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At least 91 records · Page 5

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

A Historical Review of Cermet Fuel Development and the Engine Performance Implications

To better understand Cermet engine performance, examined historical material development reports two issues: High vaporization rate of UO2, High temperature chemical stability of UO2. Cladding and chemical stabilizers each result in large, order of magnitude improvements in high temperature performance. Few samples were tested above 2770 K. Results above 2770 K are ambiguous. Contemporary testing may clarify performance. Cermet sample testing during the NERVA Rover era. Important properties, melting temperature, vaporization rate, strength, Brittle-to-Ductile Transition, cermet sample test results, engine performance, location, peak temperature.

Nuclear Propulsion

Irradiation of TZM: Uranium dioxide fuel pin at 1700 K

A fuel pin clad with TZM and containing solid pellets of uranium dioxide was fission heated in a static helium-cooled capsule at a maximum surface temperature of 1700 K for approximately 1000 hr and to a total burnup of 2.0 percent of the uranium-235. The results of the postirradiation examination indicated: (1) A transverse, intergranular failure of the fuel pin occurred when the fuel pin reached 2.0-percent burnup. This corresponds to 1330 kW-hr/cu cm, where the volume is the sum of the fuel, clad, and void volumes in the fuel region. (2) The maximum swelling of the fuel pin was less than 1.5 percent on the fuel-pin diameter. (3) There was no visible interaction between the TZM clad and the UO2. (4) Irradiation at 1700 K produced a course-grained structure, with an average grain diameter of 0.02 centimeter and with some of the grains extending one-half of the thickness of the clad. (5) Below approximately 1500 K, the irradiation of the clad produced a moderately fine-grained structure, with an average grain diameter of 0.004 centimeter.

Mcdonald, G. E.

Design, fabrication, and operation of capsules for the irradiation testing of candidate advanced space reactor fuel pins

Fuel irradiation experiments were designed, built, and operated to test uranium mononitride (UN) fuel clad in tungsten-lined T-111 and uranium dioxide fuel clad in both tungsten-lined T-111 and tungsten-lined Nb-1% Zr. A total of nine fuel pins was irradiated at average cladding temperatures ranging from 931 to 1015 C. The UN experiments, capsules UN-4 and -5, operated for 10,480 and 10,037 hr, respectively, at an average linear heat generation rate of 10 kW/ft. The UO2 experiment, capsule UN-6, operated for 8333 hr at an average linear heat generation rate of approximately 5 kW/ft. Following irradiation, the nine fuel pins were removed from their capsules, externally examined, and sent to the NASA Plum Brook Facility for more detailed postirradiation examination. During visual examination, it was discovered that the cladding of the fuel pin containing dense UN in each of capsules UN-4 and -5 had failed, exposing the UN fuel to the NaK in which the pins were submerged and permitting the release of fission gas from the failed pins. A rough analysis of the fission gas seen in samples of the gas in the fuel pin region indicated fission gas release-to-birth rates from these fuel pins in the range of .00001.

Thoms, K. R.

Heat pipe nuclear reactor for space power

A heat-pipe-cooled nuclear reactor has been designed to provide 3.2 MWth to an out-of-core thermionic conversion system. The reactor is a fast reactor designed to operate at a nominal heat-pipe temperature of 1675 K. Each reactor fuel element consists of a hexagonal molybdenum block which is bonded along its axis to one end of a molybdenum/lithium-vapor heat pipe. The block is perforated with an array of longitudinal holes which are loaded with UO2 pellets. The heat pipe transfers heat directly to a string of six thermionic converters which are bonded along the other end of the heat pipe. An assembly of 90 such fuel elements forms a hexagonal core. The core is surrounded by a thermal radiation shield, a thin thermal neutron absorber, and a BeO reflector containing boron-loaded control drums.

Koening, D. R.

Integral Experiment Request 523 CED-2 Report

This report documents the final design phase of the Critical Experiment Design (CED-2) conducted as part of integral experiment request (IER) 523. The purpose of IER 523 is to determine critical configurations of 35 weight percent (wt%) enriched uranium dioxide beryllium oxide (UO 2 -BeO) material driven by an annular ring of Seven Percent Critical Experiment (7uPCX) fuel rods at Sandia National Laboratories (Sandia). The experiments will provide benchmark data on water moderated, intermediately enriched UO2 systems as well as Be nuclear data. The experiment will also provide partial validation for the beryllium oxide (BeO) thermal neutron scattering law (TSL) in the thermal energy range. Experiment design concepts, neutronic analysis results, and proposed paths for continuing the CED process are presented. This report builds on the feasibility and justification of experimental need report (CED-0) and preliminary experiment design report (CED-1) completed in December 2021 and September 2023, respectively [1, 2].

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Cluster Dynamics Simulations of Intra-Granular Fission Gas Bubble Size and Pressure Evolution in UO 2

Fission gases such as xenon (Xe) play a critical role in determining the behavior and response of nuclear fuel. Given that Xe has little solubility in UO 2 , it accumulates and forms bubbles, which significantly impact fuel performance. Intra- and inter-granular bubble nucleation and growth can lead to fuel swelling, and once bubbles interconnect at grain boundaries, fission gas can be released into the plenum. At low temperatures, limited uranium vacancy mobility can restrict swelling, therefore causing the bubbles to become highly pressurized. Consequently, this can induce micro-cracking, promote fission gas release (increasing the likelihood of cladding failure), and even lead to fuel pulverization under accident conditions such as a loss of coolant accident. As bubble evolution is strongly influenced by local temperature and fission rate, markedly different behavior occurs across the radial profile of the fuel pellet. Capturing the mechanisms that underpin bubble evolution is therefore important to predict these behaviors in the fuel. Previous models describing important mechanisms informed by lower length scale simulations have been developed under the NEAMS program. These can describe the evolution of a single bubble type (i.e., single value for radius and pressure) at each position in the pellet, for instance using the Centipede cluster dynamic code. However, in reality, a full distribution in bubble sizes and pressures exists within the microstructure at a given position in the pellet. To address this the cluster dynamics code Xolotl, which can predict Xe and vacancy phase space (i.e., bubble distributions) for intra-granular bubbles, has been used before. Prior work benchmarked the Xolotl code against the Centipede cluster dynamics code to ensure compatibility and to verify that mobile defect properties are adequately transferred between the two codes, along with some physics improvements. In this work, we go further by introducing a physics-based set of improvements that will allow us to accurately predict bubble size distributions and internal bubble pressures under representative UO 2 irradiation conditions. The improvements include (i) coupling bubble-defect reaction energies to a virial equation of state (EOS), (ii) including a bubble surface tension contribution, (iii) incorporating radiation-induced re-solution of Xe and vacancies, (iv) enabling pressure-driven dislocation loop punching through an effective emission of interstitial clusters informed by interstitial loop energetics, (v) accounting for radiation induced athermal diffusion of Xe, and (vi) implementing a Booth-type grain boundary sink representation for all mobile defects and defect clusters. After these modifications, we observe good agreement of Xolotl fission gas bubble size and concentration predictions with legacy experimental measurements. Additionally, it allows the distribution of Xe bubble pressures and radius to also be predicted and compared to data produced through the Advanced Fuels Campaign (AFC) program. Here, we have done this by running simulations under conditions similar to the AFC post-irradiation examination (PIE) samples irradiated at North Anna 2 light water reactor (LWR). Our results shows excellent agreement with these experimental measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Microstructural and Oxidation Effects of Nb Additions to U3Si2

U3Si2 is a long term, accident-tolerant nuclear fuel candidate for light-water reactors because of its superior thermal conductivity and increased uranium density when compared to traditional uranium dioxide (UO2). While reducing internal thermal stresses and increasing efficiency, U3Si2 exhibits energetic oxidation during certain off-normal and accident scenarios, which include coolant or steam exposure. To mitigate this, Nb is investigated as an alloy constituent to enhance corrosion resistance and increase mechanical strength. The work presented investigates the response of Nb-alloyed U3Si2 to steam atmospheres. A thermogravimetric analysis is conducted in flowing steam to T > 1000 °C to assess oxidation resistance. The phase characterization of as-melted, thermally annealed and post-oxidation compositions with up to 12 vol% Nb by powder X-ray diffraction, scanning electron microscopy, and energy dispersive spectroscopy is reported.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

The 0E2 benchmarks for PWR UO 2 decay heat: an analysis from the NEA WPNCS

This paper presents the work performed in the subgroup 16 of the Working Party for Nuclear Criticality Safety (WPNCS) of the OECD Nuclear Energy Agency. The main goal was to define two decay heat benchmarks for Spent Nuclear Fuel (one pincell and one assembly), perform calculations and compare and analyze the results in light of existing calorimetric measurements. The selected case is the PWR UO2 assembly 0E2, irradiated at the Ringhals-3 reactor and measured at the Clab facility in Sweden. In total, 21 institutes worldwide participated to the exercise, leading to 55 calculated results (named C). It was found that the measured decay heat values (E) can be satisfactorily reproduced with two-dimensional assembly calculations, leading to an average C/E value of 0.99, with an uncertainty (or one standard deviation) of ±0.01.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Assessment of buffer-IPyC thermomechanical debonding behavior using new experimental strength data in BISON

TRIstructural ISOtropic (TRISO) fuel is a nuclear fuel commonly used in High Temperature Gas-cooled Reactors (HTGRs). A single sub-millimeter-diameter TRISO fuel particle consists of a spherical fuel kernel surrounded by four coating layers: a low-density pyrocarbon buffer layer, an inner pyrolytic carbon (IPyC) layer, a silicon carbide (SiC) layer, and an outer pyrolytic carbon (OPyC) layer. The kernel is commonly made of UO2 or a mixture of uranium carbide and uranium oxide (UCO). During reactor operation, the TRISO coating layers are subjected to irradiation-induced dimensional changes and the associated thermomechanical behavior of each layer. One of the observed behaviors is gap formation between the buffer and IPyC layer due to the porous buffer’s irradiation-induced shrinkage exceeding that of the IPyC layer. Not all irradiated particles will experience buffer-IPyC gap formation. The debonding may be partial, or it may be nearly total. However, from post-irradiation examination of UCO TRISO fuels irradiated as part of the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program, it was concluded that partial buffer-IPyC debonding was the most common type of buffer-IPyC interaction. To predict TRISO thermomechanical performance, multi-physics models have been built that are being continually updated and refined. The BISON code is a finite element-based nuclear fuel performance code that may be used for 1D, 2D, and 3D TRISO particle simulations. This code is used to calculate fuel temperature, kernel swelling, buffer densification, thermal and irradiation creep, fracture, and fission gas production and release. One of the recent additions to the BISON code is the ability to model the process of layer debonding. This paper will focus on the simulation results of the improved BISON debonding model that will utilize updated strengths measured from irradiated AGR TRISO fuel particles. The new experimental strength data from micromechanical tests of irradiated TRISO fuel samples were exercised in the BISON simulations and compared to baseline strength data to assess their applicability in the models. This also includes updated buffer-IPyC bond strengths to simulate layer delamination. Based on current experimental observations it is noted that the buffer-IPyC separation occurs not exactly at the junction of these two layers, but more on the side of the buffer layer. That observation is also implemented in the TRISO interface debonding model. This improved modeling approach using experimental strength data to characterize buffer-IPyC debonding and its potential subsequent cracking will be presented in the paper along with comparisons to available experimental observations.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Evaluating the diffusion of Kr in UO 2 and ADOPT TM using time-of-flight elastic recoil detection analysis (ToF-erda)

A combination of 300 keV 84 Kr ion implantation and Time-of-Flight Elastic Recoil Detection Analysis is utilized to investigate the diffusion of Kr in UO 2 and ADOPT TM fuels. Composition depth-profiles on the nanometer scale were obtained, both for as-implanted samples and after annealing at 800°C for 1 hour. Observed drifts in the 84 Kr profiles could be associated with short-range diffusion mechanisms. The approach employed here provides the possibility to make direct comparisons with atomistic scale modelling data, and can be of service as a separate effect test in line with the Accelerated Fuel Qualification initiative.

ADOPT UO2

Advances in the Development of a WCl6 CVD System for Coating UO2 Powders with Tungsten

Demonstrated viability and utilization of: a) Fluidized powder bed. b) WCl6 CVD process. c) Coated spherical particles with tungsten. The highly corrosive nature of the WCl6 solid reagent limits material of construction. Indications that identifying optimized process variables with require substantial effort and will likely vary with changes in fuel requirements.

Mireles, Omar R.

Development of a TRISO assessment case for BISON based on transient experiments in the NSRR

The tristructural isotropic (TRISO) fuel assessment and validation database currently available in BISON is based mainly on steady-state irradiation and high-temperature furnace testing. Transient assessment cases are needed to support ongoing U.S. industry efforts to design and deploy commercial reactors that utilize TRISO fuels. Most available historical transient tests involving TRISO fuels were characterized by power densities, temperatures, and energy depositions that were highly conservative with respect to typical high-temperature gas-cooled reactor (HTGR) accident conditions. Nonetheless, assessment of BISON's predictive capabilities, adaptation of material properties toward high-temperature and high-particle-power regimes, and development of a systematic approach to validating BISON for TRISO transient applications now motivate the modeling of historical transient tests. This work describes the development of 1-D thermal models of transient experiments conducted at the Nuclear Safety Research Reactor (NSRR) in Japan, with BISON predictions of energy deposition, UO2 melting onset, and molten volume fractions being compared against experimental measurements. Melting is accounted for by defining an effective specific heat capacity for UO2—one that leverages the material's heat of melting. BISON's predictions of energy deposition and molten volume fraction are in good agreement with the experimental data from the low-energy-deposition tests; however, BISON tends to overpredict melting at higher energy depositions. Though overly conservative compared to the operating conditions expected for near-term TRISO-fueled reactor applications, these simulations effectively exercise BISON TRISO models over a wider range of conditions than those encompassed by the existing assessment database. Potential contributors to the observed discrepancies are noted and additional future developments proposed.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS

ASMS 2024 Investigation of Uranyl Perchlorate Anion Complexes in the Gas Phase via Infrared Multiphoton Dissociation and Collision Induced Dissociation

Investigation of Uranyl Perchlorate Anion Complexes in the Gas Phase via Infrared Multiphoton Dissociation and Collision Induced Dissociation Brittany D. M. Hodges, Christopher A. Zarzana, JungSoo Kim, Jonathan Martens, and W. C. M. Berden Introduction (120 words max) Effects of electronic structure on chemical bonding and reactivity play critical roles shaping the chemical bonding and reactivity behaviors of heavy elements. Understanding the role of f electrons in bond formation between the actinide-series elements like uranium with other ligands is critical for solving technical challenges associated with these heavy elements, important to nuclear fuel cycles, efficient separations of rare earth metals, and understanding the chemistry of stored nuclear fuels and related environmental management sites. In this study, we further examine the interactions between uranyl and the perchlorate ion in order to understand the structures of these ions through the use of IRMPD. Here we report the IRMPD spectra of [UO2(ClO4)3]-, [UO3(ClO4)2]-, and a proposed transition state. Methods (120 word max) IRMPD spectra and CID spectra were acquired using a Bruker amaZon QIT/MS instrument at the Free-Electron Lasers for Infrared eXperiments (FELIX) laboratory at Radboud University. The FELIX QIT/MS is modified to allow for the high-intensity tunable IR beam from FELIX to be directed into the ion packet, resulting in multiphoton dissociation that is measured only when the IR frequency is in resonance with an adequately high absorption vibrational mode of the mass-selected complex. DFT geometry optimizations and frequency calculations using the Gaussian suite of programs were performed using B3LYP, TPSSh, and PBE0 level of theory with 6-31+G(d) basis for the O, C, H, and N atoms and the SDD basis set for U. The SDD basis set employs the Stuttgart/Dresden effective core potential. Preliminary Data or Plenary Speakers Abstract (300 words max) Metal ion clusters of uranyl perchlorate were formed via direct electrospray ionization. For each metal ligand complex of interest, the parent ion was isolated and collision induced dissociation fragmentation and Infrared Multiphoton Dissociation (IRMPD) fragmentation spectra were acquired. Results presented here are the first look at the IRMPD spectra of [UO3(ClO4)2]-, [UO2(ClO4)3]-. Structures were examined using Gaussian at different levels of theory B3LYP level of theory, TPPSh and PBE0 levels, to reflect the behaviors of uranium metal ligand complexes most accurately. In these structures, we identified an overlap between each of these uranyl stretches resulting in their largely being obscured by a perchlorate mode. The CID product spectra agree with similar structures reported by Groenewold for uranyl nitrate in 2006 (10.1021/ja058106n).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Imaging and Analysis of Insoluble Electrorefiner Material

Throughout pyroprocessing efforts at the Hot Fuel Examination Facility (HFEF), insoluble material has accumulated in the Electrorefiner (ER) vessel. The objective of this effort was to analyze the accumulated material to determine its origin. Material was removed from the ER salt bath and distilled to remove excess salt prior to performing analysis. Three samples were sent for chemical and isotopic analysis and underwent an ethyl acetate-bromine dissolution to segregate the oxide fraction from the metal fraction. Actinide concentrations were determined using a quadrupole–inductively coupled plasma–mass spectrometer (Q-ICP-MS). Three additional samples were sent for morphologic and elemental analysis by scanning electron microscopy (SEM) with Energy Dispersive X-ray (EDX) analysis at the Irradiated Materials Characterization Laboratory (IMCL). Analyses suggest that the material is primarily composed of UO2. with a small fraction of metal. This study draws no single conclusion as to the origin of the insoluble material in the ER. The particle sizes and morphologies observed in SEM micrographs indicate that the larger particles observed may be a result of introducing material to the ER that has not been completely reduced in Oxide Reduction (OR) operations, which precede electrorefining. Smaller particles may be due to reactions with oxygen and moisture present in HFEF. This research suggests that microscopic analysis of fuel particles before and after OR operations (including after distillation) as well as the uranium product collected on the cathode in the ER would increase understanding about particle morphology within the pyrochemical process.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS