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DOE OSTI2021

Summary of Previous Mechanical Test Data on ODS Alloys 14YWT and OFRAC up to 1000ºC

The Nanostructured Ferritic Alloys (NFA) 14YWT and OFRAC were developed for future fission and fusion nuclear energy reactors requiring high-temperature mechanical properties that are tolerant to extreme neutron irradiation environments. The NFA contain a high concentration of Ti-, Y- and O-enriched nanoclusters (NC) and ultra-fine grains to achieve high temperature strength and creep properties and high sink strength for trapping irradiation induced point defects to minimize hardening and swelling and transmutated He atoms to form intragranular nano-size bubbles that prevent formation of coarse bubbles on grain boundaries that cause embrittlement. The mechanical properties of 14YWT and OFRAC have been acquired from tensile and creep tests conducted in the past at Oak Ridge National Laboratory. The development of 14YWT started in 2000, resulting in the production of numerous heats. Tensile properties were obtained from eleven heats of 14YWT from room temperature to 800ºC. Tensile data for the SM10 heat of 14YWT was extended to 1,000ºC. Initial development of OFRAC occurred in 2016. Tensile tests conducted from room temperature to 800ºC revealed similar properties of OFRAC with those obtained from the newer generation of 14YWT heats. The creep properties of 14YWT-SM10 evaluated using constant stress tensile and load time-to-failure tests at 800ºC showed low minimum creep rates with stresses of 200 and 100 MPa. The single time-to-failure test of 14YWT-SM10 at 800ºC and 100 MPa was terminated after 20,357 hours with no specimen failure and a low creep strain of ~0.24 %. The creep properties of OFRAC determined from strain-rate jump tests at were similar those of 14YWT-SM10. The stress exponent for 14YWT and OFRAC at 800ºC are similar and are consistent with threshold stress behavior. Since both 14YWT and OFRAC are candidates for fuel cladding in future fast reactors, several fabrication studies were recently conducted and have successfully demonstrated that thin wall tubes can be fabricated from 14YWT and OFRAC by cold pilger rolling and high precision tube rolling. The high temperature mechanical properties and feasibility of fabricating thin wall tubes make 14YWT and OFRAC candidates for application as heat pipes in advanced micro-reactors. The purpose of this report is to summarize the previously obtained tensile and creep data at temperatures up to 1000ºC for NFA 14YWT and OFRAC that have been acquired over the past 20 years at ORNL.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Impact of iodide ions on the speciation of radiolytic transients in molten LiCl–KCl eutectic salt mixtures

The fate of fission-product iodine is critical for the deployment of next generation molten salt reactor technologies, owing to its volatility and biological impacts if it were to be released into the environment. To date, little is known on how ionizing radiation fields influence the redox chemistry, speciation, and transport of iodine in high temperature molten salts. Here we employ picosecond electron pulse irradiation techniques to elucidate for the first time the impact of iodide ions (I – ) on the speciation and chemical kinetics of the primary radiation-induced transient radicals generated in molten chloride salt mixtures (e S – and Cl 2 ˙– ) as a function of temperature (400–700 °C). In the presence of I – ions (≥ 1 wt% KI in LiCl–KCl eutectic), we find that the transient spectrum following the electron pulse is composed of at least three overlapping species: the e S – and the Cl 2 ˙– and ICl ˙– radical anions, for which a deconvoluted spectrum of the latter is reported here for the first time in molten salts. This new transient spectrum was consistent with gas phase density functional theory calculations. The lifetime of the e S – was unaffected by the addition of I – ions. The newly observed interhalogen radical anion, ICl˙ – , exhibited a lifetime on the order of microseconds over the investigated temperature range. The associated chemical kinetics indicate that the predominate mechanism of ICl˙ – decay is via reaction with the Cl 2 ˙– radical anion. The iodine containing product of this reaction is expected to be ICl 2 – , which will have implications for the transport of fission-product iodine in MSR technologies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Bubble Mass Transport Measurement in the Large-Scale Test Loops at Oak Ridge National Laboratory

Molten salts are complex fluids that incorporate multi-phase behavior depending on the chemistry and the physical properties of the entrained components. These components include the carrier salt, the actinide fuel, and fission, activation, and corrosion products, the concentrations of which depends on the burnup history of the salt. Radionuclide transport from the salt into the cover gas / off-gas system depends on volatility as predicted by thermochemistry, but data from the Molten Salt Reactor Experiment (MSRE) conducted in the late 1960s suggest that bubble formation and transport are also important. Anomalously high fractions of noble metals were found in the off-gas system and were attributed to transportation with parent salt aerosols and their association with rising noble gas bubbles. The prediction of such phenomena requires coupled neutronic, thermal hydraulic, and chemical equilibrium calculations, the framework of which is being developed within the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program supported by the US Department of Energy (DOE) Office of Nuclear Energy (NE). However, separate effects tests and models of experiments using tools such as SAM and Thermochimica can guide model developers through important processes. Conversely, model development guides the choice of experiments and systems to provide data that are relevant for validation. This report describes several experiments that tracked gas transport in molten salts, ranging from small-scale systems to large-scale loops. Gas transportation in a molten salt, LiCl-KCl, has been studied using the shadowgraph technique. Sensors such as residual gas analysis, Raman spectroscopy, and laser-induced breakdown spectroscopy have been tested for off-gas measurements. These data were used to interpret how the gases move through the upstream salt / cover gas and the interface between them. Differential pressure measurements were able to detect individual gas bubbles as they popped at the liquid–gas interface. Salt aerosols were collected on a cascade impactor. Their formation was also observed directly via the shadowgraph method, and most of these aerosols were launched ballistically into the cover gas. Fine mists could also be observed. Convection currents through the salt were visualized and can be used to calculate the thermophysical properties of the salt itself. The apparatuses described in this report and in a previous work (McFarlane et al. 2023) have been commissioned and are available for use in making further measurements of salt/surrogate fission product behavior. Novel approaches using neutron imaging are planned for the study of fluoride salts, which cannot be contained in quartz, so shadowgraph visualization is not available. Bubble transport in convective flow and in a slow-moving salt column are planned. The mobile laser-induced breakdown spectroscopy (LIBS) system is available for several applications, including iodine capture in a molten hydroxide scrubber, H2 transport though molten salts to complement Raman analysis, and online tracking of salt aerosol generation, transport, and deposition. This report summarizes the findings from FY24 and the plans for FY25. The work completes milestone M2AT-24OR0702013 of the DOE-NE Advanced Reactor Technology, Molten Salt Reactor Campaign, DOE-NE-5.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2026

BISON analyses of TRISO fuel performance, its dependence on time-at-temperature, and possible implications for fuel design and qualification

The Advanced Gas Reactor Fuel Development and Qualification (AGR) program has established a substantial technical foundation to support private entry into the U.S. high-temperature gas-cooled reactor market. However, emerging tristructural isotropic (TRISO)-fueled reactor applications include small modular reactors and microreactors with longer fuel residence times, which may expose fuels to higher time-at-temperature (TAT) values than were explored by the AGR program. Increased TAT could affect diffusive and thermomechanical behaviors such as Pd penetration, fission gas release, creep, and fission product transport. In this work, we applied multiscale best-estimate BISON fuel performance modeling to assess these effects within a representative design space based on the AGR-5/6/7 experiment and analyzed trends in predicted particle and compact fuel performance metrics with possible implications for near-term fuel design and qualification. BISON unambiguously predicted that TRISO fuel performance is sensitive to TAT. Increasing TAT was not predicted to increase the magnitude of failure-inducing tangential stresses in particle coating layers. Predictions obtained using a mechanistic model for Pd penetration indicated that penetration depth does not depend strongly on TAT. While these observations suggest that AGR testing provides a conservative upper bound for the steady-state operation of TRISO particles at lower powers and higher residence times, BISON also predicted that the release of poorly retained Ag would increase with TAT. Because these analyses applied models to extrapolate beyond the available experimental data, the authors recommend performing targeted experiments to confirm these predictions. Nevertheless, these predictions may provide reactor developers with enough confidence to make near-term design decisions associated with the potential fuel performance trade-offs of increasing TAT.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Report to NCSP on 2008 DANCE measurements of 233 U($\eta$,$\gamma$)

Uranium-233 plays an important role in the Th-U fuel cycle, with substantial production in the cycle. This cycle has been proposed as an alternative to the U-Pu fuel cycle due to its reduced production of transuranic elements. An accurate measurement of the 233 U($\eta$,$\gamma$) cross section is required by the National Criticality Safety Program (NCSP) to complete the neutron-induced cross section data, where experimental capture cross section data are scarce and were measured decades ago. The most recent capture cross section data available in the literature were measured in 2007 at the n_TOF facility (CERN); in the 60s measurements were performed at Rensselaer Polytechnic Institute (RPI) and at LANL. Finally, as reported by ORNL, a new evaluation with a revised (renormalized) fission cross section is needed on 233 U. The challenge for this measurement lies in the difficulty of measuring the capture cross section data in the competing fission background, as the fission cross section is around one order of magnitude larger than the capture cross section for 233 U. The accuracy of a capture cross section measurement depends on discrimination between $\gamma$’s produced in capture and fission reactions, for which an experimental setup combining capture and fission detectors is needed. For the ($\eta$,$\gamma$) cross section measurement at LANSCE, this discrimination is achieved by combining the Detector for Advanced Neutron Capture Experiments (DANCE), to measure $\gamma$’s from capture reactions, with a Parallel Plate Avalanche Counter (PPAC) to tag the $\gamma$’s produced by fission. This method was successfully used to measure 235 U and 239 Pu capture cross sections. In these measurements, the neutron capture cross section was determined in a large fission background well above 100 keV. As part of the NCSP nuclear data effort, we have looked at past DANCE measurements on 233 U($\eta$,$\gamma$) and evaluated whether existing data is adequate to apply this technique.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Updates and Validation for the n+ 63,65 Cu Cross Sections [Abstract]

The neutron induced total, elastic, and capture cross sections of 63,65 Cu isotopes were selected for evaluation in the resolved and unresolved resonance energy ranges by the National Criticality Safety Program to resolve discrepancies related to benchmark performance. This is especially evident for the series of ZEUS benchmarks in which copper is used as a reflector. Because copper is also used as structural material in both fission and fusion reactors, the need to address benchmark discrepancies linked to nuclear data deficiencies is a task of primary importance. The aim of this work is to describe the steps of evaluation work towards a consistent improvement of the benchmark performance. The R-matrix analysis with the SAMMY code focused on the 63 Cu(n,γ) reaction channel between 100-300 keV coupled to unresolved resonance region parameters up to 650 keV to fit average cross section data from a recent experiment. Due to the high sensitivity of many benchmarks to elastic scattering angular distribution data, especially for the 65 Cu isotope, the impact of these data was tested by generating Legendre coefficients from both resonance parameters and the Hauser-Feshbach model. Guided by the findings of Shaw et al., the performance of the current evaluation for 65 Cu was compared to that of ENDF/B-VII.1 and ENDF/B-VIII.0 by testing the reactivity coefficients corresponding to the validation suite of experimental criticality benchmarks for thermal, intermediate, and fast systems taken from the International Criticality Safety Benchmark Experiments Project Handbook. The benchmark performance is especially sensitive to 63 Cu(n,γ) and 65 Cu elastic scattering for neutron energies in the 100–500 keV region, whereas 100 keV is the upper limit of the resolved resonance region in the ENDF/B-VIII.0 evaluations for 63,65 Cu. The results highlight the need to handle the transition from the resolved resonance region to the high energy region carefully.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2025

In Situ Spectroscopic Monitoring of MSR Molten Salt and Off-Gas Systems

A significant challenge that must be overcome before commercialization of molten salt reactors is tracking special nuclear material (SNM) through the reactor and subsystems such as fuel chemical processing and off-gas systems. In recent years, several approaches have been explored to track SNM, fission products, and corrosion products in these different subsystems. One such approach is to employ laser and optical spectroscopy to measure the atomic and molecular signals of MSR salts. The advantages of these approaches are that they typically are non-intrusive and offer the capability of process monitoring while still providing low uncertainties. At the Idaho National Laboratory, spectroscopy approaches such as laser-induced breakdown spectroscopy (LIBS) and ultraviolet-visible (UV-Vis) spectroscopy have been utilized to investigate molten salts in an aerosol (LiCl, KCl, RbCl2, NdCl3, and PrCl3) and vapor phases (MgCl5, NdCl5, and ZrCl4) with success. Testing to date has yielded qualitative information on all the above species and quantitative data and analytical figures of merit for species in the vapor phases. These findings, including results from ongoing testing, as well as the experimental conditions and potential applications will be presented.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗
DOE OSTI2025

Multimetallic Layered Composites (MMLCs) for Rapid, Economical Advanced Reactor Deployment (Final Report)

This project focused on the development of multi-metallic layered composites (MMLCs) for advanced fission reactor technologies. There are many instances where one alloy or material simply cannot meet all the demands thrown at it by a reactor system, or cannot allow it to perform as strongly as one would like. Instead of focusing all our effort on developing one perfect alloy, we seek to leverage the design principle of “separation of functionality,” used in many other arenas in design, to boost performance beyond single alloys alone. One illustrative example shows the power of this approach for molten salt-cooled reactors: A three meter tall, three meter diameter reactor vessel made of Incoloy 800 was quoted at $\$$500k in 2018. A Hastelloy N vessel was quoted at $\$$5M. An MMLC vessel, in which a layer of Hastelloy N would be weld-overlaid onto Incoloy 800, was quoted at $\$$700k, and it would achieve the same performance. The potential economic gains of leveraging this approach are therefore substantial. At a minimum, each MMLC would contain one core structural layer and one coolant-facing corrosion-resistant layer. Sometimes, MMLCs required buffer layers, as the structural and corrosion-resistant layers were metallurgically incompatible. In other words, they didn’t always play nice, thus separating layers compatible with both functioned as intermediaries to keep the composite together. However, in doing so we inevitably produce new interfaces, where new issues can arise. Therefore, this project focused on what happens at these interfaces from a combination of high temperatures, irradiation, corrosion, and time. After all, a reactor makes money when it is operating, and outages of any kind erode its economic viability. First, we set out to experimentally prove that MMLCs for at least two advanced reactor systems can be made, today, in US domestic facilities. In this respect we were successful – one MMLC (a Ni-201/Incoloy 800H composite) was successfully made and drawn into two-inch coolant piping. Others were attempted, though new issues relating to cracking in vanadium layers for one and radiation damage performance of the corrosion-resistant layer in another prevented us from moving further in those specific arenas – these are engineering problems which deserve continued focus after this project. Additional experimental work focused on long-term corrosion testing of the outermost layers of the salt-cooled and liquid lead-cooled MMLC concepts, which would then be fed into predictions of how long the MMLCs could last. Next, computational (thermodynamics and atomistic) simulation studies studied how much we expect the interfaces to “blend,” due to the mixing action of neutron irradiation. This eats into both the margin for the structural layer of each MMLC, as dilution from the corrosion-resistant layer into the structural layer would decrease the total load-bearing capacity of an MMLC of finite size. On the other hand, dilution of the corrosion-resistant layer into the structural layer further reduced the margin of corrodible material, reducing the lifetime of the MMLC or necessitating extra thickness to be imparted to the MMLC to meet its functional requirements. Work here focused on irradiation-induced segregation to predict new phases which may embrittle the MMLCs, as well as quantifying irradiation-induced mixing at each interface. The results showed that mixing is expected, but it is both steady and therefore predictable, and not lifetime-limiting for most MMLC concepts – it simply has to be accounted for in calculations of reactor performance when utilizing an MMLC. Then, full-core simulations using the experimentally-derived corrosion data, the computationally discovered irradiation-induced mixing data (partially validated by experiment), and existing, benchmarked core designs for large and small sized reactor concepts (one salt-cooled, one lead-cooled) were conducted to quantify any expansion of reactor operating envelopes achieved by utilizing these MMLCs. This new framework, called REX (Reactor Envelope Expansion), incorporates a combination of core neutronics, thermal hydraulics, and the material performance data derived from this project to see how using an MMLC expands advanced fission reactor operating envelopes. It was discovered that in some cases, MMLC utilization does indeed increase the maximum operating temperatures and cycle lengths of reactor concepts, while in other cases it does not. Finally, our tech-to-market (T2M) strategy was not necessarily to create specific embodiments of MMLCs for immediate sale (because getting into the nuclear market is incredibly slow and laden with regulation, this is a long-term goal), but rather immediate stimulation of US industry using the design approach of MMLCs derived from this project. In this respect we were successful, as one of the PhD students funded on this project co-founded Allium Engineering, Inc., which created a stainless steel / low-alloy steel MMLC to function as chloride corrosion-resistant rebar for embedding into concrete structures. Allium Engineering continues to be successful, having recently opened their first factory as of this writing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Second Report of the Nuclear Data Subcommittee of the Nuclear Science Advisory Committee

The central importance of the nuclear data curated by the US Nuclear Data Program (USNDP) for clean energy generation, national security, nonproliferation, medical applications, and space exploration as well as basic science was described in a prior report issued by the DOE/NSF Nuclear Science Advisory Committee subcommittee on Nuclear Data (NSAC-ND) in September 2022. In this report, we present a set of fourteen (14) recommendations that will enhance and advance DOE-NP's stewardship of nuclear data. The first three recommendations focus on the existing core USNDP capabilities, namely: 1) Support the nuclear structure evaluation workforce to improve the currency, consistency, and accessibility of the Evaluated Nuclear Structure Data File (ENSDF); 2) Enhance nuclear reaction evaluation within the USNDP in support of the Evaluated Nuclear Data File (ENDF) through expansion of the workforce and integration of high-performance computing, automation, and machine learning and; 3) Continue atomic mass evaluation in support AME and NUBASE databases. This is followed by eight (8) recommendations representing new cross-cutting initiatives involving both measurement and evaluation to address outstanding nuclear data needs. These new initiatives require a highly trained, diverse workforce that includes personnel with expertise from both inside and outside the nuclear physics community from which evaluators have traditionally been recruited. As such, many of these initiatives are accomplished via a Topical Nuclear Data Collaborations (TNDC). A TNDC is made up of domestic and international stakeholders, subject matter and nuclear data experts, and nuclear data evaluators and features a workforce development plan to ensure that nuclear data evaluators maintain currency in the relevant applications and are seen as equity partners in the endeavor. These include: 1) Establish a coordinated effort to improve evaluation and modeling in nuclear astrophysics for stellar dynamics, multi-messenger astronomy and nucleosynthesis; 2) Initiate a TNDC to develop and maintain nuclear structure evaluation beyond discrete states, including nuclear level densities, photon strength functions and photonuclear data for improved reaction modeling, and exploring nuclear structure at finite temperature; 3) Create a TNDC to perform correlated fission data evaluation, including cross sections, fragment yields, v(A), v(E n ) for nuclear energy, national security, nonproliferation and basic science; 4) From a panel of subject matter experts to establish and annually update a roster of key decay data to nurture its accelerated dissemination including both measurement and evaluation for targeted high-value nuclides for national security, nonproliferation and medical applications; 5) Comprehensive, consistent neutron-induced structure and reaction data for nuclear energy, national security, nonproliferation and planetary nuclear spectroscopy; 6) Charged-particle stopping powers for detector design, space effects and ion beam therapy; 7) High-energy reactions for space exploration and medical nuclide production, and; 8) The creation of an infrastructure for open data and data preservation for use by the entire nuclear physics community. All told, these initiatives require approximately $6.5M increase in NP support of the USNDP in fiscal year 2023 dollars and would require at least 3-5 years to carry out due to the length of time needed to recruit and train new nuclear data researchers. This relatively modest investment would help ensure that the fruits of the nuclear data research carried out by DOE-NP and its collaborators would be brought to bear to address some of the most important needs of our nation and the world. To ensure effective execution of this plan, we present an overview of recruitment, training, and retention goals for the USNDP, the centerpiece of which is a mutually agreed upon code of conduct. Finally, we identify the facility and instrumentation needed to perform the recommended experimental activities. This includes a short review of target fabrication capabilities, reactors, neutron beam, light- and heavy-stable ion, gamma-ray, high-energy and radioactive ion beam facilities. Lastly, a more complete appendix of experimental facilities previously compiled is included with new input provided for 6 facilities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Investigation of neutron noise in a micro-scale, natural circulation molten salt fission battery system

The Molten Salt Reactor (MSR) concept is a rapidly evolving Generation IV design that has recently attracted favorable attention due to the potential for reducing waste generation, realizing passive safety features, and seizing on the opportunity for cost effective economics. A specific novel micro-MSR, natural circulation, battery design concept involves placing all primary components within a single reactor vessel containment without the need of primary forced pumping. This small modular, integral design presents potential cost savings while producing safety, reliable, and transportable carbon-free power for decades. This investigation evaluates the neutron noise induced by density and flow fluctuations in a natural circulation MSR battery concept being developed at the University of Idaho. This study finds numerical solutions to the one-dimensional, one-group, coupled diffusion equations for a bare, homogeneous core, and evaluates neutron flux and delayed neutron precursor concentration noise due to core flow and fuel salt density perturbation sources. Noise analysis shows both point kinetic and space-dependent behavior is present despite the small size, low-flow, closely-coupled nature of the natural circulation MSR concept. Analysis shows that the low flow of the convective system results in noise behavior typically representative of a larger forced-circulation MSR system. Finally, noise techniques may also be useful in MSR core diagnostics as a non-invasive, low-cost radiological option to traditional monitoring schemes.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Evaluation of Irradiation Creep Effects in HT9 Cladding for FAST Experiments

The push for advanced reactor fuels for improved reactor safety and efficiency had led to a renewed interest in metallic fuel for nuclear reactor applications. Experimental investigation is necessary to ensure a robust understanding of the thermomechanical properties of new metallic fuel designs. Unfortunately, with the current experimental facilities, thoroughly investigating the responses of metallic fuel burnup would take a prohibitively long time. To alleviate this, the Fission Accelerated Steady State Test (FAST) was developed to accelerate the irradiation testing while simultaneously decreasing the sensitivity to fabrication tolerances by reducing the fuel diameter and scaling the experiment. This method successfully scales the radiation effects on the fuel, but the HT9 cladding is not exposed to prototypic radiation conditions. This raises questions on whether the FAST experiment results are truly indicative of the HT9 cladding performance due to radiation induced creep effects not being appropriately accounted for. Using BISON fuel performance code, the simulated FAST cladding strain is compared to simulated EBR-II cladding strain. This is done through a sensitivity study of input parameters and scaling of neutron fluence on the cladding. This allows a parametric comparison of physical phenomena on the effective difference between cladding strains between FAST and equivalent burnup EBR-II fuel pins. The results show that the irradiation induced deformation (creep or swelling) is insignificant compared to the thermal-mechanical deformation. Therefore, the difference between the FAST experiment cladding and the EBR-II experiment cladding is negligible and comparison of fuel system performance between the two experiments is appropriate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Coupled physics simulation of fracture in nuclear fuel pellets induced by resistive heating

While it is well known that the UO 2 fuel used in light-water reactors cracks early in its life in the reactor, it is very difficult to collect in-reactor data regarding fuel cracking initiation and propagation to validate fracture models in fuel performance codes. Most fracture data comes from the post-irradiation examination of fuel that has been subjected to long and complex power histories. Replicating the thermal gradients experienced in this fuel to study crack initiation and propagation in a laboratory environment is challenging. This is primarily because the fuel is heated volumetrically by fission, which is difficult to replicate. One way to approximate this volumetric heating out of the reactor is to use electrical resistance (or Joule heating). An electrical conductivity model has been developed and coupled with the existing thermomechanical modeling capability in the BISON nuclear fuel performance code. This will permit simulation of experiments that use resistive heating for the purpose of validating fracture models in BISON. The modeling approach developed here is applied to simulate both historical and current resistive heating experiments on ceramic nuclear fuel.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Vacancy-driven variations in the phonon density of states of fast neutron irradiated nuclear graphite

Research examining radiation damage and its effects in graphite began in the 1940’s during the development of moderated nuclear reactors. Interest in this topic is expanding because of emerging applications associated with fullerenes and carbon nanostructures as well as its long-standing use as a fission moderator. In this work, we report the measurements of the full phonon density of states of irradiated nuclear graphite using inelastic neutron scattering experiments at room temperature. The samples were previously exposed to different levels of neutron doses and irradiation temperatures. The phonon density of states of perfect and defected graphite supercells including different configurations of vacancies and interstitials were calculated using first-principles direct method. Despite high neutron irradiation doses, the scattering measurements show that the induced damage is localized, and the layered structure is preserved. In conclusion, a comparison of the measured phonon densities of states of irradiated samples with those calculated of defected supercells indicates that the main changes observed are mainly attributed to formation of vacancies.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Thermal conductivity degradation due to radiation-induced amorphization in U 3 Si 2 : A pilot study

Here, in this study, we investigate the thermal conductivity of U 3 Si 2 amorphized by ion irradiation using 84 MeV 136 Xe ions at 190 °C. The suspended-bridge method was utilized to measure the thermal conductivity, allowing for a detailed analysis of the specimen while minimizing interference from other crystalline phases. Our results indicate that the thermal conductivity of amorphous U 3 Si 2 is significantly lower than that of unirradiated crystalline U 3 Si 2 . These findings are consistent with recent studies on in-pile-irradiated U 3 Si 2 samples that consider the effects of U 3 Si 2 amorphization, fission gas bubbles, and other impurities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Qualitative and quantitative analysis of neutron irradiation effects in SiC/SiC composites using X-ray computed tomography

Silicon carbide fiber-reinforced silicon carbide matrix (SiC/SiC) composites are candidate materials for cladding of light water reactor (LWR) fuels. Loss of fission product gas retention due to the formation of microcrack networks is considered a potential failure mechanism for SiC/SiC-cladded fuels. In this work, a variety of SiC/SiC composite tubes were irradiated with and without an LWR-relevant radial heat flux in the High Flux Isotope Reactor, followed by detailed characterization with X-ray computed tomography (XCT). This first set of XCT data for neutron-irradiated samples confirmed that the internal stresses arising from a combination of temperature gradients and irradiation-induced swelling act as the primary driver for cracking. Consequently, while the observed cracking patterns varied depending on the tube architectures, the sharp edges of relatively large pores were found to be the common stress concentrator. These findings are useful to help improve the design and manufacturing of SiC/SiC fuel claddings for reduced failure probability.

42 ENGINEERING↗
DOE OSTI2020

Summary of the Postirradiation Examination of the First Samples from a MiniFuel Irradiation

An overview of postirradiation examination results for uranium nitride kernels and uranium nitride coated particles irradiated in the High Flux Isotope Reactor are presented. This is the first postirradiation examination of the MiniFuel irradiation vehicle that was recently developed to rapidly screen different nuclear fuel concepts. Observations on fission gas release, irradiation conditions and microstructure of the irradiated fuel show good fuel performance at the low burnup achieved in this initial irradiation. The burnup measured by mass spectrometry ranged from 5.9 to 10 MWd/kgU as was achieved after only 68 effective full power days of irradiation. Results from silicon carbide thermometry measurements further benchmarked the MiniFuel irradiation vehicle and indicated fuel was irradiated at temperatures ranging from 410-460°C. Extensive microstructural characterization on the irradiated fuel was performed and no significant irradiation induced changes were observed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

AGR-3/4 TRISO Fuel Compact Ceramography

The combined third and fourth irradiation in the Advanced Gas Reactor (AGR) program (AGR-3/4) contained tristructural isotropic (TRISO)-coated particle fuel and designed-to-fail (DTF) fuel particles. The DTF particles were only coated with highly anisotropic pyrocarbon (PyC) so they would purposely fail during the AGR-3/4 irradiation and provide a source of fission products for measurement. To observe the post-irradiation morphology of these DTF particles and the TRISO-coated particles, three AGR-3/4 compacts were mounted in epoxy, sectioned above their centerlines, and ground/polished. Three rounds of grinding/polishing and optical microscopy were performed so that the particles could be observed at multiple planes. Each compact contained approximately 1,872 TRISO particles and exactly 20 DTF particles. The three AGR-3/4 compacts examined covered a wide temperature range and featured both the hottest average irradiation temperature (1375°C) and the coldest/lowest burnup (872°C and 5.5% fissions per initial metal atom) of any compacts to undergo post-irradiation examination (PIE) in the AGR program to date. A total of 29 DTF particles were located and observed via microscopy across the three compacts. All the DTF particles observed via microscopy had completely failed PyC coatings. Some different DTF kernel and PyC morphologies were observed that have been attributed to the differences in irradiation temperature and/or burnup. At low and medium irradiation temperatures (roughly 850 to 1050°C), it appears irradiation-induced dimensional changes in the DTF PyC caused it to fracture and fold in on itself, and the kernel deformed to accommodate this PyC deformation. The extent of DTF kernel deformation to accommodate DTF PyC buckling tended to be greater for the medium-temperature fuel compared to the cold fuel. In the high-irradiation-temperature compact (1375°C), the DTF PyC layer appears to have completely reacted chemically with the kernel material. The only material surrounding the DTF particles in this hot compact resembles the compact matrix material. Observations of the TRISO-coated driver fuel particles and fuel compact graphitic matrix were also made. The TRISO particle kernels in the medium-temperature compact (1047°C), and many in the high-temperature compact (1375°C), showed morphologies consistent with what was seen in AGR-1 and AGR-2. In other TRISO particles from the high-temperature compact, a spatial gradient in the kernel appearance was evident. Here the cool side of the kernel (away from the center of the compact) had a much darker appearance (like that of the buffer and pyrocarbon). This is the first observation of this kind of kernel spatial gradient in AGR fuel. It is believed that the high irradiation temperature of that compact (an average of 1375°C) activates or accelerates an unidentified chemical reaction, and the temperature gradient within the fuel causes a sharp spatial gradient. The low-temperature/low-burnup compact also showed unique kernel morphologies where the TRISO-coated particles had clearly distinguishable oxide and carbide phases at the center of the kernel, an oxide rind surrounding this, and remnants of a carbide skin surrounding the oxide rind. These are features observed in the as-fabricated fuel that are no longer present in higher burnup fuel. Occasional gaps between the outer pyrolytic carbon (OPyC) and graphitic matrix material were observed in all compacts. Gaps were most often found in the small, matrix-filled spaces between adjacent particles. Finally, buffer morphologies in AGR-3/4 TRISO particles were like those observed in AGR-1 and AGR-2, and the buffer fracture frequencies in AGR-3/4 and AGR-2 TRISO particles were plotted versus fast neutron fluence and irradiation temperature. In AGR-3/4 the buffer fracture rate was highest (23%) for an irradiation temperature of 1047°C and a fast fluence of 5.18E25 n/m 2 . Increasing the irradiation temperature to 1375°C reduced the buffer fracture rate to 14%. Reducing the irradiation temperature to 872°C and the fast fluence by a factor of 3 reduced the buffer fracture rate to 7%. The temperature and fluence dependencies observed for AGR-3/4 buffer fracture were consistent with those observed in AGR-2. Lower fluences and/or higher temperatures significantly reduced the buffer fracture frequencies. Lower buffer fracture frequencies were also observed at lower temperatures as long as the fluence was also significantly reduced. This is believed to be due to lower fluence resulting in less irradiation-induced dimensional change (shrinkage) of the buffer, and a higher temperature promoting enhanced creep relaxation of stresses within the buffer, leading to less buffer fracture.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

ORNL Neutron Cross Section Measurements of 90 Zr

Nuclear criticality modeling and simulations rely on the quality of the existing evaluated nuclear data libraries such as Evaluated Nuclear Data File (ENDF)/B, the Joint Evaluated Fission and Fusion (JEFF) nuclear data library, or the Japanese Evaluated Nuclear Data Library (JENDL). In some cases, the cross-section evaluations of those libraries were found to be deficient in describing criticality benchmarks accurately. More than two decades ago, the US Nuclear Criticality Safety Program (NCSP) established a Nuclear Data (ND) task which encompassed experiments and evaluations. In response to this, the Oak Ridge National Laboratory (ORNL) formed a Nuclear Criticality and Data group which performed ND experiments, data analysis, and evaluations to produce ENDF files for the ND libraries as identified in the NCSP Five-Year Plan. Before being submitted to the ENDF library, files were processed and tested for performance by running benchmark calculations. This procedure was centralized in the ORNL group and is now often referred to as the ND pipeline. NCSP collaborates with the Joint Research Center (JRC) of the European Commission in Geel, Belgium, to perform high-resolution neutron-induced cross section measurements at the Geel Linear Accelerator (GELINA). The objective is to address emerging ND problems in criticality calculations. Difficulties with ND include insufficient neutron energy range, missing covariances, and previously unrecognized inaccuracies with experiments. New neutron total and capture cross sections of 90 Zr in the neutron energy range from 100 eV to several hundred keV were recently performed. These measured data will be used, together with existing high-resolution transmission data from a metallic 90 Zr sample, to improve representation of the cross sections.

97 MATHEMATICS AND COMPUTING↗