated burnups of 9.01–10.69% fissions per initial metal atom (FIMA), and the average calculated fluences of fast neutrons with energies E n > 0.18 MeV were 3.05–3.53×10 25 n/m 2 (Sterbentz 2014). The calculated time-average, volume-average Capsule 3 compact temperatures were 996–1,062°C. However, Capsule 3 compact temperatures varied several hundred degrees across each compact, and the timeaverage minimum (TA min ) and time-average maximum (TA max ) temperatures were between 889–999°C and 1,072–1,105°C, respectively (Hawkes 2014). After irradiation, the AGR-2 test train was transferred from ATR to the INL Materials and Fuels Complex for inspection and disassembly (Ploger, Demkowicz, and Harp 2015). The initial inspection included dimensional metrology of the compacts and graphite fuel holders. Like all the AGR-2 compacts, the compacts in Capsule 3 shrank slightly during irradiation, as expected, with an average length reduction of 1.07–1.24% and an average diameter reduction of 0.13–0.41%. Post-irradiation examination (PIE) of the capsule components was completed to measure select fission products ( 90 Sr, 110m Ag, 134 Cs, 137 Cs, 144 Ce, and 154 Eu) outside the compacts (Stempien and Demkowicz 2020). This involved gamma counting of the graphite and graphoil spacers at the top and bottom of each capsule, acid leaching for radiochemical analysis of fission products on the metallic capsule components, and burn-leach analysis of the graphite holders. The total amount of 110mAg measured on the Capsule 3 components was 13% of the calculated capsule inventory. This was significantly lower than the amount of 110m Ag measured on the three UCO capsule components, which ranged from 32–70%. The lower 110m Ag release in Capsule 3 was likely due to lower peak temperatures compared with the UCO fuel capsules (Hawkes 2014). Measured inventories of the other select fission products were also lower in Capsule 3.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Microscopy Report on UCO Fuel Kernels from Selected AGR-1 and AGR-2 Experiments

A variety of neutron irradiation experiments were completed at Idaho National Laboratory (INL) on tristructural isotropic (TRISO) coated particles contained in a graphitic matrix as part of the Advanced Gas Reactor (AGR) fuel development and qualification program. Although the initial advanced microscopy and microanalysis studies on AGR-1 particles focused predominantly on the SiC layer?s role as the main fission-product containment, studies were further expanded to evaluate UCO kernels of selected AGR-1 and AGR-2 coated particles. Fuel kernels tested in the AGR-1 and AGR-2 experiments is composed of a mixture of UO2 and UC, with a nominal as-fabricated stoichiometry of UO1.37 C0.35 and UO1.43 C0.39, respectively. These as-fabricated kernel-stoichiometry values are determined at the completion of kernel fabrication and do not account for any changes that will occur during the subsequent coating and compacting processes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling mesoscale fission gas behavior in UO2 by directly coupling the phase field method to spatially resolved cluster dynamics

Abstract Fission gas release within uranium dioxide nuclear fuel occurs as gas atoms diffuse through grains and arrive at grain boundary (GB) bubbles; these GB bubbles grow and interconnect with grain edge bubbles; and grain edge tunnels grow and connect to free surfaces. In this study, a hybrid multi-scale/multi-physics simulation approach is presented to investigate these mechanisms of fission gas release at the mesoscale. In this approach, fission gas production, diffusion, clustering to form intragranular bubbles, and re-solution within grains are included using spatially resolved cluster dynamics in the Xolotl code. GB migration and intergranular bubble growth and coalescence are included using the phase field method in the MARMOT code. This hybrid model couples Xolotl to MARMOT using the MultiApp and Transfer systems in the MOOSE framework, with Xolotl passing the arrival rate of gas atoms at GBs and intergranular bubble surfaces to MARMOT and MARMOT passing evolved GBs and bubble surface positions to Xolotl. The coupled approach performs well on the two-dimensional simulations performed in this work, producing similar results to the standard phase field model when Xolotl does not include fission gas clustering or re-solution. The hybrid model performs well computationally, with a negligible cost of coupling Xolotl and MARMOT and good parallel scalability. The hybrid model predicts that intragranular fission gas clustering and bubble formation results in up to 70% of the fission gas being trapped within grains, causing the increase in the intergranular bubble fraction to slow by a factor of six. Re-solution has a small impact on the fission gas behavior at 1800 K but it has a much larger impact at 1000 K, resulting in a twenty-times increase in the concentration of single gas atoms within grains. Due to the low diffusion rate, this increase in mobile gas atoms only results in a small acceleration in the growth of the intergranular bubble fraction. Finally, the hybrid model accounts for migrating GBs sweeping up gas atoms. This results in faster intergranular bubble growth with smaller initial grain sizes, since the additional GB migration results in more immobile gas clusters reaching GBs.

Kim, Dong-Uk↗

High density UO2 and high thermal conductivity UO2 composites by spark plasma sintering (SPS)

Embodiments of the invention are directed to a method for production of a nuclear fuel pellet by spark plasma sintering (SPS), wherein a fuel pellet with more than 80% TD or more than 90% TD is formed. The SPS can be performed with the imposition of a controlled uniaxial pressure applied at the maximum temperature of the processing to achieve a very high density, in excess of 95% TD, at temperatures of 850 to 1600° C. The formation of a fuel pellet can be carried out in one hour or less. In an embodiment of the invention, a nuclear fuel pellet comprises UO 2 and a highly thermally conductive material, such as SiC or diamond.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A combined theoretical-experimental investigation of thermal transport in low-dose irradiated thorium dioxide

During reactor operation, nuclear fuels are subject to extreme temperature and irradiation conditions which can significantly degrade the fuel's thermal transport properties. The reduction in thermal conductivity of the fuel as a result of irradiation-induced lattice defects is arguably the most important fuel performance metric in regard to reactor efficiency and safety. Because thorium dioxide (ThO2) is suitable as a model system for more complex materials such as UO2 and its mixed oxides, we present a theoretical investigation of thermal conductivity reduction seen in defect-bearing thorium dioxide and compare directly to experimental measurements. Phonon-mediated thermal transport of the fuel is modeled by a solution to the Boltzmann transport equation (BTE) for phonons. A cluster dynamics (CD) model for lattice defect evolution during irradiation predicts defect densities which are used as input to the BTE for modeling phonon-defect scatterings. Phonon scatterings by lattice defects include those from point defects and vacancy clusters and interstitial clusters of various sizes. The CD model is benchmarked against structural defect characterization of irradiated thorium dioxide using electron microscopy. Thermal conductivity predicted by the BTE model is compared to measured values for irradiated thorium dioxide specimens below room temperature to isolate effects of phonon-defect scattering from intrinsic 3-phonon processes, which dominate at higher temperatures. The computed conductivity values are in partial agreement at temperatures close to room temperature while slight deviations are observed at the lowest measured temperatures, suggesting that implemented phonon-defect scattering cross-section expressions may not be adequate for low temperatures. The presented work provides a necessary investigation of the influence of irradiation induced defects on fuel performance and represents a first step toward a full characterization of phonon mediated thermal transport in irradiated materials with complex defect microstructure.

36 MATERIALS SCIENCE↗

Multiscale Modeling of Cr 2 O 3 -doped UO 2 Creep and Fracture

The pursuit of UO 2 fuel with various dopants (e.g., Cr 2 O 3 , Al 2 O 3 ) for improved accident tolerance due to larger grain sizes and suspected reductions in fission gas release and creep requires advanced modeling and simulation tools. These tools enable rapid multiscale development and understanding of material behavior in regimes where experimental measurements may be lacking. This work builds upon previous multiscale modeling efforts for fission gas behavior of Cr 2 O 3 -doped UO 2 to begin looking at the effects of dopants on mechanical properties with a particular focus on creep and fracture. The results indicate that dislocation climb is the most dominate creep mechanism at almost all temperatures with sensitivity analyses further providing evidence in support of that claim. Limited experimental data from the Advanced Fuels Campaign (AFC) program in the U. S. Department of Energy on tensile strength of Cr 2 O 3 -doped UO 2 indicates that fracture may be less severe in doped specimens. The results on creep and fracture are preliminary given the large uncertainty associated with the models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multiscale Modeling of Cr 2 O 3 -doped UO 2 Creep and Fracture (Rev.1)

The pursuit of UO 2 fuel with various dopants (e.g., Cr 2 O 3 and Al 2 O 3 ) for improved accident tolerance due to larger grain sizes and suspected reductions in fission gas release and creep requires advanced modeling and simulation tools. Such tools enable rapid multiscale development and enhanced understanding of material behavior in regimes for which experimental measurements may be lacking. This work builds on previous multiscale modeling efforts targeting the fission gas behavior of Cr 2 O 3 -doped UO 2 , in order to begin exploring the effects of dopants on mechanical properties, with a particular focus on creep and fracture. The results indicate that dislocation climb is the most dominate creep mechanism at almost all temperatures, and sensitivity analyses provide evidence in further support of this claim. The limited experimental data generated by the U.S. Department of Energy’s Advanced Fuels Campaign (AFC) on the tensile strength of Cr 2 O 3 -doped UO 2 indicate that fracture may be less severe in doped specimens. The results on creep and fracture are preliminary, given the large degree of uncertainty associated with the models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

In-Situ Transmission Electron Microscopy Study of the Evolution of Extended Defects in Oxide Nuclear Fuels

In-situ transmission electron microscopy (TEM) with simulated extreme environments is an effective tool for understanding and tracking microstructural changes down to the atomic scale. The objective of this research is to study the effect of temperature on the evolution of extended defects in ThO2 and UO2. Here, we present in-situ TEM isochronal thermal annealing experiments using a micro-electro-mechanical-system (MEMS)-based heating holder. ThO2 and UO2 single crystal specimens were grown inside an inert silver ampoule using hydrothermal synthesis. Both samples were irradiated using 2 MeV protons at 600oC up to 0.1 dpa at Texas A&M University’s Accelerator Laboratory. Fig. 1a shows a weak-beam dark field TEM image of ThO2 after irradiation, indicating the presence of faulted 1/3 <111> type dislocation loops. This presentation will discuss the effect of annealing temperature (600oC, 800oC, 1000oC, 1100oC, etc.) on dislocation loop density, size and distribution, loop nature (interstitial/vacancies) and Burgers vector, as well as the formation of voids in both ThO2 and UO2. This work will also discuss the interaction between defects during annealing. The in-situ TEM annealing cycle is shown in Fig 1b. This research significantly improves the understanding of defect behavior in oxide nuclear fuels with temperature and will aid computational modeling efforts. This work was supported as part of the Center for Thermal Energy Transport under Irradiation (TETI) Energy Frontier Research Center, funded by the U.S. Department of Energy Office of Science.

36 MATERIALS SCIENCE↗