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At least 55 records · Page 3

In-situ ion irradiation induced nanograin growth in a spent UO 2 fuel

This study investigates the irradiation-driven evolution of nanograins in the early-stage restructured rim region of medium burnup spent uranium dioxide (UO 2 ) fuel. Transmission electron microscopy (TEM) lamellas prepared from Belgium Reactor 3 (BR-3) fuel were subjected to in-situ 300 keV Xe ion irradiations under varying doses, fluxes, and temperatures to evaluate their effect on the evolution of the nanograins. Our results reveal that the nanograins grow during ion irradiation. Additionally, the growth is most pronounced at elevated temperatures (300 °C), moderate at room temperature, and negligible at cryogenic temperature (−223 °C). This behavior indicates that thermal activation, alongside irradiation effects, is essential to overcome grain boundary pinning by fission gas bubbles, metallic precipitates, and porosity. Furthermore, while nanograins (<200 nm) consistently coarsened under irradiation, larger grains did not undergo further restructuring, which can be attributed to the strong defect annihilation at TEM lamella surfaces combined with the limited electronic stopping power of low energy Xe ions used in this work. These findings highlight the roles of thermal spike effects, defect mobility, and impurity pinning in governing grain evolution in the rim region of spent UO 2 fuel during ion irradiation, providing key insights for predictive models of restructuring and performance of the high burnup nuclear fuel.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS

UO2 microstructural evolutions induced by Ni, Mo, and W dopants for intentional forensics

The concept of tagging nuclear fuel with a chemical barcode to enable forensics analysis across the nuclear fuel cycle is an area of active investigation, particularly to ensure fabrication viability without disrupting current fuel performance. This study explored the feasibility of using Ni, Mo, and W isotopic double-spikes as dopants in UO2 fuel from the perspective of fuel fabrication. Doped UO2 pellets were produced using conventional fuel fabrication processes, including powder mixing, sieving, pressing, and sintering in a reductive atmosphere. Two composition levels, 100 and 1000 ppm, were evaluated for each dopant element with isotopic double-spike configurations. For the Ni system, additional dopant concentrations of 250 and 500 ppm were produced with nonperturbed isotopic ratios. The results demonstrated that successful incorporation of Ni, Mo, and W double-spikes into UO2 pellets occurred with minimal shift in final density or dopant loss during pellet fabrication. Isotopic analysis confirmed the presence of the double-spike signature even when diluted with natural isotopic material in ratio of 1:5 in the fabrication process. Microstructural examinations revealed different impacts on grain size compared with undoped UO2. This study showed that Ni incorporation up to ∼500 ppm promoted moderate grain growth, whereas the Mo and W systems caused grain size reduction at all concentrations. Changes in the UO2 lattice parameter as a function of composition were detected exclusively for Ni up to 500 ppm, indicating that the Ni solid solution was the main factor for the observed grain growth. Insoluble (Mo and W) or supersaturated (Ni > 500 ppm) conditions produced grain size reduction. The Ni-doped pellets in the solution range resulted in a final microstructure within fuel specifications, demonstrating its potential benefits of employing complex dopant systems for potential nuclear forensic applications.

36 MATERIALS SCIENCE

Methodology for Producing a Uniform Distribution of UO2 in a Tungsten Matrix

Current work at NASA's Marshall Space Flight Center (MSFC) is focused on the development CERMET fuel materials for Nuclear Thermal Propulsion (NTP). The CERMETs consist of uranium dioxide (UO2) fuel particles embedded in a tungsten (W) metal matrix. Initial testing of W-UO2 samples fabricated from fine angular powders performed reasonably well, but suffered from significant fuel loss during repeated thermal cycling due to agglomeration of the UO2 (1). The blended powder mixtures resulted in a non-uniform dispersion of the UO2 particles in the tungsten matrix, which allows rapid vaporization of the interconnected UO2 from the sample edges into the bulk material. Also, the angular powders create areas of stress concentrations due to thermal expansion mismatch, which eventually cracks the tungsten matrix. Evenly coating spherical UO2 particles with chemical vapor deposited (CVD) tungsten prior to consolidation was previously demonstrated to provide improved performance. However, the CVD processing technology is expensive and not currently available. In order to reduce cost and enhance performance, a powder coating process has been developed at MSFC to produce a uniform distribution of the spherical UO2 particles in a tungsten matrix. The method involves utilization of a polyethylene binder during mixing which leads to fine tungsten powders clinging to the larger UO2 spherical particles. This process was developed using HfO2 as a surrogate for UO2. Enough powder was mixed to make 8 discs (2cm diameter x 8mm thickness) using spark plasma sintering. A uniaxial pressure of 50 MPa was used at four different temperatures (2 samples at each temperature). The first two samples were heated to 1400C and 1500C respectively for 5 minutes. Densities for these samples were less than 85% of theoretical, so the time at temperature was increased to 20 minutes for the remaining samples. The highest densities were achieved for the two samples sintered at 1700C (approx. 92% of theoretical). Scanning electron microscopy (SEM) of the mixed powders and the sintered samples along with energy dispersive x-ray analysis was obtained. The SEM of the powders clearly show the fine W powder adhered to the larger HfO2 particles and a uniform distribution of HfO2 particles in a tungsten matrix upon densification. Vicker's Microhardness testing was also performed on all samples using 0.5, 1.0 and 2.0 kg loads. Five indents were made at each load level. All indents were placed in the tungsten matrix to assist as a proxy in measuring densification. The highest hardness value was obtained for the 1700C specimens. The hardness average for these samples was 312.14 MPa. This powder processing method has been applied to W/UO2 powders with the SEM of the powders appearing similar to the W/HfO2 powder images.

Tucker, Dennis S.

Uranium nitride fuel fabrication for SP-100 reactors

Fuel pins of uranium mononitride clad in Nb-1 percent Zr were fabricated for irradiation tests in EBR-II. Laboratory scale process parameters to synthesize UN powders and fabricate UN pellets were developed. Uranium mononitride was prepared by converting UO2 to UN. Fuel pellets were prepared by communition of UN briquettes, uniaxial pressing, and high temperature sintering. Techniques for machining, cleaning, and welding Nb-1 percent Zr cladding components were developed. End caps were electron beam welded to the tubing. Helium back-fill holes were sealed with a laser weld.

Mason, Richard E.

Analytical workflow dependence of experimental observables for uranium chemistries

In this work, we investigated how the sequencing of laboratory analytical methods used for chemical and morphological characterization influences analytical findings for particulate materials relevant to the nuclear fuel cycle, including UO2, U3O8, studtite (UO2O2·4H2O), and β-UO3, in the context of nuclear forensic analysis. Particles of each chemistry obtained from consistent production batches were exposed to Raman spectroscopy and scanning electron microscopy in varying orders to elucidate how the order in which the techniques are applied influences morphological and chemical observations as a function of particle size. The results indicate that particles from all four chemistries exposed to high-resolution electron imaging before Raman spectral analysis demonstrate optical vibrational spectral changes that reduce accurate interpretation of the underlying chemistry via Raman spectral analysis. We hypothesize that these changes are due to the thermal load of the electron beam imparted to the sample being unable to be dissipated by materials with poor thermal conduction properties. Results from this study will aid in determining best practices for forensic analysis procedures to reduce uncertainty in chemical determination of unknown particulate samples.

Manns, Rebecca [University of Nevada, Las Vegas]

UZrCN Synthesis via Arc Melting - A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE

UZrCN Formation via Arc Melting – A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE

Assembly Bowing Reactivity Calculation Methodology Applied to Lead Fast Reactor

Ducted assemblies bow during operation due to power and temperature gradients which can be influenced by operating flow rates. For fast spectrum cores using ducted assemblies, the bowing behavior follows that of the duct and because there are gaps between the ducts, the bowing can result in compaction or expansion of the active core. This local displacement can have a positive or negative impact and knowing the net effect during transients is important for system reactivity control. Keeping the net bowing reactivity worth low is possible with attentive placement of load pads above the active core and selecting load pad gap thicknesses that result in a desired behavior at standard operating conditions. This paper considers a Lead Fast Reactor (LFR) concept fueled by HALEU UO2 developed by Westinghouse Electric Company (WEC) and applies a workflow of Argonne-developed codes to estimate the core bowing reactivity worth. Using orifice flow rates grouped by assembly type, the net reactivity impact due to core assembly bowing for the LFR was found to be small and in line with other liquid metal fast reactors: +29/+32/+35 pcm, or about +$0.049/+$0.055/+$0.059, for BOEC/MOEC/EOEC, respectively.

bowing reactivity

Identifying microstructures susceptible to pulverization in commercially irradiated high burnup UO2 under LOCA conditions

High burnup fuel fragmentation (HBFF) has been a concern in the nuclear industry for many years. When UO2 reaches and exceeds pellet average burnups around 55 GWd/tU, microstructural changes in the fuel pellet begin to occur that render the pellet susceptible to fine fragmentation under loss-of-coolant accident (LOCA) conditions. During a LOCA event, the cladding balloons and bursts, potentially releasing part of these fine fuel fragments into the reactor pressure vessel. This process is known as fuel fragmentation, relocation, and dispersal (FFRD). Presently, the US nuclear industry is developing a safety basis for FFRD with the goal of increasing burnups and pressurized water reactor cycle lengths. Increased cycle lengths would push the burnup limits of the fuel rods past the known threshold for HBFF susceptibility. In this work, the microstructural impact on HBFF was investigated by comparing the microstructures of as-irradiated rod segments to their post-LOCA tested counterparts. This investigation found that varied operational histories result in different microstructural evolutions across the pellet radius, which impacts the fragmentation behavior and radial location of the fragmentation. It is noted that regions with a high bubble density and a high density of grain boundaries fragment under LOCA-relevant conditions. In addition to the fragmentation that has been previously reported at the periphery of the fuel, fragmentation was also noted in the dark zone toward the fuel center. Analysis of the power histories of the fuel samples suggests that the dark zone forms in the central regions of the pellet between temperatures of approximately 740 and 960 °C.

McKinney, Casey [ORNL] (ORCID:0000000335383614)

Statistical fracture behavior of doped UO 2 using a ball-on-ring equibiaxial flexure test method

Metal oxide dopants, such as titanium and chromium oxides, have garnered considerable attention for their potential to increase grain size (≥ 30 µm) in UO 2 fuel, purportedly enhancing fission gas retention during reactor operation. Fuel performance is significantly impacted by fuel fracture behavior, so it is important to understand the effects of enhanced grain size and dopant content on UO 2 fuel fracture. UO 2 pellets were doped with 0.1 wt% TiO 2 and 0.3 wt% Cr 2 O 3 to alter density and grain size. Inductively coupled plasma mass spectroscopy measured dopant levels pre- and post-sintering. X-ray diffraction revealed lattice changes and microstrain via Rietveld refinement. Field emission scanning electron microscopy determined grain sizes of approximately 30 µm for TiO 2 doping and 7 µm for Cr 2 O 3 doping. Transverse rupture strength tests were performed on over 30 samples per dataset to obtain characteristic strength and Weibull modulus. Results indicate no statistical difference in fracture strength between 0.1 wt% TiO 2 doped UO 2 and undoped UO 2 , while 0.3 wt% Cr 2 O 3 doped UO 2 exhibited a 20% decrease in fracture strength. Doped UO 2 samples also showed reduced Weibull modulus compared to undoped UO 2 , suggesting increased scatter in fracture strength. This study's findings suggest that titanium and chromium oxide doping in UO 2 , regardless of grain size, induce residual stresses, decreasing fracture strength and increasing variability in fracture behavior.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Nuclear Thermal Rocket Simulation in NPSS

Four nuclear thermal rocket (NTR) models have been created in the Numerical Propulsion System Simulation (NPSS) framework. The models are divided into two categories. One set is based upon the ZrC-graphite composite fuel element and tie tube-style reactor developed during the Nuclear Engine for Rocket Vehicle Application (NERVA) project in the late 1960s and early 1970s. The other reactor set is based upon a W-UO2 ceramic- metallic (CERMET) fuel element. Within each category, a small and a large thrust engine are modeled. The small engine models utilize RL-10 turbomachinery performance maps and have a thrust of approximately 33.4 kN (7,500 lbf ). The large engine models utilize scaled RL-60 turbomachinery performance maps and have a thrust of approximately 111.2 kN (25,000 lbf ). Power deposition profiles for each reactor were obtained from a detailed Monte Carlo N-Particle (MCNP5) model of the reactor cores. Performance factors such as thermodynamic state points, thrust, specific impulse, reactor power level, and maximum fuel temperature are analyzed for each engine design.

Belair, Michael L.

Nuclear Thermal Rocket Simulation in NPSS

Four nuclear thermal rocket (NTR) models have been created in the Numerical Propulsion System Simulation (NPSS) framework. The models are divided into two categories. One set is based upon the ZrC-graphite composite fuel element and tie tube-style reactor developed during the Nuclear Engine for Rocket Vehicle Application (NERVA) project in the late 1960s and early 1970s. The other reactor set is based upon a W-UO2 ceramic-metallic (CERMET) fuel element. Within each category, a small and a large thrust engine are modeled. The small engine models utilize RL-10 turbomachinery performance maps and have a thrust of approximately 33.4 kN (7,500 lbf ). The large engine models utilize scaled RL-60 turbomachinery performance maps and have a thrust of approximately 111.2 kN (25,000 lbf ). Power deposition profiles for each reactor were obtained from a detailed Monte Carlo N-Particle (MCNP5) model of the reactor cores. Performance factors such as thermodynamic state points, thrust, specific impulse, reactor power level, and maximum fuel temperature are analyzed for each engine design.

Belair, Michael L.

Results of a preliminary experimental investigation of a vapor transport fuel pin

In-Pile experimental tests were conducted on two fuel pins mounted side-by-side in a holder assembly. The fuel pins consisted of stacked fully enriched UO2 pellets enclosed in a type 316 stainless steel clad 1/2 inch outside diameter and 3 inches in length. Each fuel pin contained four pellets for a total of 22 grams of fuel weight. The experiment was operated to maintain the maximum clad temperature at 395 K corresponding to a fuel temperature at the central void surface of 2350 K. Total primary coolant water flow past the pin holder was calculated to be 110 gallons per minute. Forty-four gallons per minute at a velocity of 36.5 feet per second flowed around each fuel pin. Calculations indicated the maximum heat flux was at the point of the highest temperature and was equal to 0.24 kW/sq cm or 7.62 Btu/hr sq ft. A series of high resolution neutron radiographs of the nuclear fueled vapor transport capsule was taken. The thermal neutrons emitted from the core of the 60 megawatt Plum Brook reactor facility were used.

Lanzo, C. D.

An Instrumented Capsule Design to Measure Thermal Conductivity in Miniature UO2 Specimens

Numerous separate effects irradiations of miniature nuclear fuel specimens have been conducted in the High Flux Isotope Reactor (HFIR) under the experimental platform designated as MiniFuel. MiniFuel is a static irradiation capability in which microstructural evolution and fuel performance phenomena are observed during postirradiation examination thereby offering a snapshot of the terminal fuel characteristics. This approach inherently requires fielding an irradiation where the experimental conditions are determined using predictive models and the pertinent outcomes are measured at the end of the test. Static irradiations can provide useful insights to the relationships between fuel performance and the pivotal irradiation conditions, namely temperature and burnup, but the ability to monitor fuel performance in situ would further support fuel development and qualification. To this end, an instrumented experiment design is being developed at Oak Ridge National Laboratory to capture thermal conductivity degradation and fission gas release during HFIR irradiation. These phenomena will be monitored using unique capsule designs that each target a different phenomenon. This paper details the thermal conductivity capsule (TCC) design and its expected performance envelope as determined using computer models. Each TCC will contain a miniature UO2 disc specimen (~0.5 mm thick × 5 mm diameter) sandwiched between metallic slugs with embedded thermocouples. The coupling of in situ temperature measurements, known thermal conductivity of the metallic components, and heat generation rates computed using high-fidelity neutronics models make the thermal conductivity measurement possible. This paper describes the reactor physics and heat transfer models used to predict the capsule’s performance and the methodology for calculating the fuel specimen’s thermal conductivity from the thermocouple measurements.

Gorton, Jacob [ORNL] (ORCID:0000000269806083)

High Power MPD Nuclear Electric Propulsion (NEP) for Artificial Gravity HOPE Missions to Callisto

This documents the results of a one-year multi-center NASA study on the prospect of sending humans to Jupiter's moon, Callisto, using an all Nuclear Electric Propulsion (NEP) space transportation system architecture with magnetoplasmadynamic (MPD) thrusters. The fission reactor system utilizes high temperature uranium dioxide (UO2) in tungsten (W) metal matrix cermet fuel and electricity is generated using advanced dynamic Brayton power conversion technology. The mission timeframe assumes on-going human Moon and Mars missions and existing space infrastructure to support launch of cargo and crewed spacecraft to Jupiter in 2041 and 2045, respectively.

McGuire, Melissa L.

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

This paper reviews test data for cermet fuel samples developed in the 1960's to better quantify Nuclear Thermal Propulsion (NTP) cermet engine performance, and to better understand contemporary fuel testing results. Over 200 cermet (W-UO2) samples were tested by thermally cycling to 2500 deg (2770 K) in hydrogen. The data indicates two issues at high temperatures: the vaporization rate of UO2 and the chemical stability of UO2. The data show that cladding and chemical stabilizers each result in large, order of magnitude improvements in high temperature performance, while other approaches yield smaller, incremental improvements. Data is very limited above 2770 K, and this complicates predictions of engine performance at high Isp. The paper considers how this material performance data translates into engine performance. In particular, the location of maximum temperature within the fuel element and the effect of heat deposition rate are examined.

Ceramic Nuclear Fuel

Speciation mapping of the oxidation layer on aged uranium dioxide using scanning transmission x-ray spectromicroscopy

In this study, UO 2 was aged in humid air and prepared as a thin section using a focused ion beam (FIB) instrument. The specimen was measured using synchrotron radiation spectromicroscopy techniques at the Beamline 11.0.2 STXM end station of the Advanced Light Source (ALS). Non-negative matrix factorization (NMF) methods were used to identify and map three component x-ray absorption near-edge structure (XANES) spectra in the oxygen K-edge data, revealing a surface layer of U 4 O 9 with a thickness of 206 ± 21 nm, and the bulk of the sample remaining as UO 2 . Uranium N 4,5 -edge XANES spectromicroscopy supports these results. The diffusion-controlled parabolic rate constant for UO 2 oxidation to U 4 O 9 was calculated from the observed layer thickness and compared to literature values. Complementary transmission electron microscopy (TEM) was used to image the sample and identify the phases present in various regions, confirming the STXM results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS