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Comparison of fluence-rate determination techniques for the Advanced Test Reactor-Critical Facility

A technique using small, enriched uranium-aluminum alloy monitors to measure fission rates in fuel plate assembly reactors was developed at the Idaho National Laboratory Radiation Measurements Laboratory in support of Advanced Test Reactor Critical (ATR-C) Facility irradiations. Previous measurements were performed to determine the correlation between the beta-particle activity and the fission rate in the U-Al monitors following irradiation. The American Society for Testing and Materials (ASTM) has established a standard practice E704 for determining neutron fluence rate by radioactivation of depleted uranium by measuring the concentration of fission-products in irradiated uranium monitors. Rather than measuring the beta-particle decay from fission-products, the decay rate of fission-products is determined by gamma-ray spectroscopy. The feasibility of using a method adapted from the ASTM standard practice E704 was investigated for ATR-C irradiations and compared to the present method by analyzing a subset of 21 monitor wires using both methods. The resulting calculated fission rates agreed with an average standard deviation of 7.45%, within the average combined measurement error of 9.05%. Practical considerations such as expected fluence-rates, sample activity, and counting-time were compared between the two methods and the sources of error for each method were investigated. Quality assurance measurements utilizing the modified ASTM standard method are recommended for future test irradiation, but gross-beta-particle counting remains the most practical solution for ATR-C fluence-rate determination.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Versatile Test Reactor Conceptual Core Design

The VTR is a 300-MW(thermal) sodium-cooled fast reactor (SFR) designed for the specific purpose of delivering unique testing capabilities to enable the advancement of all reactor technologies. With its flux level, irradiation volume, and operational flexibility, the VTR will enable accelerated testing of materials, fuels, and various components needing irradiation testing. Proven SFR technologies and design approaches have been leveraged in designing the VTR core, ensuring the highest possible readiness level. This resulted in the VTR using ternary metallic fuel and delivering fast flux levels in excess of 4 x 10 15 n/cm 2 ∙ s over large useful volumes, corresponding to about 60 dpa/year in steel. As part of the design efforts, the VTR core performance has been determined for a representative configuration, ensuring that the reactivity control systems offer sufficient shutdown margins, that the core can be safely cooled in all situations, and that reactivity feedback coefficients are conducive to a favorable safety behavior. Furthermore, the incorporation of features such as fuel assembly storage in the shield region supports the flexible and reliable operation of the VTR. Additional design work has been ongoing as well. This includes thorough shielding performance evaluations to ensure safe operation of the VTR, verification and validation of the design tools used to achieve compliance with Nuclear Quality Assurance (NQA-1) requirements, early assessment of the impact of irradiation experiments on the core performance envelope and associated margins, and in-depth uncertainty quantification efforts to quantify the anticipated range of performance characteristics. An experimental program supporting the VTR core design has been set up, with the current focus being on thermal-hydraulic experiments. The purpose of this experimental program is to obtain confirmatory measurements to serve directly as part of the core design basis or as part of the validation cases supporting the simulation tools used.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Destructive PIE and Safety Testing of Six AGR-5/6/7 Capsule 2 Compacts

This study evaluates fission product retention and particle failure mechanisms in AGR-5/6/7 Capsule 2 uranium carbide and uranium oxide (UCO) tristructural isotropic (TRISO) fuel under high-temperature gas reactor accident-relevant conditions using high-temperature safety tests and destructive post-irradiation examination. Three Capsule 2 compacts were held isothermally at 1600°C for approximately 300 hours and one compact at 1800°C for approximately 300 hours; two additional compacts were examined in the as-irradiated state. Post-test deconsolidation–leach–burn–leach (DLBL) quantified nuclide inventories in matrix and particles. Individual particles were surveyed for radioisotope inventories, and microanalytical approaches resolved microstructural evolution and fission product distributions within the coating layers. At 1600°C, no krypton was detected above the minimum detectable limit, and cesium releases were far below a single particle equivalent, indicating the absence of full TRISO failure or SiC failures. Silver releases were limited and primarily reflected depleted post-irradiation inventories, consistent with prior compact-level exams indicating substantial in-pile 110m Ag loss. At 1800°C, cumulative 134 Cs release of approximately 2.5 particle equivalents and delayed 85 Kr totaling approximately 0.53 particle equivalents were consistent with one full TRISO failure and two SiC failures. Europium and strontium releases were roughly one order of magnitude higher than at 1600°C and comparable to AGR-1/AGR-2 high-temperature tests, with sustained late-hold rates indicating diffusion through intact coatings coupled with matrix depletion. Overall, AGR-5/6/7 Capsule 2 UCO fuel demonstrated fission product retention during safety testing consistent with prior AGR campaigns, while distinctive in-pile 110m Ag depletion and measurable 1600°C europium loss motivate targeted follow-on studies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

FITT OXIDATION TEST PLAN

This plan describes the post irradiation examination (PIE) oxidation testing activities to be performed by Oak Ridge National Laboratory (ORNL) on individual particles from Compact 5 4 2 taken from the Advanced Gas Reactor (AGR) experiment, AGR 2. This work will be performed in accordance with the general objectives outlined in the AGR 2 PIE Plan1 and guidance in the ORNL PIE Statement of Work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

FITT OXIDATION TEST PLAN

This plan describes the post irradiation examination (PIE) oxidation testing activities to be performed by Oak Ridge National Laboratory (ORNL) on individual particles from Compact 5 4 2 taken from the Advanced Gas Reactor (AGR) experiment, AGR 2. This work will be performed in accordance with the general objectives outlined in the AGR 2 PIE Plan1 and guidance in the ORNL PIE Statement of Work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Strength and rupture geometry of un-irradiated C26M FeCrAl under LOCA burst testing conditions

Ferritic iron-chromium-aluminum (FeCrAl) alloys are an accident tolerant fuel candidate to replace the incumbent Zr-based claddings. Nuclear grade FeCrAl alloys are marked by superior high temperature mechanical behavior and exceptional steam oxidation resistance, both of which increase safety margins during accident scenarios. In the present study, the loss of coolant accident (LOCA) burst behaviors of three un-irradiated commercially fabricated cladding materials in a simulated LOCA environment were compared: (1) T35Y2, a 1 st generation nuclear grade FeCrAl, (2) C26M, a 2 nd generation nuclear grade FeCrAl, and (3) Zircaloy-2. Both FeCrAl alloys showed improved mechanical strength and steam oxidation resistance compared to Zircaloy-2. C26M claddings burst at significantly higher temperatures for all tested engineering hoop stresses, had limited ballooning, and demonstrated preferential fuel retention behavior in terms of burst opening area and length. High temperature tensile data for C26M is also presented. For both un-irradiated FeCrAl alloys, it was found that a distinct “threshold” burst stress signified the transition between small and large openings. Finally, higher threshold hoop stresses were associated with higher uniaxial strength for the FeCrAl alloys, indicating that tensile data, rather than creep data, could be useful for predicting rupture size and assessing fuel dispersal concerns.

36 MATERIALS SCIENCE↗

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.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

BRR Cask Use for Pu-238 Isotope Production

The Department of Energy (DOE), in partnership with its national laboratories and the National Aeronautics and Space Administration (NASA), is responsible to produce Pu-238 isotope in the United States for use in space exploration. Major activities in the DOE complex are focused at Idaho National Laboratory (INL) and Oak Ridge National Laboratory (ORNL). INL is responsible for storing Np-237 feedstock, irradiation qualification in the Advanced Test Reactor (ATR), and irradiating targets containing Np-237 to produce Pu-238. ORNL is responsible for target design, target fabrication, irradiation qualification in HFIR, and processing of targets to extract Pu-238 heat source material. A key part of the program lifecycle is moving irradiated targets from INL to ORNL. The BEA Research Reactor (BRR) cask was identified as a potential shipping cask for the transport of both unirradiated and irradiated targets between the project sites. This paper will discuss the production at INL and shipment of Pu-238 to ORNL using the BRR cask.

07 ISOTOPE AND RADIATION SOURCES↗

Fuel Specification for Uranium Monocarbide FAST Fuel Specimens

This specification outlines the fabrication requirements for kernel compact uranium monocarbide (UC) fuel to be fabricated at General Atomics (GA) and is already issued in EDMS and is going thru LRS so that it can be shared with the Vendor. The UC fuel will be irradiated in the Advanced Test Reactor (ATR) using the Irradiation System for High-Throughput Acquisition (ISHA-1). The primary objective of the ISHA-1 capsule design is to deliver to Idaho National Lab (INL) a semi-universal drop-in capsule that can facilitate the irradiation of both fissile and structural materials in a variety of ATR positions. This irradiation experiment will support the need for development of Accelerated Fuel Qualification (AFQ) methods.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization of Intrinsic Fiber Optic Temperature Sensors by In-core and Furnace Testing

Increased research and development in nuclear technology has raised the demand for novel sensors and instrumentation to meet data objectives, and survive in different conditions and environments, beyond conventional light water reactor (LWR) environments. Expediting the deployment of advanced nuclear technologies by developing, demonstrating, and qualifying advanced reactor fuel forms necessitates a deeper understanding of how irradiation affects fuels and materials' performance. To achieve a more comprehensive understanding of fuels and materials performance, researchers require more specialized experiments and measurements. The demand for innovative sensors to support nuclear fuel development arises from the complexity of materials' behavior under irradiation and the challenges of deploying instrumentation in Material Test Reactors (MTRs) for irradiation tests. Additionally, measurements of material properties require integrated measurement systems to characterize thermal properties, mechanical properties, chemistry, and microstructure [1]. Among the potential measurement techniques, optical fiber-based sensors have been identified as potential sensors to measure different physical phenomena such as temperature, strain, pressure, and fluid level. Optical fiber sensors have the capability to provide multi-sensing and multiplexing instrumentation, allowing the measurement of different physical parameters within a single sensor configuration, and transmitting data collected at multiple locations through a single fiber. They offer immunity to electromagnetic interference, electrical passivity, compatibility with various sensing methodologies, and cost-effectiveness. Beyond their widespread use in telecommunications, silica fiber-based instruments are utilized in industrial applications, even at temperatures reaching 300?400°C, such as distributed temperature sensing in oil and gas recovery. The Department of Energy (DOE) is interested in using fiber optics to support fuel cycle development [2]. Fiber optics are an excellent candidate for harsh environment sensing, including sensing at very high temperatures (1900oC for sapphire optical fibers). Distributed fiber optic sensing has been deployed in other harsh environments like coal gasification plants [3]. Distributed strain sensing, which operates similarly to distributed temperature sensing, has been deployed to monitor underground mines and fibers have been imbedded in soil to monitor sink-hole development [4][5]. The application of fiber optic sensors to advanced reactor development is a promising area of research.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Irradiation of Mo-100 Targets and Testing Fe(ll)CI 2 Precipitation for Tc-99 Removal

The production of molybdenum-99 (Mo-99) is a critical step in the generation of technetium-99m (Tc-99m), a radioisotope widely used in medical imaging. NorthStar Medical Radioisotopes, LLC is planning to produce the important medical radioisotope Mo-99 through a photonuclear reaction on molybdenum-100 (Mo-100). Accelerator production of Mo-99 using enriched Mo-100 targets yields undesirable isotopes, such as niobium-95 (Nb-95) and zirconium-95 (Zr-95). Previous studies reported that Nb and Zr isotopes can be effectively removed from Mo-99 products through coprecipitation with Fe(III). To enable the potential utilization of the first milking of Tc-99m from a Mo-99/Tc-99m generator, it is desirable to remove long-lived Tc-99. This can be accomplished by substituting Fe(III) with Fe(II) during the precipitation step, without affecting the removal of Zr and Nb isotopes. Previous experiments demonstrated up to 99+% removal of Tc using this method. It was also observed that the presence of hydrogen peroxide significantly impacts Tc removal. This was evident in the processing of enriched Mo-100 targets, where only 25% of Tc was removed. To further investigate this, another irradiation of enriched Mo-100 disks was conducted, followed by Tc-99 removal using Fe(II). Prior to irradiation, experimental conditions for Tc removal were optimized through several test runs using Mo-100 disks spiked with Tc-99. The results of these tests are discussed in this report.

07 ISOTOPE AND RADIATION SOURCES↗

Design and commissioning of an e-beam irradiation beamline at the Upgraded Injector Test Facility at Jefferson Lab

We report the Upgraded Injector Test Facility (UITF) at Jefferson Lab is a continuous-wave superconducting linear accelerator capable of providing an electron beam with energy up to 10 MeV. A beamline for electron-beam irradiation has been designed, installed and successfully commissioned at this facility, aimed at the degradation study of 1,4-dioxane and per- and polyfluoroalkyl substances (PFAS) in wastewater treatment. A solenoid with a peak axial magnetic field of up to 0.28 T and a set of raster coils were used to obtain a Gaussian beam profile with a transverse standard deviation of ~ 15.0 mm at the target location. Monte-Carlo simulations using FLUKA were carried out to calculate the total absorbed dose and the dose distribution in the sample volume inside the target cell. The simulations were benchmarked experimentally by dosimetry mapping using optichromic dosimeters. The results of the irradiation experiments showed a ~ 95% reduction of 1,4-dioxane in ultra-pure water for a dose of 1 kGy, demonstrating the potential of electron-beam irradiation towards addressing growing challenges in environmental remediation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Post-irradiation examination of commercial tantalum alloys following neutron irradiation

Post irradiation examination of two commercial tantalum alloys (based on Ta-8 %W) revealed significant irradiation hardening following neutron irradiation in the High Flux Isotope Reactor at Oak Ridge National Laboratory. Tensile samples of commercial Ta alloys T-111 and ASTAR-811C were irradiated to a total neutron fluence (E > 0.1 MeV) in the range (2–4)x10 21 n/cm 2 (0.39–0.75 dpa) at an irradiation temperature near 900 °C. Tensile testing conducted at room temperature and at 800 °C revealed significant irradiation hardening under all test conditions. Samples that were tensile tested at room temperature exhibited brittle failure, whereas ductility was maintained for elevated temperature testing. The irradiation hardening and embrittlement noted for both alloys was attributed to irradiation-induced dislocation loop formation as confirmed through scanning transmission electron microscopy analysis. Corresponding energy dispersive x-ray spectroscopy revealed radiation-induced segregation of Hf in these loop populations. This Hf enrichment is shown to result in eventual co-precipitation of elongated (Hf,O)-rich precipitates along the dislocation loops. Further, these results show that irradiation hardening is enhanced via irradiation-enhanced precipitation at elevated irradiation temperatures. Consequently, the minimum recommended operating temperature window for Ta alloys should be increased to account for observed hardening/embrittlement at irradiation temperatures as high as 900 °C (1,173 K).

36 MATERIALS SCIENCE↗

Effects of Neutron Irradiation on the Bond Strength of Steel Embedded in Concrete

The structural integrity of the concrete biological shield (CBS) in light water reactors (LWRs) exposed to long-term radiation raises the question of the effects of fast-neutron and gamma irradiation on the bond properties of embedded carbon-steel reinforcement in concrete, which is critical to the transfer of in-service and accidental loads. The design and execution of a first-of-a-kind irradiation experiment conducted in the LVR-15 test reactor (Czech Republic) are presented along with preliminary post-irradiation examination and testing results. Preliminary analysis shows that the fast neutron flux affects the radiation-induced volumetric of concrete aggregate, that the gamma irradiation induces shrinkage of the chemically bonded water in cementitious hydrates and that the bond strength of steel in concrete at the tested irradiation conditions decreases moderately.

Le Pape, Yann↗

Design Report on the MiniFuel Instrumented Test Apparatus for Understanding Radiation Effects

Most nuclear fuels irradiations at Oak Ridge National Laboratory (ORNL) over the past decade have been conducted using MiniFuel—a static capsule design employing subscale fuel specimens to collect separate-effects irradiated fuel performance data. Irradiation conditions for MiniFuel experiments are predicted pre-test using reactor physics, and thermal models are verified post-irradiation via SiC dilatometry and various spectrometry methods. Relevant fuel performance parameters are also observed post-irradiation in a hot cell, thereby providing a single data point for each parameter representing the cumulative effects of the irradiation conditions. Substantially more data can be harvested from a single test and within a shorter duration by instrumenting irradiation vehicles and measuring desired quantities in situ. This report presents the design and analysis of the MiniFuel INstrumented Irradiation Test Apparatus for Understanding Radiation Effects (MINITAURE)—an instrumented test rig based on the separate-effects MiniFuel concept that aims to capture fission gas release (FGR) and thermal conductivity degradation of fuel specimens during irradiation in the High Flux Isotope Reactor (HFIR). MINITAURE will be integrated with the Materials Irradiation Facility (MIF) located in the HFIR building outside the reactor containment. The MIF will act as the instrumentation and control center for the experiment, enabling real-time feedback from in situ sensors and control of irradiation temperatures via a gas delivery system. Two unique capsule designs were developed to capture each phenomenon: the thermal conductivity capsule, which uses a thermopile method to estimate fuel specimen thermal conductivity, and the fission gas release capsule, which will have continuous flowing gas communication to high-purity germanium detectors that are housed in the MIF for monitoring FGR. This report details the reactor physics and heat transfer modeling activities that were used to inform the experiment design and predict capsule performance. It also describes out-of-pile activities conducted to stand up this new capability and verify the measurement techniques. Modeling efforts to date have demonstrated the feasibility of the in situ measurement techniques and supported the development of the MINITAURE assembly configuration. Out-of-pile testing of the thermal conductivity measurement shows promise in capturing relative changes in thermal conductivity. However, significant errors exist in the measured absolute value, posing a need for further refinement.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Status memorandum on ORNL support of vendor irradiation capsule design and ASME irradiation code development and new ASTM test standard development activities

This report is in submission of completion of the Level 4 milestone number M4TG-24OR0501111 within the larger Advanced Reactor Technologies Gas Cooled Reactor program at Oak Ridge National Laboratory (ORNL). The focus of this year’s efforts is to continue support of industry needs related to the development of future industry-funded irradiation programs. At ORNL these efforts included the development of a generalized three-dimensional CAD model of an irradiation creep capsules for graphite, cost estimates of the expansion of the Materials Irradiation Facility (MIF), involvement with ASTM D02.F0 “Manufactured Carbon and Graphite Products” and the ASME Boiler and Pressure Vessel Code, and publication of papers supporting these efforts. This report will document the status of these activities.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Nuclear fuel irradiation testbed for nuclear security applications

The nuclear security community has long been interested in the identification and quantification of nuclear material signatures to understand a material’s provenance, use, and ultimate application. New forensics signatures and methods intended for non-traditional or advanced nuclear fuel applications require fuel irradiation experiments to demonstrate viability and validity. Integral fuel irradiations have historically required significant costs and long timelines to design, irradiate, and characterize. This paper describes how a recently developed nuclear fuel irradiation testbed can be used to provide a low cost, rapid turnaround, modular test environment for irradiation and evaluation of nuclear fuel specimens for nuclear security applications. The irradiation testbed houses six small ‘MiniFuel’ samples within hermetically sealed capsules inside targets that can be removed in between each ∼25-day operating cycle of the High Flux Isotope Reactor (HFIR). As many as nine targets can be irradiated using a single irradiation position (reflector region) in HFIR, allowing for varying irradiation temperatures and burnups. A suite of hot cell capabilities have been established to perform post-irradiation examination for measuring performance (e.g., fuel swelling, fission gas release) and facilitating experiment disassembly for subsequent property measurements, microstructural analysis, or chemical assay. This new testbed allows fuel irradiations to be conducted on an accelerated timeframe to enable rapid proof of concept testing and to provide reference material for nuclear fuel security applications. Recent applications using this testbed include the testing of isotopic taggants in UO 2 fuel (intentional forensics), testing of U-10Mo fuel for down-conversion of highly enriched uranium–fueled reactors, and the production of irradiated UO 2 fuel material for signature analysis of its isotopic composition (plutonium, fission gases, etc.).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

High resolution microstructural, chemical studies and localized burnup analysis in an irradiated U–10Zr metallic fuel

This study involves high resolution characterization of a sodium bonded solid uranium (U)-10 wt% zirconium (Zr) metallic fuel irradiated in Fast Flux Test Facility (FFTF). The fuel centerline temperature during irradiation was estimated to be around 675 °C with the peak burnup 13.1 atomic percent. Samples for transmission electron microscopy (TEM) and atom probe tomography (APT) were prepared from different regions/zones in the fuel cross section radially to elucidate the microstructural changes and chemical redistribution of solute elements as well as fission products during irradiation experiment. TEM results indicate the irradiation in fast flux testing leads to the formation of extensive Zr-rich precipitates with varying sizes in the U–Zr fuel matrix. APT analysis performed to investigate redistribution of Zr, U and fission products along the radial direction of fuel pin showed Zr-rich precipitates entrapping the fission products in higher concentration as compared to the α-U phases. Here, the local burnup ( 235 U depletion) is found to be consistent, calculated by quantification of 235 U, 236 U and 238 U isotopes from mass spectrum obtained from APT along the radial direction. Zr-rich precipitation and its implication on fuel constitutional redistribution are discussed based on SEM, TEM and APT results.

APT↗