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Summary of Leach-Burn-Leach Round-Robin Test Results

Tristructural isotropic (TRISO) coated particle fuel is of interest to multiple member states associated with the Generation IV International Forum (GIF). Qualification and acceptance testing of TRISO fuel includes the determination of particle defect fractions and impurities in the as-fabricated TRISO fuel particle and/or composited fuel form, which are typically determined using burn-leach (BL) or leach-burn-leach (LBL) analysis methods. A round-robin test focusing on LBL analysis was undertaken by the GIF Very High Temperature Reactor System Fuel and Fuel Cycle Project Management Board. Participating in this LBL round-robin test were research staff from the Institute of Nuclear and New Energy Technology (INET) in the People’s Republic of China, the Korean Atomic Energy Research Institute (KAERI) in the Republic of Korea, and Oak Ridge National Laboratory (ORNL) in the United States of America. The motivation of this LBL benchmarking exercise was to explore consistency in results generated by LBL and to elucidate the potential influence of variations in the procedures used by the participating members on the accurate determination of the measured fuel properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Generation IV Benchmarking of TRISO Fuel Performance Models Under Accident Conditions Final Report

The Generation IV International Forum (GIF) is a co-operative international endeavor of fourteen members organized to carry out the research and development needed to establish the feasibility and performance capabilities of the next generation nuclear energy systems. GIF selected six reactor technologies, amongst which is the Very High Temperature Reactor (VHTR) that is primarily dedicated to the cogeneration of electricity and hydrogen. The technical basis for VHTR is the tristructural isotropic (TRISO)-coated particle fuel, the graphite as the core structure, helium coolant, as well as the dedicated core layout and lower power density to removal decay heat in a natural way. At the heart of safety features of the VHTR concept lie the TRISO fuel particles that are designed to keep their structural integrity and retain fission products at temperatures up to 1600°C. As part as the design and future operation of VHTRs, a key aspect is the accurate prediction of fuel performance under irradiation and accident conditions. Modeling and simulation allow prediction of TRISO fuel behavior when subject to neutron flux and in high temperature accident scenarios. The refinement of the fuel performance models and codes is performed by comparison to in-pile and out-of-pile experimental data that reproduce the expected irradiation conditions in high temperature gas-cooled reactors (HTGRs). Historically, the International Atomic Energy Agency (IAEA) developed a benchmark dedicated to the validation of predictive methods for fuel and fission product behavior through the Coordinated Research Program CRP-2 (IAEA, 1997). CRP-2 was later updated to cover fuel fabrication, quality assurance, irradiation performance, safety testing, and spent fuel. The scope of the resulting CRP-6 benchmarks focused on HTGR fuel performance and fission product release (IAEA, 2012). Taking advantage of additional TRISO fuel fabrication, irradiation, and safety testing campaigns, GIF launched a Generation IV Benchmarking of TRISO Fuel Performance Models under Accident Conditions in late 2015. This GIF benchmark is a three-year program steered by Idaho National Laboratory (INL, USA). The other participants include the Japan Atomic Energy Agency (JAEA, Japan) and the Korea Atomic Energy Research Institute (KAERI, Korea). The objectives of the benchmark are to: follow on the IAEA CRP benchmarks, (2) model fission product release under accident conditions, (3) compare results obtained by the fuel performance modeling codes of the benchmark participants, and (4) compare these code predictions to experimental data. Safety tests chosen for modeling include the first and second experiments of the Advanced Gas Reactor program (AGR-1 and AGR-2) and the High Flux Reactor (HFR) EU1bis experiment. This report presents the results obtained by the three research institutions using their respective fuel performance modeling codes. Comparisons of the corresponding fission product release predictions are made with experimental data from AGR-1, AGR-2, and HFR-EU1bis. The benchmark results show good agreements between all participants but also show a general trend of over-prediction of the experimental release data, which is mainly attributed to the use of over-estimated diffusion coefficients.

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A Machine Learning Approach Toward Improving QA/QC of Coated Particle Fuels

Coated particle fuels, such as the tristructural isotropic (TRISO) fuel particle, have been studied and developed for decades for high-temperature gas reactor (HTGR) applications because of their efficiency and relative stability under off-normal conditions. Critical to this development is a strong understanding of the relationship between fuel fabrication, properties and performance, as is how the former can be adjusted and improved to optimize the latter. Accordingly, wide-scale implementation of coated nuclear particle fuels requires thorough and robust quality assurance/quality control (QA/QC) methods for fabrication, characterization, and deployment

Conry, Bryan [ORNL] (ORCID:0000000236089604)↗

An Overview of Neutron Irradiated SiC Layer Behavior using Micro-and Nano-Characterization Techniques

The complexity of fission product distribution and composition within the SiC layer of tristructural isotropic (TRISO) coated particles, irradiation effects on the SiC structure as well as the variable nature of metallic fission product release, has led to the exploration of multiple micro- and nano-characterization techniques. The fine scale of the fission product precipitates necessitates unique learnings and application of electron microscopic techniques with irradiated fuel during the Advanced Gas Reactor (AGR)-1 experiment analysis. A summarized discussion on the specific advanced techniques with associated method development for TRISO coated particles is provided followed by the down selected techniques currently considered to provide the highest impact. Techniques considered are electron probe micro-analyzer (EPMA), scanning transmission electron microscopy (STEM), and Precession electron diffraction (PED). SiC grain boundary characteristics are evaluated due to the mobility of specific fission products through grain boundaries. PED was performed for understanding the role of grain boundary character on fission product transport. One set of comparative analyses between AGR-1 and AGR-2 particles leads to a finding that the AGR-1, high-Ag-retention particle, had statistically more coincidence site lattice (CSL)-related grain boundaries (but fewer low-angle grain boundaries), compared to the AGR-2 particle. This implies that CSL-related grain boundaries may have a direct influence on Ag retention. However, precipitates were found on a relatively small fraction of CSL-related grain boundaries in both particles. In another set of comparison between AGR-1 and AGR-2 particles that were subjected to safety testing, there is significant differences in average SiC grain boundary distributions, but the fission product distributions on these grain boundaries are very similar.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Micro- and Nano-techniques for the Study of Fission Product Precipitation in SiC Layer

The complexity of fission product distribution and composition within the SiC layer of tristructural isotropic (TRISO) coated particles, irradiation effects on the SiC structure as well as the variable nature of metallic fission product release, has led to the exploration of multiple micro- and nano-characterization techniques. The fine scale of the fission product precipitates necessitates unique learnings and application of electron microscopic techniques with irradiated fuel during the Advanced Gas Reactor (AGR)-1 experiment analysis. A summarized discussion on the specific advanced techniques with associated method development for TRISO coated particles is provided followed by the down selected techniques currently considered to provide the highest impact. Techniques considered are electron probe micro-analyzer (EPMA), scanning transmission electron microscopy (STEM), and Precession electron diffraction (PED). SiC grain boundary characteristics are evaluated due to the mobility of specific fission products through grain boundaries. PED was performed for understanding the role of grain boundary character on fission product transport. One set of comparative analyses between AGR-1 and AGR-2 particles leads to a finding that the AGR-1, high-Ag-retention particle, had statistically more coincidence site lattice (CSL)-related grain boundaries (but fewer low-angle grain boundaries), compared to the AGR-2 particle. This implies that CSL-related grain boundaries may have a direct influence on Ag retention. However, precipitates were found on a relatively small fraction of CSL-related grain boundaries in both particles. In another set of comparison between AGR-1 and AGR-2 particles that were subjected to safety testing, there is significant differences in average SiC grain boundary distributions, but the fission product distributions on these grain boundaries are very similar.

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Develop and Connect TRISO Failure Analysis and Uncertainty Quantification to Fission Product Release Calculation Capability

The U.S. Department of Energy’s Nuclear Energy Advanced Modeling and Simulation (NEAMS) program aims to develop predictive capabilities by applying computational methods to the analysis and design of advanced reactor and fuel cycle systems. This program has been providing engineering-scale support for the development of BISON, a high-fidelity and high-resolution fuel performance tool. Stress-based failure probability has been developed and analyzed to assess the integrity of tri-structural isotropic (TRISO) fuel particles during fuel life cycles. While simple, stress-based approaches to failure probability leveraging the Weibull statistical distribution entails a number of drawbacks when stress concentration occurs near crack tips, including finite element mesh size dependency. In this report, we use an interaction integral approach to the computation of stress intensity factors in functionally graded materials (FGM) for axisymmetric models. The inner pyrolytic carbon (IPyC) cracking induced silicon carbide (SiC) failure is one of the dominated failure modes in TRISO failure analysis. In this study, we consider a crack in the IPyC layer perpendicular to the SiC layer. The interface between these two TRISO layers is considered to be porous, which we simulate considering a transition of mechanical properties over the porous length. These aspects are considered in the computation of stress intensity factor (SIF) from a fracture mechanics approach and compared with the known stress-based failure probability approach.

42 ENGINEERING↗

Redistribution of radionuclides in irradiated AGR-1 UCO TRISO fuel after 1800 °C safety testing

Release of radionuclides from intact tristructural-isotropic (TRISO) coated particle fuel at normal and accident conditions is a primary metric of fuel performance. The distribution of fission products and actinides in the TRISO layers of individual particles provides insight on radionuclide transport and release behavior and was determined using scanning electron microscopy analysis. Particles were isolated from an irradiated fuel compact (AGR-1 Compact 4-4-2) and analyzed as-irradiated or after individual particle safety-testing at 1800 °C for 650 h. Particles were selected for comparison based on their remaining 110mAg fission product inventory. These comparisons corroborated the observation that the 110m Ag inventory is a marker for relative irradiation temperature based on observed radionuclide distribution in the SiC layer. The comparison also indicated that the in-pile behavior influences the fission product and actinide species interactions with the TRISO layers during high temperature exposure after irradiation. The analysis confirms both palladium and uranium diffusion, as well as other species, are active in the UCO TRISO fuel system at 1800 °C and that palladium transport is active at lower temperatures relative to uranium. While diffusion across the SiC layer was observed, the intact nature of the SiC layer after the 1800 °C, 650-h exposure indicates the SiC layer maintained its functionality as a fission product barrier by mitigating release of radionuclides at beyond accident margin temperatures.

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Determination of preferential binder oxidation in HTGR matrix material subjected to high temperature steam

Graphitic matrix material encapsulates tristructural isotropic (TRISO) coated fuel particles and is a structural component for both pebble and cylindrical fuel compacts in high temperature gas reactor (HTGR) designs. In an off-normal event involving steam exposure, the matrix material is exposed to oxidants, leading to degradation of the fuel compact and subsequent exposure of the TRISO particle fuel to oxidizing species. This study presents microstructural characterization of matrix material after exposure to high temperature (1200°C), 48 kPa steam in which the evolved microstructure demonstrated nonuniform degradation. Subsequent Raman spectroscopy determined the nature of the remaining material post-exposure. Finally, the electron microscopy characterization suggests and Raman spectroscopic analysis confirms, under off-normal conditions, the carbonized phenolic resin binder is preferentially oxidized ahead of the graphite flake filler and is responsible for the nonuniform degradation and enhanced depth of attack.

36 MATERIALS SCIENCE↗

Advanced Gas Reactor Fuel Specification Technical Bases

The technical bases for the TRISO-coated particle fuel specifications used by the AGR Program during its fabrication process development and fuel qualification efforts are provided based on historical HTGR fabrication experience in the U.S. and Germany and improvements and insights gained during execution of the AGR Program. The technical bases are provided for specified properties of the kernel, the TRISO coating layers, the fuel particle, and fuel compact in terms of fabricability considerations, in-pile fuel performance, and fission product release under normal and off-normal conditions.

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Comparison between PARFUME and Bison Using the AGR-2 Irradiation Experiment

This report documents comparisons between Fuel Model (PARFUME) model predictions versus Bison for selected compacts from the second irradiation test of the Advanced Gas Reactor (AGR) program that occurred from June 2010 to October 2013 in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). PARFUME is a fuel performance analysis and modeling code, used for evaluating gas-reactor tristructural isotropic (TRISO) coated particle fuel for prismatic, pebble bed, plate, and cylindrical type fuel geometries. PARFUME is an integrated mechanistic computer code that evaluates the thermal, mechanical, and physico-chemical behavior of TRISO coated-fuel particles and the probability for fuel failure given the particle-to-particle statistical variations in physical dimensions and material properties that arise during the fuel fabrication process. Bison is a nuclear fuel performance application built using the Multiphysics Object-Oriented Simulation Environment (MOOSE) finite element library (Permann 2020). Bison is capable of modeling multiple fuel forms in a wide variety of dimensions and geometries. It solves coupled nonlinear partial differential equations, including heat conduction, mechanics, fission product species transport etc., in a fully implicit manner. Comparisons between PARFUME and Bison were performed using four compacts from the AGR-2 experiment. Selected outputs were chosen based on their impact on the probability of the SiC layer failing. In general there was good agreement between PARFUME and Bison with the exception of predicting the gap formed between the buffer and IPyC. Further comparisons between PARFUME and Bison are planned to further develop Bison’s capabilities.

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FGMS-poster

Idaho National Laboratory (INL) performs post irradiation examination (PIE) of tri-structural isotropic (TRISO)-coated particle fuel to help qualify it for high temperature gas cooled reactors. TRISO fuel compacts are re-irradiated in the Neutron Radiography Reactor (NRAD) to generate the short lived fission products needed for fission product release testing. The Fuel Accident Condition Simulator (FACS) furnace and newly added Screen Neutron Irradiated Fuel for Failure (SNIFF) furnace heat the compacts in helium to temperatures of up to 2,000°C, prompting fission product release—predominantly gaseous xenon and krypton isotopes and condensable products such as cesium—from failed particles. These released isotopes are transported to a fission gas monitoring system (FGMS 1 or FGMS 3), where they accumulate in cryogenic cold traps and are quantified using high-purity germanium (HPGe) detectors. The addition of SNIFF and FGMS 3 increases throughput by enabling simultaneous testing of multiple compacts. Furthermore, automated INL developed software provides continuous, near-real time monitoring of fission product inventories and manages the liquid nitrogen cooling of the traps. These system enhancements improve the efficiency, data quality, and testing capacity of TRISO fuel performance evaluations.

07 - ISOTOPES AND RADIATION SOURCES↗

Oxidation Testing and Examination of AGR-2 Particles

Post-irradiation examination (PIE) oxidation testing is being performed at Oak Ridge National Laboratory (ORNL) on fuel particles from the second Advanced Gas Reactor (AGR) irradiation experiment (AGR-2). Tristructural isotropic (TRISO)-coated particles containing mixed uranium carbide and uranium oxide (UCO) fuel kernels were taken from AGR-2 Compact 5-4-2 and heated in the Furnace for Irradiated TRISO Testing (FITT) under varying oxidizing conditions. Details on Compact 5-4-2 PIE can be found in a previous report (Hunn et al. 2018).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Results of the AGR-5/6/7 UCO TRISO fuel irradiation test in the Advanced Test Reactor

AGR-5/6/7 was the last in a series of irradiation experiments sponsored by the U.S. Department of Energy in support of the development and qualification of TRISO coated particle fuel for use in a high-temperature gas-cooled reactor. This experiment was conducted to verify the performance of the reference-design TRISO-coated low-enriched UCO fuel for modular high-temperature gas-cooled reactor normal operating conditions and to explore fuel performance at temperatures substantially beyond those typical of normal operation. A total of 194 UCO fuel compacts in five capsules were irradiated in the Advanced Test Reactor for 360.9 effective full-power days, achieving final burnup ranging from 5.66% to 15.26% fissions per initial heavy metal atom and fast neutron fluence ranging from 1.62 × 10 25 to 5.55 × 10 25 n/m 2 (E > 0.18 MeV). Calculated time-averaged fuel temperatures ranged from 467 °C to 1432 °C, with a peak fuel temperature of 1536 °C. During the first five irradiation cycles (∼180 effective full-power days), 85m Kr fission gas release-rate-to-birth-rate ratios were 10 −7 –10 −6 , indicating no particle failures. Near the end of the sixth cycle, a substantial number of in-pile particle failures occurred in Capsule 1. The fission gas release from this capsule impacted the readings from the other four capsules and led to unreliable fission gas release measurements for all capsules during the last four cycles. A preliminary post-irradiation examination of Capsule 1 fuel and internal components revealed the in-pile particle failures resulted from operational issues with the capsule, not subpar performance of the fuel particles.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Review and Assessment of NGNP PIRTs for TRISO and HTGR Technologies

The main objective of this technical report is to ensure that research and development (R&D) needs are identified to address the significant (highly ranked) technical challenges related to TRISO-coated particle fuel, high-temperature gas-reactor (HTGR) technologies, and other TRISO-related advanced designs by recognizing the existing foundation of identified R&D needs and augmenting that foundation with insights drawn from current TRISO-related research results and R&D needs related to novel applications of TRISO-related technologies that extend beyond the traditional HTGR designs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fission Product Diffusion in Silicon Carbide: As Revealed by Computer Simulations and Experimental Measurements

The diffusion and release of fission products through silicon carbide in the tri-structural isotropic (TRISO) fuel particles remain unsolved for decades. The underlying mechanism is quite challenging to be determined. To help unveil the mysterious story, the current work applies molecular dynamics method to show the stability of silver, palladium, ruthenium and iodine as an interstitial and their atomic diffusion along coincident site lattice (CSL) boundary, especially ?3 grain boundary (GB). The major finding presents a much faster diffusion along GB than in bulk for all elements considered. The reasonably close estimate to experiments and simulations where available has confirmed the important role of grain boundary diffusion of Ag and Pd in SiC. However, the discrepancy addressed in Ag with measurements from fuel studies suggest a more complicated mechanism, which might be in correlation with high energy grain boundaries or the presence of crack. The subsequent characterization of Ru and I distribution in SiC-PyC-SiC diffusion couples, which have been ion irradiated at 900?C to 10 dpa and 20 dpa, has performed by secondary ion mass spectrometry (SIMS) analysis. The experiment measurements correlate well with the grain boundary diffusion by simulation, which provide further evidences that the grain boundary diffusion cannot be neglected once the fission products are accessible at the grain boundary.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Automated Segmentation of Twin Boundaries in TRISO Silicon Carbide Using Deep Neural Networks

Coated particle fuels, such as the tristructural isotropic (TRISO) fuel particle, are essential for high-temperature gas reactor (HTGR) applications due to their efficiency and stability under normal and off-normal conditions. However, widespread commercialization and deployment of this technology for next-generation nuclear applications require robust quality assurance and quality control (QA/QC) methods linking fabrication, properties, and performance. Of the many important metrics for TRISO QA/QC, quantification of the silicon carbide (SiC) microstructure is critical because it correlates with fission product retention during irradiation. Previous work has shown extensive twinning of the SiC microstructure, which strongly affects microstructural metrics; however, twin grain boundaries are not expected play a significant role in fission product diffusion. This report summarizes the initial development, training, and testing of a machine learning image processing algorithm to detect twin grain boundaries in a backscattered electron image, which can be removed so that microstructural metrics can be recalculated for legacy data. Further development and deployment of this model will provide automated, scalable improvement of potential QA/QC methods for the SiC layer of TRISO particles.

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