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  1. Characterization of the radial microstructural evolution in LWR UO2 using electron backscatter diffraction

    Studies on high burnup UO2 subjected to loss-of-coolant accident conditions have shown that restructured regions of the fuel are susceptible to pulverization and eventual dispersal. Due to a lack of pre-test characterization, the distinct microstructural features rendering the fuel prone to fragmentation remain ambiguous. Four samples of commercially irradiated light-water reactor UO2 have been characterized utilizing electron backscatter diffraction to assess the susceptible microstructure. The microscopy focused on determining the burnup and temperature conditions responsible for the formation of the different microstructural regions where the regions were denoted as the high-burnup structure (HBS), HBS transition, mid-radial, restructured central, and central region. Previous works have outlined the specific conditions required for the restructuring of the microstructure into the HBS, but the conditions responsible for the restructuring in the central region of the fuel are not well understood. The four analyzed samples confirm a burnup threshold of 61 GWd/tU, and an unknown temperature range is needed to facilitate the formation of the restructured central region. In conclusion, additional fuel performance evaluations are needed to quantify the temperature range promoting restructuring in the central region.

  2. Microstructural heterogeneity of the buffer layer of TRISO nuclear fuel particles

    Tristructural isotropic (TRISO) nuclear fuel particles contain a layered spherical shell designed to retain fission products; however, failure occurs in rare cases—commonly initiated in the porous pyrocarbon buffer layer. Achieving a comprehensive understanding of the buffer-initiated failure mechanisms requires detailed characterization of the buffer porosity and its heterogeneous distribution across multiple length scales. Here we performed FIB-SEM tomography across the buffer layer thickness (~100 µm) to produce 3D reconstructions of the buffer microstructure with 50 nm spatial resolution. We found an average overall porosity of ~14%, which does not solely account for the low density of the buffer (50% of the theoretical density). Additionally, the local porosity and its fluctuation increase from the kernel interface towards the inner pyrocarbon (IPyC) layer, which we attribute to the chemical vapor deposition process conditions during the TRISO particle fabrication. Detailed characterization of the porous microstructure—including analysis of the pore size, distribution, shape, and orientation—provides insight into the process-structure-property-performance relations of TRISO nuclear fuel particles and will inform multiscale models designed to predict the failure of TRISO particles under irradiation.

  3. Comparison of unirradiated and irradiated AGR-2 TRISO fuel particle oxidation response

    The silicon carbide (SiC) coating in a tristructural isotropic (TRISO) particle acts as a barrier to fission product release during reactor operation and accident scenarios. Oxidation and subsequent failure of the SiC layer during a rare air ingress event is a proposed mechanism for fission product release in a high-temperature gas-cooled reactor (HTGR). Although previous oxidation studies have analyzed unirradiated TRISO particle response, this study compared the oxidation behavior of irradiated and unirradiated TRISO particles from the second Advanced Gas Reactor Fuel Development and Qualification Program irradiation experiment (AGR-2). Particles with exposed SiC were subjected to six varying oxidizing tests in the Furnace for Irradiated TRISO Testing (FITT), examined for failure fraction with the Irradiated Microsphere Gamma Analyzer (IMGA) and characterized with focused ion beam and scanning/transmission electron microscopy techniques to analyze the oxide layer. Uncorrelated unirradiated particle failures throughout the series of exposures suggests that external factors inherent to the experiment increased particle failure sensitivity. However, irradiated particle observations indicated an increased failure response at 400 h 1400 °C in both 2% and 21% O2 atmospheres above failure associated with external factors. Oxide thickness measurements after 400 h at 1400 °C revealed a greater oxidation rate than predicted by parabolic growth, which was attributed to the increased complexity of the oxide structure at longer exposure times. Altering the atmosphere from 21% to 2% O2 reduced the average oxide thickness by approximately 12%–14% in both irradiated and unirradiated particles at 400 h 1400 °C. Altogether, the minor variations observed between irradiated and unirradiated particles in this study led to the conclusion that unirradiated TRISO particles can be used to approximate irradiated TRISO oxidation kinetics.

  4. Microstructural analysis of tristructural isotropic particles in high-temperature steam mixed gas atmospheres

    High-temperature gas-cooled reactors (HTGRs) use tristructural isotropic (TRISO) particles embedded in a graphitic matrix material to form the integral fuel element. Potential off-normal reactor conditions for HTGRs include steam ingress with temperatures above 1,000 °C. Fuel element exposure to steam can cause the graphitic matrix material to evolve, forming an atmosphere composed of oxidants and oxidation products and potentially exposing the TRISO particles to these conditions. Investigating the oxidation response of TRISO particles exposed to a mixed gas atmosphere will provide insight into the stability under off-normal conditions. In this study, surrogate TRISO particles were exposed to high temperatures (T = 1,200 °C) in flowing steam (3% < pH2O < 21%) and CO (pCO < 1%) to determine the oxidation behavior of the SiC layer when exposed to various mixed gas atmospheres. Scanning electron microscopy, x-ray diffraction, and focused ion beam milling was used to determine the impact of CO and steam on the oxidation behavior of the SiC layer. Therefore, the data presented demonstrates how the SiC layer showed strong oxidation resistance due to limited SiO2 growth and maintained its structural integrity under these off-normal conditions.

  5. Investigation of Coincidence Counting for Improving Minimal Detectable Activity of 110mAg in Single Particle Gamma Analysis

    Post-irradiation examination (PIE) of fuel particles from the fourth Advanced Gas Reactor Fuel Development and Qualification (AGR) Program irradiation (AGR-5/6/7) is being performed at Oak Ridge National Laboratory (ORNL). Tristructural isotropic (TRISO)-coated particles and associated compacts for the AGR-5/6/7 experiment fabricated by BWX Technologies Nuclear Operations Group were formed into a graphite matrix compact and irradiated at the Advanced Test Reactor at Idaho National Laboratory. At ORNL, particles are deconsolidated from the graphite matrix compact and individually scanned for emitted gamma rays with the Irradiated Microsphere Gamma Analyzer (IMGA). The IMGA system comprises a single high purity germanium (HPGe) detector, an automated particle handling vacuum system, and an ORTEC DSPEC-50 digital spectrometer for gamma ray analysis. IMGA quantifies gamma ray-emitting fission product inventories of individual TRISO particles, and these inventories can be compared with the measured average inventories per particle and radionuclide inventories predicted by AGR-5/6/7 physics calculations to determine if a particle experienced radionuclide release. Details on IMGA data collection methods can be found in the literature. The TRISO particle’s SiC layer provides structural support, as well as a barrier for fission product release during irradiation or subsequent safety testing. A weakened or compromised SiC layer can be identified by the release of radionuclides, such as 137Cs, which is detected by IMGA. However, select radionuclides, such as 90Sr, 110mAg, and 154Eu have been shown to migrate through an intact SiC layer. Measurement of the radionuclide 110mAg is significant as its release has been shown to be particularly sensitive to in-reactor conditions (e.g., temperature) with broad variable particle to-particle release behaviors observed within a single compact. As such, 110mAg activity is often used for particle selection for comprehensive PIE as bounding 110mAg retention particles are hypothesized to represent limits in particle behaviors within a compact. As TRISO particle fuel PIE activities continue over time, IMGA measurements of the 110mAg inventory are eventually hindered because of its relatively short half-life (~250 days). As the fuel ages from its end of irradiation (EOI) date, the measurement uncertainty and minimum detectable activity (MDA) of 110mAg increase because the detector background continuum begins to dominate. For particles from the second AGR irradiation experiment (AGR-2), the 110mAg MDA was above 20% of the calculated average particle inventory after approximately five half-lives, and 110mAg activity was no longer measurable with IMGA after approximately seven half-lives. Therefore, coincidence counting approaches have been explored to determine feasibility of leveraging new approaches to overcome limitations associated with increasing MDA over time.

  6. AGR-2 irradiated TRISO particle IPyC/SiC interface analysis using FIB-SEM tomography

    In this work, the morphology in the interface region between the inner pyrolytic carbon layer (IPyC) and silicon carbide (SiC) layers in tristructural-isotropic (TRISO) particle fuel from the AGR-2 irradiation experiment were studied using focused ion beam-scanning electron microscopy tomography. This work quantitatively described the interface and corresponding relevant metrics to understand how the microstructural features at the IPyC/SiC interface may influence actinide and fission product interactions with the SiC layer. Particles were selected with varied 110mAg retention rates, and their volumes were reconstructed and analyzed for distributions of pores, fission product/actinide features, SiC, and IPyC. It was found that porosity accommodates fission products in the interface and SiC layers. The largest fission product/actinide precipitates were found in the interface region. This was also where the largest number fraction of fission products/actinides was found, consistent with SEM showing fission product/actinide pileup along selected areas of the interface region.

  7. High-temperature oxidation behavior of the SiC layer of TRISO particles in low-pressure oxygen

    Abstract Surrogate tristructural‐isotropic (TRISO)‐coated fuel particles were oxidized in 0.2 kPa O 2 at 1200–1600°C to examine the behavior of the SiC layer and understand the mechanisms. The thickness and microstructure of the resultant SiO 2 layers were analyzed using scanning electron microscopy, focused ion beam, and transmission electron microscopy. The majority of the surface comprised smooth, amorphous SiO 2 with a constant thickness indicative of passive oxidation. The apparent activation energy for oxide growth was 188 ± 8 kJ/mol and consistent across all temperatures in 0.2 kPa O 2 . The relationship between activation energy and oxidation mechanism is discussed. Raised nodules of porous, crystalline SiO 2 were dispersed across the surface, suggesting that active oxidation and redeposition occurred in those locations. These nodules were correlated with clusters of nanocrystalline SiC grains, which may facilitate active oxidation. These findings suggest that microstructural inhomogeneities such as irregular grain size influence the oxidation response of the SiC layer of TRISO particles and may influence their accident tolerance.

  8. Texture analysis of AGR program matrix materials

    We report the fuel form for high-temperature gas-cooled reactors consists of tristructural isotropic (TRISO) particles embedded in a matrix of graphite flake and carbonized resin. The process of overcoating particles prior to compacting yields a circumferential orientation of the graphite flake surrounding the TRISO particles, which is modified to varied extents when overcoated particles are pressed into the final fuel form. As graphite is highly anisotropic, the texture may impact the properties and performance of the fuel. Ellipsometry was used to measure the texture of the matrix for fueled compacts and unfueled “matrix-only” samples. Results indicated local texture related to the spherical particles in compacts associated with overcoating versus a more linear layered structure in “matrix-only” samples.

  9. Simulation of a TRISO MiniFuel irradiation experiment with data-informed uncertainty quantification

    An irradiation experiment using tristructural isotropic (TRISO) fuel particles and the miniature fuel (MiniFuel) irradiation vehicle was performed in Oak Ridge National Laboratory’s High Flux Isotope Reactor (HFIR) to support development of the Kairos Power fluoride salt–cooled, high-temperature reactor (KP-FHR). Here, this paper describes modeling predictions of temperatures and fuel burnup for the as-built experiment. An uncertainty quantification (UQ) analysis was performed to determine the effect of TRISO particle volume and position on the temperature predictions at various fuel heat generation rates (HGRs). This UQ study utilized fuel kernel position and volume measurements previously collected using X-ray computed tomography (XCT) techniques and Monte Carlo sampling methods to generate fuel compact cases that were then analyzed using a finite element thermal model. The UQ analysis indicated that uncertainty in calculated temperatures caused by varying TRISO particle arrangement is relatively small, even at high fuel HGR. Final predictions of particle temperatures throughout the irradiation are shown to be relevant to KP-FHR normal and off-normal operating conditions and to previous TRISO irradiation experiments. The combination of XCT with UQ analyses will inform post-irradiation examination (PIE) of the irradiated fuel compacts, and these analyses can be used to develop fuel performance models for coated particle fuel forms. Both PIE of separate-effects irradiation data and enhanced fuel performance modeling support accelerated qualification of TRISO fuels for a broad range of advanced reactor applications. The novel approach demonstrated here of measuring TRISO particle configurations with XCT methods and generating representative fuel compacts for finite element modeling and UQ analysis could be leveraged by the broader particle fuel community in the development of other TRISO fuel experiments in which these variables may have a significant impact on key outcomes.

  10. Nuclear fuel irradiation testbed for nuclear security applications

    The nuclear security community has long been interested in the identification and quantification of nuclear material signatures to understand a material’s provenance, use, and ultimate application. New forensics signatures and methods intended for non-traditional or advanced nuclear fuel applications require fuel irradiation experiments to demonstrate viability and validity. Integral fuel irradiations have historically required significant costs and long timelines to design, irradiate, and characterize. This paper describes how a recently developed nuclear fuel irradiation testbed can be used to provide a low cost, rapid turnaround, modular test environment for irradiation and evaluation of nuclear fuel specimens for nuclear security applications. The irradiation testbed houses six small ‘MiniFuel’ samples within hermetically sealed capsules inside targets that can be removed in between each ~25-day operating cycle of the High Flux Isotope Reactor (HFIR). As many as nine targets can be irradiated using a single irradiation position (reflector region) in HFIR, allowing for varying irradiation temperatures and burnups. A suite of hot cell capabilities have been established to perform post-irradiation examination for measuring performance (e.g., fuel swelling, fission gas release) and facilitating experiment disassembly for subsequent property measurements, microstructural analysis, or chemical assay. This new testbed allows fuel irradiations to be conducted on an accelerated timeframe to enable rapid proof of concept testing and to provide reference material for nuclear fuel security applications. Recent applications using this testbed include the testing of isotopic taggants in UO2 fuel (intentional forensics), testing of U-10Mo fuel for down-conversion of highly enriched uranium–fueled reactors, and the production of irradiated UO2 fuel material for signature analysis of its isotopic composition (plutonium, fission gases, etc.).


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