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Contributions to the mechanistic understanding of the microstructural evolution in irradiated U-Mo dispersion fuel

Here, advanced microstructural characterization techniques, such as scanning electron microscopy (SEM) and scanning transmission electron microscopy - energy dispersive x-ray spectroscopy (STEM-EDS), were used to interpret the fuel microstructure evolution and fission products behavior in U-Mo dispersion fuel irradiated in the Advanced Test Reactor (ATR) as part of the European Mini-Plate Irradiation Experiment (EMPIrE) test. The larger as-fabricated fuel grain size achieved by heat-treating the U-Mo powder resulted in slower high burnup structure (HBS) development and reduced fission gas porosity. Slower HBS kinetics was observed at the fuel kernels’ periphery, which contained smaller and less fission gas bubbles at all fission densities (FDs) investigated and was attributed to a locally reduced damage density and fission products concentration, as corroborated with Monte Carlo simulations. The non-refined grains at the fuel kernel periphery hosted a perfectly ordered fission Gas Bubble Superlattice (GBS) up to 6.3 × 10 21 fissions/cm 3 . Nano-scale STEM-EDS analysis presented in this study provided useful information on the GBS characteristic morphology and evolution in U-Mo fuel. The concentration of fission gas in the GBS progressively increased with FD, pointing to an evolution of the nanobubble pressure status with irradiation. A possible connection between the GBS collapse and HBS onset is proposed for which there exists a threshold in the misorientation of the refined sub-grains above which the GBS stability during irradiation is no longer preserved, resulting in the GBS collapse.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The use of U3Si2/Al dispersion fuel for high power research reactors

In order to investigate the irradiation performance of U3Si2/Al dispersion fuel at relatively aggressive reactor conditions, compared to how this fuel is typically used in a research or test reactor, post irradiation examination was performed on two fuel plates that were irradiated at ~270 W/cm2 average surface heat flux and to a maximum local burnup greater than 8 × 1021 fissions/cm3 in the Advanced Test Reactor as part of the RERTR-8 experiment. As part of the non-destructive examinations that were performed on both fuel plates, detailed thickness measurements using a high-fidelity measurement bench were performed on one fuel plate and a segment of the second fuel plate. This paper provides the first reported results of such high-resolution thickness measurements for U3Si2/Al dispersion fuel plates, containing primarily the U3Si2 fuel phase, irradiated at such power levels to high burnup. For destructive examination using optical metallography, samples were generated from both irradiated plates. Localized regions of high swelling (characteristic of internal blistering) were observed on the surface of both fuel plates, suggesting that the performance limits had been reached for each plate. Destructive examinations showed that the fuel particles that are primarily U3Si2, which become amorphous during irradiation, in both plates contained relatively large fission gas bubbles with evidence of fission gas bubble interconnection.

Wachs, Daniel M.↗

Implications of point defect accumulation on UO 2 thermal conductivity and fission gas release under accelerated fuel irradiation

Evaluation of thermal properties is a crucial factor for nuclear fuel performance. During reactor operation, the accumulation of fission products and irradiation-induced lattice defects are responsible for degradation in thermal conductivity. Consequently, it affects fuel temperature and fission gas release (FGR) among other Multiphysics processes important for economics and safety analysis. We analyze the implications of point defects (PD) accumulation described using a rate theory (RT) Model on lattice thermal conductivity of UO 2 . Here, we demonstrate that fission rate-dependent point defect concentrations have the largest impact on in-pile thermal conductivity in the periphery of light water reactor fuels below a temperature threshold governed by the migration barrier of defects. Our analysis provides a mechanistic description of this phenomena which current fuel performance codes treat empirically. The reduction of thermal conductivity in the low -temperature rim region acts as additional thermal resistance and leads to a temperature notably larger than suggested by Lucuta thermal conductivity correlation. These effects are anticipated to have notable impacts when fuels are exposed to accelerated radiation. The impact of such point defect-informed treatment of thermal conductivity on fuel performance is evaluated by a detailed analysis of fission gas behavior and its release. We consider several models capturing different stages of fission gas bubble evolution and fission gas release (FGR). Finally, a new fission rate-dependent correction to the Lucuta correlation is proposed. The results show a significant reduction in thermal conductivity at the fuels’ periphery and an increase in fuel centerline temperature specifically at low burnups. Ultimately a modified LC shows a higher FGR compared to the original LC, while the acceleration process results in a reduction in overall FGR.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of ZrN coating and heat treatment on U-Mo dispersion fuel systems under irradiation

The stability of U-Mo fuel particles embedded in an Al matrix under irradiation can be enhanced through ZrN coatings and/or heat treatment. Here, the present study investigates the irradiation behavior of fuel plates containing U-Mo fuel particles fabricated under various heat-treatment conditions and ZrN coating thicknesses. Different fission densities were also applied to each fuel plate to evaluate the effects of these variables. Results indicate that higher fission densities lead to more grain recrystallization and high burnup structure (HBS) development in the fuel particles. Heat treatment was found to mitigate the accumulation of fission gas bubbles in fuel particles at low fission densities by coarsening their grains. Fuel particles with ZrN coatings of a 1.2 μm thickness or above exhibited reduced formation of U-Mo/Al interaction layers, suggesting the existence of a critical ZrN coating thickness that minimizes the development of these layers. Fission gas bubbles were predominantly observed at grain boundaries of U-Mo fuel particles irradiated at low fission densities. Subgrain boundaries, which appeared to originate from the original grain boundaries containing fission gas bubbles or HBSs, were also observed, indicating the early stage of HBS propagation in the fuel particles.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

In-situ ion irradiation of fission products in a spent UO 2 fuel

This study investigates the behavior of fission gas bubbles and five metal precipitates (5MPs) (Mo, Ru, Rh, Tc, Pd) in spent uranium dioxide (UO 2 ) fuel under various ion irradiation doses, temperatures, and flux conditions. Utilizing in-situ ion irradiation and advanced transmission electron microscopy, we analyzed the evolution of fission gas bubbles and 5MPs in UO 2 samples from the Belgium Reactor 3 (BR-3). Our findings reveal significant shrinkage of fission gas bubbles and 5MPs with increasing irradiation dose, accompanied by a decrease in pair density. We demonstrate that ion irradiation induces a homogeneous re-solution process where individual atoms are ejected from bubbles and precipitates, leading to their dissolution and subsequent re-precipitation in the matrix. In conclusion, this study provides critical insights into the dynamic behavior of fission products under irradiation, facilitating the development of predictive models and contributing to the optimization of nuclear fuel performance and safety.

Fission products↗

In-situ ion irradiation of a spent UO2 fuel: evolution of fission products and nanograins with radiation dose

This study investigates the behavior of fission gas bubbles, five metal precipitates (5MPs) (Mo, Ru, Rh, Tc, Pd) and nanograins in spent uranium dioxide (UO2) fuel under various ion irradiation doses, temperatures, and flux conditions. Utilizing in-situ ion irradiation and advanced transmission electron microscopy, we analyzed the evolution of fission gas bubbles, 5MPs and nanograins in UO2 samples from the Belgium Reactor 3 (BR-3). Our findings reveal significant shrinkage of fission gas bubbles and 5MPs with increasing irradiation dose, accompanied by a decrease in pair density. The study also reveals nanograin coarsening under irradiation. We demonstrate that ion irradiation induces a homogeneous re-solution process where individual atoms are ejected from bubbles and precipitates, leading to their dissolution and subsequent re-precipitation in the matrix. This study provides critical insights into the dynamic behavior of fission products and nanograins under irradiation, facilitating the development of predictive models and contributing to the optimization of nuclear fuel performance and safety.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of ZrN Coating and Heat Treatment on U-Mo Dispersion Fuel under Irradiation

The stability of U-Mo fuel particles in Al matrix can be improved using ZrN coating and heat treatment. This study investigated irradiation behaviors of fuel plates containing U-Mo fuel particles fabricated with different conditions including heat treatment and the thickness of ZrN coating. Additionally, different fission densities were applied to each fuel plate to understand how varying fission densities affect its irradiation behaviors. This study showed that more recrystallization of grains and development of high burnup structure (HBS) occurred in irradiated fuel particles with higher fission densities. Heat treatment reduced the accumulation of fission gas bubbles in the fuel particles by coarsening their grains. The fuel particles with a ZrN coating thickness of 1.2-1.8 µm showed less significant development of U-Mo/Al interaction layers than the particles with a coating thickness of 0.5 µm after irradiation. This might indicate the existence of a critical thickness of ZrN coating to minimize the formation of the interaction layers. Fission gas bubbles were observed at grain boundaries of irradiated U-Mo fuel particles at low fission densities, and the formation of dendritic features with a darker contrast was identified in backscattered electron images. These features stemmed from grain boundaries with fission gas bubbles or HBS, and some of them contained the bubbles, indicating that they might represent an early stage of HBS propagation in the fuel particles.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluation of the Effect of Burnup Acceleration on UO 2 Microstructure Evolution

Accelerated fuel qualification (AFQ) is a methodology by which new nuclear fuels are developed in an accelerated time frame compared with historical fuel qualification approaches. AFQ generally relies on high-fidelity physics-based modeling and simulation tools to adequately describe fuel performance as well as on revolutionary methods to accelerate burnup accumulation and collect relevant data more quickly. This report summarizes the use of advanced fuel modeling and simulation tools to evaluate microstructures from commercially irradiated fuel and microstructures from proposed MiniFuel irradiations, in which burnup accumulation is accelerated while prototypic temperature conditions are maintained. In this milestone, we used the mesoscale fuel performance code MARMOT to model the evolution of irradiated UO 2 microstructures and their potential restructuring at high burnup. The simulation conditions were informed by BISON models of both commercially irradiated fuel and MiniFuel. A first set of simulations investigated the recrystallization behavior of fully dense microstructures and showed full recrystallization at burnups as low as 52 MWd/kgU at 950°C. However, these simulations did not account for the presence of fission gas bubbles (predicted by BISON). Therefore, a second set of simulations including fission gas bubbles was performed and indicated that at the lowest temperature considered (650°C), the porous UO 2 microstructures have the highest total Gibbs free energies and are likely to recrystallize earlier than higher temperature cases (800 and 950°C), which agrees with high-burnup fuel characterization data. The results also showed that at lower temperature (650°C), the total free energies of the PWR fuel and MiniFuel microstructures are not significantly different. However, at the highest temperature (950°C), MiniFuel microstructures have a lower free energy than that of the PWR fuel microstructure. The competing effects between the temperature-dependent grain nucleation rate and the reduction of the free energy of the microstructure at higher temperature as a result of diffusion indicated that restructuring may occur at even higher temperatures than those considered in this study. In addition to the microstructure evolution modeling efforts, the burnup gradient across a single fuel specimen was also considered. This evaluation was for the VXF-15 position of the High Flux Isotope Reactor (HFIR) using the code suite HFIRCON, which was developed to automate the workflow for evaluating targets and fuel as they are irradiated in HFIR. The burnup gradient evaluation showed a dependence on both the axial and radial locations within the specimen, with a maximum difference of 1.7 between the inner and outermost radial layers. This relationship was further supported by considering the fission product speciation with respect to location within the specimen, which showed a higher concentration of 239 Pu, 240 Pu, and 241 Pu on the outer radial locations of the specimen than the center. The findings of the burnup and speciation evaluation show that some amount of self-shielding is occurring in the specimen when irradiated in the high-flux environment of HFIR; however, this impact is more pronounced for natural uranium when compared to 6% enrichment due to the higher ratio of 238 U in the specimen. Further analyses are required to understand the sensitivity of this gradient to spatial mesh and enrichment of the specimen.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Multiscale Microscopy Characterization of High Burnup LWR UO 2 Before and After LOCA Testing

Previous microscopy work within the campaign has observed increased porosity coupled with subgrain formation in the mid-radial region of the fuel. However, examinations of high burnup fuel taken from multiple reactors with different operating conditions have shown that this structure can move radially inward depending on the fuel operating conditions. It is currently theorized that inter- and intragranular fission gas bubble nucleation is precursory to the grain subdivision observed in the mid-radial and central regions of the fuel. Characterization of samples after loss-of-coolant accident (LOCA) testing has revealed that these restructured regions with a high density of bubbles and subgrains pulverize during the transient test. It appears that the increase in fission gas bubbles coupled with grain subdivision renders the fuel mechanically weaker during a LOCA transient and thus susceptible to fuel fragmentation relocation and dispersal (FFRD). Work this past fiscal year has prioritized understanding this behavior by using advanced microscopy to investigate fission gas behavior in the as-irradiated and post-LOCA state. Additional work has been performed to verify the theory described above by analyzing multiple post-LOCA optical micrographs and comparing that to as-irradiated microstructural data. This document reports progress in the post-irradiation characterization of high burnup nuclear fuel with emphasis on the restructured fuel regions, particularly how microstructural features influence FFRD and fission gas release behavior in LOCA conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multi-scale simulation of high burnup UO2 nuclear fuel during loss-of-coolant accident conditions

To improve the economics of commercial nuclear energy generation, U.S. utilities are currently seeking licensing approval to operate UO2 fuel to higher burnups. One significant safety issue that must be addressed to obtain approval is the potential for fine fragmentation/pulverization of the fuel during a loss-of-coolant accident (LOCA). It has been hypothesized that pulverization is caused by the rapid increase of pressure in fission gas bubbles in the high burnup region of the fuel during a LOCA. To better understand this phenomenon, a novel phase-field model of the fission gas bubble microstructure in UO2 has been developed and implemented in Idaho National Laboratory (INL)'s Marmot application for phase-field simulation of nuclear materials. Simulations of the bubble response to steady-state and transient conditions were conducted, and the results were used to inform a mechanistic model of pulverization in BISON, INL’s fuel performance simulation code.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multiscale modeling for high burnup structure formation and associated pulverization

This report summarizes the lower length scale modeling work performed in the fiscal year 2023 under the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program to capture the microstrutural evolution and associated pulverization criteria in the high burnup regions. This year, the resolution mechanisms within the cluster dynamics code has been updated and it influence on the bubble growth in HBS regions at the mesoscale is studied. To improve the accuracy of phase-field models of fission gas bubble growth, a new Helmholtz free energy for high-density Xe gas is derived from a virial equation of state. Two previously used strategies for representing net vacancy production in phase-field models of fission gas bubble growth are compared with each other and with analytical models of bubble growth. The vacancy source only model is found to be more convenient to parameterize realistically compared with the vacancy source+sink model. Furthermore, the phase-field-fracture simulation have been performed using MD- informed failure stress values and realistic HBS structure obtained from the phase-field simulations. We also present the uncertainty bands on prediction of the critical stress to account for the effect of the lower length scale variabilities on the failure criteria at the mesoscale. It is observed that pulverization may occur in partially restructured regions with restructuring fraction as low as 17%. In light of this, an update to the BISON’s pulverization criteria is recommended.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mesoscale Modeling for Restructuring and Fragmentation in High Burnup UO 2

This report summarizes the mesoscale modeling conducted in fiscal year 2025 under the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program, focusing on the microstructural evolution and restructuring in high burnup UO 2 nuclear fuel and its impact on fuel fragmentation. We developed a pioneering phase-field model to simulate restructuring behavior across different regions of high burnup fuel, including the dark zone and rim region. A grand-potential-based phase-field model is employed to concurrently evaluate subgrain formation and the growth of fission gas bubbles within the fuel. An energy-based subgrain formation criterion was introduced to simulate the restructuring process. The effects of temperature and burnup rate were studied to capture how each of these parameters influences the characteristics of the restructured fuel. Subgrain formation was observed to initiate around existing fission gas bubbles and proceed toward triple junctions, grain boundaries, and grain interiors. Under a given subgrain formation rate, the rate of restructuring increases with rising fuel temperature. The restructuring occurs faster with higher burnup rate. A restructuring bias was observed within the microstructure, due to the variation in defect accumulation when comparing different grains. Microstructures corresponding to the dark zone and rim region can be obtained by parameterizing the model with the appropriate defect production rate, as determined based on the burnup rate and temperature. The predicted microstructures are consistent with experimental observations of the restructured regions. Based on the mesoscale simulations, a mechanistic model for restructuring and grain size evolution was implemented in BISON. Thus, this work provides a first-of-its-kind restructuring model for different regions of high-burnup fuel to BISON. It was shown that the model predicts appropriate grain size evolution along fuel radius as those observed in experiments. This model enables BISON to predict the effect of restructuring on the fission gas release. Finally, the phase-field fracture simulation with dark zone specific microstructures were presented to provide the fragmentation criteria for the dark zone. This work introduces a first-of-its-kind restructuring model for high burnup fuel, significantly enhancing BISON's predictive capabilities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mesoscale modeling of restructuring in high burnup UO 2 fuel

Here, this work aims to simulate the restructuring behavior observed in different regions of high burnup fuel, providing a first-of-its-kind restructuring model for the dark zone and rim region of high-burnup UO 2 fuel. We employed a grand-potential-based phase-field model to concurrently evaluate subgrain formation and the growth of fission gas bubbles within the fuel. An energy-based subgrain formation criterion was introduced to simulate the restructuring process. The effects of different initial conditions and different modeling parameters were systematically studied to capture how each of these parameters influences the characteristics of the restructured fuel. Subgrain formation was observed to begin around existing fission gas bubbles and proceed toward triple junctions, grain boundaries, and grain interiors. Restructuring was demonstrated to be influenced by a combination of initial dislocation densities, burnup rate, subgrain formation rate, and temperature. Under a given subgrain formation rate, the rate of restructuring increases with rising fuel temperature. A restructuring bias was observed within the microstructure, due to the variation in defect accumulation when comparing different grains. Microstructures corresponding to the dark zone and rim region can be obtained by parameterizing the model with the appropriate defect production rate, as determined based on the burnup rate and temperature. Furthermore, bubble size and distribution do not significantly affect the rate of restructuring. The predicted microstructures are consistent with experimental observations of the restructured regions. Finally, we present a correlation demonstrating the evolution of the restructuring volume fraction as a function of local burnup.

UO2↗

Computational determination of a primary diffusion mode in γ U-10Mo under irradiation

Low enriched uranium (< 20 % 235 U)-molybdenum (U-Mo) monolithic fuel is the primary candidate for high performance research and test reactors, and is in the process of being qualified to replace highly enriched uranium (≥ 20 % 23 5U) fuel. As part of the qualification process, it is critical to understand and predict the behavior of fission gas bubbles under irradiation, which affects fuel swelling and fuel failure. Mechanistic fuel models are being developed that can both reproduce the existing experimental data for fuel swelling, and be further applied to irradiation conditions beyond the experimental scope. Diffusion of species under irradiation conditions is an important parameter in the mechanistic fuel models; however, no temperature-relevant experimental diffusion data exists. In the present work, radiation-enhanced diffusion coefficients of U, Mo, and Xe in λU-10wt.%Mo were calculated in the temperature range between 300 K and 1400 K via rate-theory models and molecular dynamics simulations with an embedded-atom method interatomic potential for the U-Mo-Xe system. Accordingly, total diffusion coefficients under relevant irradiation conditions are determined using previously obtained intrinsic thermal diffusion and radiation-driven diffusion coefficients, as well as the newly calculated radiation-enhanced diffusion coefficients presented herein. Radiation-enhanced diffusion of U and Mo was dominant in the intermediate temperature range, whereas radiation-enhanced diffusion of Xe did not significantly contribute to total diffusion of Xe at the relevant fission rate densities. Radiation-enhanced diffusion of Xe became faster than both intrinsic thermal diffusion and radiation-driven diffusion at a fission rate density of 5 x 10 22 fissions/m 3 /s, which is higher than the typical fission rate density range in research reactors. The temperature regime that radiation-enhanced diffusion of each element dominated was dependent on the fission rate density. Finally, the total diffusion coefficients of U, Mo, and Xe, updated in this work, will be utilized as parameters in the mechanistic fuel models to help predict the behavior of fission gas bubbles under irradiation more accurately.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Microstructural and Micro-Chemical Evolutions in the Irradiated UCO Fuel Kernels of AGR-1 and AGR-2 TRISO Fuel Particles

AGR-1 and AGR-2 TRISO fuel particles were fabricated with slightly different fuel kernel chemical compositions, modified fabrication processes, different fuel kernel diameters, and changed 235U enrichments. To correlate those differences with the fuel kernel responses to neutron irradiations in terms of irradiated fuel microstructure, fission products chemical and physical states, and fission gas bubble evolutions, extensive microstructural and analytical characterizations were conducted. The studies used a state of art transmission electron microscopy (TEM) equipped with Energy-dispersive X-ray spectroscopy (EDS) of four silicon solid-state detectors which have super sensitivity and fast speed. The TEM specimens were prepared from selected AGR-1 and AGR-2 irradiated fuel kernels exposed to safety testing after irradiation. The particles were chosen to represent a representative irradiation conditions with a fuel burnup within the range from 10.8 to 18.6% FIMA, and the time-average volume-average temperatures vary from 1070 to 1287°C. The 235U enrichment was 19.74 wt.% for the AGR1 fuel kernels and 14.03 wt.% for the AGR-2 fuel kernels. The TEM results show that there were significant microstructural reconstructions in the irradiated fuel kernels for both the AGR-1 and AGR-2 fuels. There are four major phases including fuel matrix of UO2 and UC, U2RuC2, and UMoC2 in the irradiated AGR2 fuel kernel. Zr and Nb form solid solution in the UC phase. UMoC2 phase often shows a detectable concentration of Tc. Pd was found to mainly locate in the buffer layer or to be associated with fission gas bubble within the UMoC2 phase. The EDS maps qualitatively show that the rare-earth fission products (Nb, et al.) preferentially reside in the UO2 phase. In contrast, in the irradiated AGR1 fuel kernel, no U2RuC2 or UMoC2 precipitates were positively identified. Instead, there is a high number of rod-shape precipitates enriched with Ru, Tc, Rh, and Pd observed in the fuel kernel center and edge zone. The difference of microstructural and micro-chemical evolutions in irradiated fuel kernels between the AGR-1 and AGR-2 TRISO fuel particle may result from a combined factor of irradiation temperature, fuel geometry and chemical composition. However, the irradiation temperature probably play a more deterministic role. Limited electron energy loss spectroscopy (EELS) characterizations on the AGR2 fuel kernel show that there is nearly no carbon in the UO2 phase while a small fraction of oxygen was detected in the UC/UMoC2 phase.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mesoscale Modeling of the Effects of Accelerated Burnup on UO2 Microstructural Evolution

Accelerating the nuclear fuel qualification process will rely on some combination of advanced modeling and simulation techniques with accelerated irradiation testing and separate effects experiments to enable the development of new fuel concepts in a shorter time frame. One of the key challenges to successfully leveraging accelerated irradiation tests will be understanding the artifacts that may be introduced with accelerated accumulation of dose and/or burnup. This work presents phase field (MARMOT) simulations of the evolution of representative 2D UO2 microstructures up to 40 MWd/kgU. Simulations were performed under both commercial light water reactor fuel conditions as well as those that would be expected for highly accelerated (~10x) burnup conditions similar to those used in the MiniFuel irradiations in Oak Ridge National Laboratory’s High Flux Isotope Reactor. The phase field model was coupled with a discrete nucleation algorithm to model re- structuring at high burnup. The effect of the different fission rates in both microstructures was investigated at two temperatures: 650?C and 800?C. The lower temperature simulations both showed an onset of restructuring at nearly 60 MWd/kgU. More extensive restructuring was obtained in the MiniFuel microstructure compared with that of the PWR fuel. At 800?C, no restructuring was obtained as a result of the thermally activated diffusion of Xe atoms and U vacancies to fission gas bubbles, which reduces the nucleation driving force. These results highlight the importance of using modeling and simulation tools to inform the environmental conditions during targeted accelerated irradiation tests to extract the most useful fuel performance data.

accelerated fuel qualification, Phase Field, Restr↗

Microstructural Changes and Chemical Analysis of Fission Products in Irradiated Uranium-7 wt.% Molybdenum Metallic Fuel Using Atom Probe Tomography

Understanding the microstructural and phase changes occurring during irradiation and their impact on metallic fuel behavior is integral to research and development of nuclear fuel programs. This paper reports systematic analysis of as-fabricated and irradiated low-enriched U-Mo (uranium-molybdenum metal alloy) fuel using atom probe tomography (APT). This study is carried out on U-7 wt.% Mo fuel particles coated with a ZrN layer contained within an Al matrix during irradiation. The dispersion fuel plates from which the fuel samples were extracted are irradiated at Belgian Nuclear Research Centre (SCK CEN) with burn-up of 52% and 66% in the framework of the SELENIUM (Surface Engineering of Low ENrIched Uranium-Molybdenum) project. The APT studies on U-Mo particles from as-fabricated fuel plates enriched to 19.8% revealed predominantly γ-phase U-Mo, along with a network of the cell boundary decorated with α-U, γ’-U2Mo, and UC precipitates along the grain boundaries. The corresponding APT characterization of irradiated fuel samples showed formation of fission gas bubbles enriched with solid fission products. The intermediate burnup sample showed a uniform distribution of the typical bubble superlattice with a radius of 2 nm arranged in a regular lattice, while the high burnup sample showed a non-uniform distribution of bubbles in grain-refined regions. There was no evidence of remnant α-U, γ’-U2Mo, and UC phases in the irradiated U-7 wt.% Mo samples.

Bachhav, Mukesh↗

Unraveling the Early-Stage Ordering of Krypton Solid Bubbles in Molybdenum: A Multimodal Study

Self-organization of defects such as fission gas bubbles in materials can lead to high inventory capacity for fission gas storage and help mitigate swelling caused by fission gases in nuclear fuel materials under radiation in nuclear reactors. Here, we report the physical mechanism of self-organization of krypton (Kr) gas bubbles in molybdenum (Mo) under ion implantation. The ion fluence and temperature-dependent formation of Kr solid bubble superlattice (SBS) in Mo were investigated by using both synchrotron-based small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM). Early stage self-organization of gas bubbles is observed at a fluence of 2.5 × 10 16 ions/cm 2 at temperatures of 300–400 °C. The bubble lattice constant increases with increasing implantation temperature from 300 to 400 °C. Both experiments and atomic kinetic Monte Carlo modeling indicate that the Kr solid bubbles are weakly ordered in comparison to previously studied helium (He) gas bubble superlattice (GBS) while the lattice constant are relatively smaller for Kr SBS compared to that of He GBS. The irradiation conditions suggest that spinodal decomposition, which is a form of phase separation, probably precedes gas bubble ordering in Mo. Altogether, our work sheds light on the formation mechanism of noble gas superlattice toward the development of radiation-tolerant materials which are important for the design of advanced nuclear reactors.

36 MATERIALS SCIENCE↗