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Determination of Average Burnup in AGR-3/4 Compacts 1-4 and 7-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined in one test train for irradiation in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011, and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support the improvement of modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and post-irradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite. These two goals were combined in the AGR-3/4 irradiation, which consisted of 12 independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. Two capsule types were used: a standard capsule and a so-called fuel body, in which the outer graphite ring included a floor and cap that fully enclosed the fuel. The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from the matrix and graphite at accident temperatures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

X-ray Computed Tomography of Irradiated and Unirradiated AGR-3/4 Compacts

X-ray Computed Tomography (XCT) has been utilized to image and characterize compacts from the combined third and fourth irradiation of the Advanced Gas Reactor (AGR) Program, AGR-3/4, fuel. The experiment contained tristructural isotropic (TRISO)-coated fuel particles as well as designed-to-fail (DTF) fuel particles. Two irradiated compacts, representing the lower and higher range of AGR-3/4 burnup (4.85% and 14.92% fissions per initial heavy metal atom FIMA) were examined. These represent the first known highly irradiated TRISO fuel compacts to be examined via X-ray CT. Additionally, two unirradiated compacts from the same production batch as the examined irradiation compacts were also imaged for a baseline comparison. As XCT of irradiated TRISO compacts is not a commonly implemented characterization technique, a significant portion of the report focuses on developed methodology and imaging conditions. A specialized sample shielding device was developed and fabricated specifically to limit received dose to staff during sample preparation for XCT and to minimize excess gamma radiation dose to sensitive electronic components with the utilized X-ray system. Significant penetration through the uranium oxycarbide fuel kernels by significantly hardening the X-ray beam with specialized proprietary filters acquired from Carl Zeiss NTS Ltd. The filter utilized resulted in an average X ray photon energy of ~110 keV which approaches uranium’s K-edge (~115 keV), maximizing penetration for a microfocus X-ray source. The gamma-radiation emitted from the irradiated AGR-3/4 TRISO compacts, has the same properties and mechanisms for interaction with matter as X-rays, thus the detection of gamma-radiation by the utilized X-ray detectors was initially a concern. However, although ?-rays did produce an observable signal on the X-ray detector, its contribution to the overall imaging results appeared negligible upon 3D reconstruction. The neglibile impact on the resulting 3D reconstructed volumes were likely the result of: (1) a significantly lower detection efficiency for ?-rays relative to X-rays; (2) An X-ray flux at the detector several orders of magnitude higher than that of the impinging ?-rays from the irradiated compacts. These results suggest that irradiated compacts with significantly higher radiation fields can be examined in the future if an acceptable route for sample handling and preparation can be determined. Additionally, the 3D imaging results of XCT can provide a valuable means of assessing compacts. While in many ways complimentary to traditional post irradiation examination techniques such as optical ceramography, XCT can provide additional insight into compact features traditionally difficult to discern directly from cross-sectional imaging alone. Preliminary analyses on kernel size, morphology (aspect ratio and sphericity), and kernel orientation were presented. Sphericity, a simple morphological shape descriptor, was utilized to screen for kernel extrusions within the high burnup compact. The number of kernel extrusions identified via XCT represented an approximate two-fold increase from the quantity of extruded particles observed (via optical ceramography) in adjacent compacts from the same irradiation capsule. While numerical analysis of the compact datasets was highly preliminary, initial results show promise for providing complimentary metrics to current AGR-3/4 PIE and potentially additional insight into the processes driving TRISO fuel degradation during reactor operation. Additional analyses to be performed at a later date include a more detailed examination of kernel size, kernel sphericity (and observed kernel extrusions), and sphericity. Given all particles can be observed in a single data volume possible correlation of spatial position with observed kernel features will also be made at a later date.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of fission product distribution and composition in the TRISO layers of AGR-2 fuel

The Advanced Gas Reactor Fuel Qualification and Development Program's second irradiation experiment focuses on the performance of fuel particles produced in an industrial-scale coating system. Ongoing post-irradiation examination efforts include exploration of tristructural-isotropic (TRISO)-coated particle fuel in the as-irradiated state and subjected to elevated temperatures to simulate accident conditions (safety testing). Scanning electron microscopy (SEM) analysis with energy dispersive x-ray spectroscopy (EDS) was used to show the distribution of fission products within the TRISO layers. The SEM analysis showed a variation of fission product distribution within the TRISO layers based on irradiation temperature, burnup, individual particle fission product inventory retention, safety testing history and kernel composition. Finally, a key observation is that particles which likely experienced higher temperature showed a greater diversity and distribution of fission products and actinides in the IPyC and SiC layers, implying that temperature is a dominant variable influencing the transport of radionuclides in TRISO particles.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compacts 8-4 and 7-4

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined into one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011, and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both to be focused on obtaining fission product transport data to support improvements in modeling. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and postirradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These goals were combined in the AGR-3/4 irradiation experiment, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a fuel body, in which the outer graphite ring included a floor and cap to fully enclose the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to obtain data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Radial Deconsolidation and Leach-Burn-Leach of AGR-3/4 Compacts 1-3, 4-3, 10-1, and 10-2

The Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s third and fourth irradiation experiments (AGR-3/4), originally planned as separate tests, were combined into one test train for irradiation in the Advanced Test Reactor at Idaho National Laboratory (INL). The irradiation test began on December 14, 2011 and ended on April 12, 2014 (Collin 2016). The originally planned AGR-3 and AGR-4 irradiation experiments were both focused on obtaining data on fission product transport to support modeling improvement. The AGR-3 experimental plan was focused on gaseous and metallic fission product release from the kernels and diffusion in the coatings during irradiation and post-irradiation safety testing. The AGR-4 experimental plan was focused on diffusivities and sorptivities in the compact matrix and reactor graphite (Petti et al. 2005). These two goals were combined in the AGR-3/4 irradiation, which consisted of twelve independently monitored capsules that each contained four AGR-3/4 compacts in a single stack surrounded by an inner ring of matrix or graphite and an outer ring of graphite. There were two capsule types: a standard capsule and a fuel body in which the outer graphite ring included a floor and cap that fully enclosed the fuel (Stempien et al. 2018a). The fuel body design supported post-irradiation safety testing of the intact fuel and ring assembly to provide data on fission product transport and release from matrix and graphite at accident temperatures (Demkowicz 2017)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development of Data Reporting Standards for High-Temperature Gas-cooled Reactor (HTGR) Nuclear Energy University Program (NEUP) Thermal-Fluid Experiments

Since 2009, the U.S. Department of Energy (DOE) Office of Nuclear Energy's Nuclear Energy University Program (NEUP) has been at the forefront of nuclear research, specifically concentrating on advancing high-temperature gas-cooled reactor (HTGR) technologies. By Fiscal Year 2023, NEUP has authorized 35 projects dedicated to HTGR research, each contributing significantly to the enhancement of our understanding of this technology. The outcomes of these diverse projects have been disseminated through final NEUP reports, peer-reviewed journal articles, and presentations at academic conferences, forming a comprehensive tapestry of knowledge. Despite the substantial value of these findings, their dissemination has been fragmented, posing challenges for accessibility to researchers and policymakers and leading to underutilization of DOE investments. Recognizing this critical gap and its potential consequences for the future of nuclear research, the Advanced Reactor Technologies (ART) Gas-Cooled Reactor (GCR) program conducted an extensive survey of completed and ongoing HTGR NEUP projects. This survey enabled the compilation of crucial data, resulting in the development of a specialized public-access database tailored for computational fluid dynamics and system code validation, specifically designed for HTGR applications. However, the data collection process revealed a significant challenge in central data organization due to individual researchers from different institutes employing varying logics and preferences for recording and documenting experimental data. Consequently, an urgent need has been identified to establish a standardized reporting format for HTGR experimental projects. Addressing this issue is essential for enhancing collaboration, maximizing the impact of DOE investments, and ensuring the seamless advancement of HTGR technologies in nuclear research.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Thermal Hydraulics Validation Activities in the ART-GCR Campaign

The Advanced Reactor Technologies - Gas Cooled Reactor Campaign (ART-GCR) is part of the United States Department of Energy - Office of Nuclear Energy's Advanced Reactor Technologies program aimed at developing a High Temperature Gas-cooled Reactor (HTGR) which will offer enhancements in safety and efficiency. The Design, Methods, and Validation arm of the ART-GCR program provides experience and advanced tools for HTGR design and analysis. The Methods and Validation arm is developing data to validate predictions of decay heat removal through an extensive experimental campaign the Natural Convection Shutdown Heat Removal Test Facility at Argonne National Laboratory. In-core thermal hydraulics validation is being facilitated through the OECD/NEA's Thermal Hydraulic Code Validation Benchmark for High Temperature Gas-Cooled Reactors using HTTF Data. That benchmark contains code-to-code and code-to-data comparisons for 3 sets of HTGR thermal hydraulics phenomena. This ongoing benchmark activity has 16 participants from 9 countries developing leading insights into HTGR thermal hydraulics code validation. The ART-GCR campaign is also working on the development of state-of-the-art MOOSE-based models of the High Temperature Engineering Test Reactor (HTTR). Through the OECD/NEA's HTTR Loss of Forced Cooling (LOFC) program, the ART-GCR campaign is developing a multiphysics transient code validation benchmark based on 3 HTTR experiments that will provide an opportunity for international collaboration on multiphysics code validation.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗

Design of a first-of-A-kind instrumented advanced test reactor irradiation Capsule experiment for In situ thermal conductivity measurements of metallic fuel

Metallic fuel undergoes dramatic microstructural changes early in life due to fission gas swelling until ~2–3 at% burnup which affects the conductivity of the material, however the evolution of metallic fuel thermal conductivity during this early phase burnup has never been successfully measured in situ. The Irradiated Material Properties Accelerated Characterization Test (IMPACT) experiment will be the first in a series of experiments to irradiate advanced nuclear metallic fuel specimens with novel embedded thermal conductivity probes in ATR. In the current work the IMPACT experiment final design and supporting analysis is reported in detail. Results are evaluated for various reactor operational conditions to meet the functional requirements of the experiment. Finally, the first iteration of this IMPACT experiment will provide data regarding thermal properties evolution in uranium-zirconium (U10Zr) fuel, but this experiment vehicle is envisioned for future advanced fuels and structural materials irradiations in ATR.

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DOE Advanced Gas Reactor Fuel Development and Qualification Program Overview

AGR-3/4 post-irradiation examination and data analysis AGR-5/6/7 PIE and safety testing Supplemental fuel microanalysis and method development Fuel oxidation testing Air/moisture Ingress Experiment (AMIX) system development (deployed in FY23) Single particle testing in FITT Data management and analysis Fuel performance modeling

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Safety Testing and Destructive Examination of AGR-2 UO 2 Compact 3-1-1

Post-irradiation examination and elevated-temperature safety testing are being performed on compacts from the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s second irradiation experiment (AGR-2). The compacts in the AGR-2 irradiation experiment held either tristructural isotropic (TRISO)-coated particles containing uranium oxide fuel kernels (UO 2 ) or TRISO-coated particles containing fuel kernels with both uranium carbide and uranium oxide phases (UCO). In UO 2 TRISO particles, oxygen released by uranium fission can react with the surrounding carbon in the buffer layer to form carbon monoxide (CO). Excess CO can lead to various irradiation performance issues under certain operating conditions, such as pressure-induced fracture, kernel migration, and silicon carbide (SiC) corrosion. In UCO TRISO particles, CO formation is reduced because the chemical potential for oxidation of uranium carbide is lower than for oxidation of carbon.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

TRISO Fuel Development and Qualification in the US

Presentation of TRISO Fuel Development and Qualification in the US. Including Status of HTGR and TRISO Technology Circa 2000, Advanced Gas Reactor focus on licensing and domestic TRISO fuel fabrication capabilities. Irradiation experiments discussed include AGR-1, AGR-2, AGR-5/6/7, and AGR-3/4. Results, of tests and Kernel and coating behaviors during irradiation, Fission product release from UCO Fuel Compacts, study of failed particles, safety and accident performance summaries, and Parfume modeling and capabilities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AFIP6-MkII and RERTR-12 Porosity Data Collection and Analysis for Modeling and Simulation

Gathering data for the improvement of nuclear fuel modeling and simulation efforts is the primary driver for this work. Mechanistic models allow for a better understanding of the material on a micro- and macrostructural level while saving time and money over traditional experiment efforts. Historically, summarized data and correlations are the inputs for empirical material models and model validation. When improving these models for nuclear fuels with experimental results, there is a lack of reliable data readily available. Experiments - RERTR-12 and AFIP6-MkII - were conducted to understand the irradiation behavior of metallic U-10Mo monolithic fuels for use in extreme reactor environments such as research reactors like the Advanced Test Reactor (ATR) or the High Flux Isotope Reactor (HFIR). Microstructural characteristics of fission gas pores (FGP) in each experiment are collected using an automated image analysis technique developed at the University of Florida and presented here. A series of statistical tests are performed to explore the reliability of the results, as well as understand where the data is lacking and what future data collection is necessary to provide sufficient information to assist modeling efforts. The focus is on the porosity, pore size, and eccentricity of FGPs formed during irradiation in three AFIP6-MkII samples and one RERTR-12 sample. From the analysis, it is clear there are substantial impacts of fission density on the pore structure, but there also exist also underlying connections between each sample and the behavior observed in the pores. Further analyses of the pre- and post-irradiation microstructure are needed to improve the understanding of these connections. An early method for microstructural data analysis is presented within and is currently being expanded to include other microstructure data.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fission Product Quantification and Burnup Analysis via Gamma Spectrometry of the AGR-5/6/7 TRISO Fuel Experiment

Five capsules containing varying configurations of TRISO fuel compacts were irradiated in the most recent Advanced Gas Reactor (AGR) TRISO test campaign, AGR-5/6/7. As part of the post-irradiation examination (PIE) of this work all the fuel compacts and capsule graphite holders were measured with the Precision Gamma Scanner (PGS) to determine isotopic activities and locations using gamma spectrometry. Measuring the compacts allowed for the comparison of physics model depletion calculations with the measured compact activity to validate models. These measurements also are used to find compacts of interest with low fission product retention that may be tested in subsequent PIE. Measurements of the holders can confirm fission product distribution and migration. Of the isotopes measured, Cs-137 and Cs-134 were used to estimate location of failed particles as well as determine a measured burnup estimation. Results from Capsule 1 compacts and the holder indicate many fuel particle failures occurred. There are high amounts of cesium in the holder near Stack 9 of Capsule 1 that corresponds to low fractions?measured-to-calculated (M/C) ratio?of cesium remaining in those compacts. All other capsules had cesium retention ratios near 1. The isotope 110mAg had less consistent results. Capsule 2 compacts exhibited a M/C of 0.20, much lower than anticipated for the temperatures these compacts underwent. Capsule 3 experienced much higher temperatures, >1300C and had an average M/C of 0.75. These are the opposite results than what was predicted by past AGR experiments for the relationship between temperature and isotope retention. Capsule 4 and 5 showed good fission product retention and agreement with the physics model predictions. The burnup results from the PGS measurements showed strong agreement between the physics models and the measured values. Using a ratio of Cs-134/Cs-137 to calculate the burnup match closely with the physics models. Additionally, the Cs-137 burnup results were less accurate but extremely close to the model results.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gamma Spectrometry Examination of the AGR-3/4 Irradiation

The results from gamma spectrometry examination of the different components from the combined third and fourth U.S. Advanced Gas Reactor (AGR) TRISO-coated particle fuel irradiation tests (AGR-3/4) have been analyzed. This experiment was designed to provide information about in-pile fission product migration. In each of the 12 capsules, a single stack of four compacts with designed-to-fail (DTF) particles surrounded by inner and outer graphite and/or graphitic matrix rings and a graphite sink ring were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). Gamma spectrometry has been used to evaluate the gamma-emitting fission product inventory of compacts from the irradiation and evaluate the burnup of these compacts based on the activity of the radioactive cesium isotopes (i.e., Cs-134 and Cs-137) in the compacts. Burnup from gamma spectrometry compares well with predicted burnup from simulations. The inner and outer rings were also examined by gamma spectrometry to evaluate the total fission product inventory of the rings, and gamma emission computed tomography (GECT) was used to investigate the spatial distribution of gamma-emitting fission products within the rings. This report focuses on results obtained via the Precision Gamma Scanner (PGS) for the compacts and inner and outer rings. These non-destructive gamma measurements are currently being compared to recent destructive measurements of spatial fission product distributions in the rings and to predictions made via mathematical modeling. A separate report discusses the entire AGR-3/4 fission product mass balance for all irradiation capsule components including the inner and outer rings, graphite sink rings, capsule spacers, capsule foils, through tubes, and felts. This report is similar to the conference proceedings: Harp, J.M., Demkowicz, P.A., and Stempien, J.D., “Initial gamma spectrometry examination of the AGR-3/4 irradiation,” International Topical Meeting High Temperature Reactor Technology (HTR 2016), Las Vegas, NV, USA, November 2016, Paper HTR2016-18593, but it has been updated to reflect all the data that has been collected on AGR-3/4 using PGS. The Appendices contain extensive data from the collected gamma spectra.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gamma Spectrometry Examination of the AGR-3/4 Irradiation

The results from gamma spectrometry examination of the different components from the combined third and fourth U.S. Advanced Gas Reactor (AGR) TRISO-coated particle fuel irradiation tests (AGR-3/4) have been analyzed. This experiment was designed to provide information about in-pile fission product migration. In each of the 12 capsules, a single stack of four compacts with designed-to-fail (DTF) particles surrounded by inner and outer graphite and/or graphitic matrix rings and a graphite sink ring were irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). Gamma spectrometry has been used to evaluate the gamma-emitting fission product inventory of compacts from the irradiation and evaluate the burnup of these compacts based on the activity of the radioactive cesium isotopes (i.e., Cs-134 and Cs-137) in the compacts. Burnup from gamma spectrometry compares well with predicted burnup from simulations. The inner and outer rings were also examined by gamma spectrometry to evaluate the total fission product inventory of the rings, and gamma emission computed tomography (GECT) was used to investigate the spatial distribution of gamma-emitting fission products within the rings. This report focuses on results obtained via the Precision Gamma Scanner (PGS) for the compacts and inner and outer rings. These non-destructive gamma measurements are currently being compared to recent destructive measurements of spatial fission product distributions in the rings and to predictions made via mathematical modeling. A separate report discusses the entire AGR-3/4 fission product mass balance for all irradiation capsule components including the inner and outer rings, graphite sink rings, capsule spacers, capsule foils, through tubes, and felts. This report is similar to the conference proceedings: Harp, J.M., Demkowicz, P.A., and Stempien, J.D., “Initial gamma spectrometry examination of the AGR-3/4 irradiation,” International Topical Meeting High Temperature Reactor Technology (HTR 2016), Las Vegas, NV, USA, November 2016, Paper HTR2016-18593, but it has been updated to reflect all the data that has been collected on AGR-3/4 using PGS. The Appendices contain extensive data from the collected gamma spectra.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

IMPACT-01 Assembly Overview [Slides]

The Irradiated Material Properties Accelerated Characterization Test (IMPACT) series of experiments will irradiate three metallic fuel alloy specimens with embedded thermal conductivity probes in the Advanced Test Reactor (ATR). Metallic fuel alloys have long been under investigation for use in advanced reactors on account of their high thermal conductivity. Metallic fuel undergoes dramatic microstructural changes early in life due to fission gas swelling until ~2-3 at% burnup when pores interconnect, thus allowing fission gas to escape into the fuel pin plenum and swelling effectively ceases. The evolution of metallic fuel thermal conductivity during this early phase has never been successfully measured in situ. This experiment will be designed to use advances in measurement sciences to characterize how thermal transport properties evolve while in reactor. The IMPACT experiment consists of three metallic fuel rodlets with thermal conductivity probes axially centered within the fuel specimen. This presentation is an overview of the IMPACT-01 assembly process with a focus MFC fuel fabrication and experiment assembly steps.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Horizontal Split Table Conceptual Design for Validation of Nuclear Data used in Advanced Reactors [Slides]

A methodology to create conceptual designs of benchmark critical experiments for advanced reactors nuclear data testing and validation was developed. A first concept was explored, pebble-bed high-temperature gas cooled reactor, based on the HTR-10 reactor. The very high correlation is a proof of concept that the design is similar to the application, and performing such critical experiments would help nuclear data testing and validation. This proof-of-concept was included in the IER-539 CED-1:Preliminary Design of a New Horizontal Split Table report. Other concepts could be explored if needed, such as Molten-salt reactor, Sodium-cooled fast reactor or Heat pipe reactors/Microreactor.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Horizontal Split Table Conceptual Design for Validation of Nuclear Data used in Advanced Reactors [Slides]

This presentation discusses a methodology that was developed to create conceptual designs of benchmark critical experiments for advanced reactors and nuclear data testing. A first concept that was explored was a pebble-bed high-temperature gas cooled reactor, based on the HTR-10 reactor. The very high correlation is a proof of concept that the design is similar to the application, and performing such critical experiments would help nuclear data testing and validation. Other concepts could be explored if needed, such as a molten-salt reactor, a sodium-cooled fast reactor, or heat pipe reactors/microreactor.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗