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At least 469 records · Page 26

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 1

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore fuel product. The long-term EnCore ® fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 2

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore ® fuel product. The long-term EnCore fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15 N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Magnification Determination for AGHCF Metallographic Images

Metallographic images generated in the Alpha Gamma Hot Cell Facility (AGHCF) have been used for quantitative and qualitative characterization of irradiated metallic fuel pins. Individual high-magnification images (micrographs) contained in AGHCF file folders and experimental notebooks are in the form of polaroid photographs labeled with AGHCF identification number, magnification, and surface condition (as-polished or etched). Low magnification composite images (photomosaics) are also available for fuel cross sections, for radial strips from the fuel center to the cladding outer diameter, and for circumferential strips of the cladding and outer fuel region. The individual images do not have scale bars. Only a few of the composite images contain scale bars. The purpose of this work is to describe and apply methods for checking the magnification (50X to 500X) of individual images and for determining the magnification (~25X to ~100X) of composite images. The metallographic images used to verify and/or determine magnification were generated during the 1989 to 1993 timeframe for cross sections of U-10Zr/HT9 fuel rods irradiated in EBR-II and for cross sections of irradiated U-10Zr/HT9 fuel-rod samples following elevated-temperature tests conducted in the out-of-pile AGHCF Fuel Behavior Test Apparatus (FBTA). Procedures are documented in the AGHCF Operations Manual for preparation of metallographic samples, for calibration verification, and for constructing composites from individual images. Calibration verification of magnification was performed at least semiannually. One standard used for calibration verification was a glass slide with vertical lines indicating distances of 1 mm, 0.1 mm and 0.01mm. Guidance is provided in the current work for determining magnification from images of the standard. In addition to the periodic calibration verification, consistency checks are recommended to verify the magnification of images taken between the routine calibration verifications. For cladding samples with or without significant fuel-cladding chemical interaction (FCCI), images taken at different magnifications (e.g., 150X and 200X) of the unaffected cladding thickness can be compared. This process is independent of changes in cladding thickness due to swelling and creep. For images taken at only one magnification of cladding regions with no FCCI, the cladding thickness determined from the images may be compared to the nominal as-built cladding thickness (15.0 ± 0.5 mils for examples used in current work)). This procedure works best for cladding that has not experienced significant swelling and/or creep (e.g., ≤2% circumferential strain at the cladding outer surface). Composite images were constructed by pasting together higher magnification images and photographing the composite to generate a negative from which the hard-copy photograph was developed. The primary purpose of the composite images was to identify interesting areas of the fuel and cladding for imaging at higher magnification. However, procedures are recommended in the current work for determining composite magnifications to allow quantitative characterization of the fuel. Composites are not recommended for determining cladding thickness or FCCI depth because magnifications are too low (generally ≤110X) and image contrast is low. Fuel cross-section composites were created by pasting together 50X or 75X images. The nominal magnification for the photographed fuel cross-section composites is 25.4X. A more precise magnification can be determined by comparing the average cladding outer diameter measured from the composite to the average cladding outer diameter measured by profilometry. Radial-strip composites were constructed by pasting together high-magnification (150X or 250X) images. The nominal magnification of radial-strip composites photographs is about 100X. A more precise method for determining the magnification of radial strips is to compare the cladding thick

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Consequence Analysis of Residual Water in a Storage Canister - 20484

Recent observations from projects sponsored under the DOE-Nuclear Energy Spent Fuel and Waste Disposition campaign show that residual free water, well above the 0.4 gm-moles that correspond to a 3 torr rebound pressure after a 30-minute hold following prototypic drying, may remain within SNF canisters used for long-term dry storage. Specifically, experimental observations in an Integrated Research Project showed subzero temperatures and a local pocket of frozen water in a mockup fuel assembly subjected to an industry practiced drying process. In gas sampling and analysis from the High Burnup (HBU) Demonstration project, using a fully loaded and dried SNF canister, indicated presence of 100 g of residual water had remained in the canister. The effects of residual water in terms of potential adverse impacts on the condition of the SNF and the canister internals during long-term dry storage has been rigorously evaluated to address inadvertent residual water contents. The impact of residual water on the fuel and canister internals, with a focus on the oxidation of the cladding and of postulated exposed (breached-clad) fuel, were evaluated using an integrated set of time-dependent environmental conditions with semi-empirical materials oxidation models. An 'integration model,' with coupled sub-models, developed and previously used by the Center for Nuclear Waste Regulatory Analysis (CNWRA), was applied and expanded with improved sub-models for water radiolysis, and for cladding and fuel oxidations. Cladding oxidation models for various alloys were developed using the rate constants for various cladding alloys in the dry storage temperature range. A burnup-dependent fuel oxidation model was developed; it accounted for inhibition effect of fission products on fuel oxidation rates. The potential for extension of the initial breach flaw (1 mm hole) was evaluated by two separate mechanics criteria. In the first case, a critical cladding strain criterion was used. In the second case, a critical stress intensity was used to evaluate stability of a planar axial flaw postulate. A failure condition exists when a sufficient amount of fuel oxidation (at the postulated breached-clad location) causes fuel pellet swelling to load the cladding to meet a mechanics criterion for flaw extension. The integration model's results provide the following insights. The radiolysis-generated oxygen is consumed with a partitioning between the cladding and the fuel. The extent of cladding oxidation is no more than 2 μm additional consumption of the cladding metal even with 10 moles of residual water, indicating that changes in cladding conditions due to water are expected to be negligible. The conditions for cladding failure (breach opening size extension) directly correlates with the extent of fuel oxidation. Fuel oxidation significant to extend the breach could occur even with 5.5 moles of residual water. The results indicate that fuel oxidation vis-a-vis cladding oxidation is more likely under a higher radiation field, i.e., when radiolytic decomposition of the residual water occurs in few years compared to several decades, and that the conditions to cause failure are increased with fuel and cladding temperatures approaching the peak storage temperature limit of 400 deg. C. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

High-burnup Experiments in Reactivity Initiated Accidents (HERA)

HERA is a joint experimental program (JEEP) operating within the Nuclear Energy Agency’s (NEA’s) framework for irradiation experiments (FIDES). HERA is dedicated to the understanding of light water reactor (LWR) fuel performance at high burnup under reactivity-initiated accidents (RIA). During RIAs the fuel cladding can be breached by one of two mechanisms; pellet-cladding mechanical interaction or high temperature balloon and rupture. Pellet-cladding mechanical interaction (PCMI) failure occurs in the early phase of an RIA transient where the fuel pellet expands rapidly into the cladding prior to any meaningful heat transfer from the pellet to the cladding. This results in high stresses in the cladding resulting in crack propagation through the base Zircaloy metal and axially along the cladding tube. Failure by PCMI is a brittle failure mode and occurs at low cladding strains, approximately 2% hoop strain. If the cladding survives the PCMI phase of the transient, it may still fail due to ballooning and rupture induced by extended exposure to high temperature. Thermal transport from the fuel pin to the coolant is significantly reduced if a transition to film boiling on the cladding surface occurs. This result in both a rapid increase in fuel temperature, which drives fission gas release, and a spike in cladding temperature, which results in loss of mechanical strength. If the internal pressure of the fuel rod is greater than the system pressure the cladding can inelastically deform and eventually rupture. Failure by swelling and rupture occurs at larger strains, generally greater than 5% hoop strain. While PCMI failures are generally seen as more limiting, the dominance of one failure mode over the other can be affected by both the cladding material conditions, and the transient evolution.

(HERA)↗

High-burnup Experiments in Reactivity Initiated Accidents (HERA)

HERA is a joint experimental program (JEEP) operating within the Nuclear Energy Agency’s (NEA’s) framework for irradiation experiments (FIDES). HERA is dedicated to the understanding of light water reactor (LWR) fuel performance at high burnup under reactivity-initiated accidents (RIA). During RIAs the fuel cladding can be breached by one of two mechanisms; pellet-cladding mechanical interaction or high temperature balloon and rupture. Pellet-cladding mechanical interaction (PCMI) failure occurs in the early phase of an RIA transient where the fuel pellet expands rapidly into the cladding prior to any meaningful heat transfer from the pellet to the cladding. This results in high stresses in the cladding resulting in crack propagation through the base Zircaloy metal and axially along the cladding tube. Failure by PCMI is a brittle failure mode and occurs at low cladding strains, approximately 2% hoop strain. If the cladding survives the PCMI phase of the transient, it may still fail due to ballooning and rupture induced by extended exposure to high temperature. Thermal transport from the fuel pin to the coolant is significantly reduced if a transition to film boiling on the cladding surface occurs. This result in both a rapid increase in fuel temperature, which drives fission gas release, and a spike in cladding temperature, which results in loss of mechanical strength. If the internal pressure of the fuel rod is greater than the system pressure the cladding can inelastically deform and eventually rupture. Failure by swelling and rupture occurs at larger strains, generally greater than 5% hoop strain. While PCMI failures are generally seen as more limiting, the dominance of one failure mode over the other can be affected by both the cladding material conditions, and the transient evolution.

(HERA)↗

Characterization of modeling and experimental data inconsistencies from burst testing for high-burnup commercial fuel rod applications

Fuel fragmentation, relocation, and dispersal are some of the largest issues remaining in the nuclear industry before rod-average burnup can be increased beyond 62 GWd/tU. The issue is primarily related to the potential for fuel to be dispersed into the reactor primary system, which may increase public risk. One way to prevent dispersal is to avoid cladding burst. The objective of this work is to support the high burnup safety case by evaluating cladding burst under high-burnup, full-length fuel rods and to identify uncertainties that could improve model predictions. The results of this analysis will evaluate realistic, prototypic loss-of-coolant accident (LOCA) conditions; support future cladding burst test designs; and inform the development of mechanistic material models. Realistic high-burnup operating conditions were implemented in the BISON fuel performance code to simulate steady-state and LOCA transient fuel rod evolution to the point at which cladding burst occurred. Parametric studies are performed to assess code response to changes in rod internal pressures and heating rates. Results were compared with simulated LOCA experiments to identify inconsistencies between commercial fuel rod analysis and experimental validation. The representative full-length fuel rod LOCA simulation results did not agree with cladding burst tests. Cladding burst tests indicated burst occurring well below (100–150 °C) those calculated in the full-length fuel rod LOCA analysis. Further investigation indicated that the cladding burst tests do not appear to be representative for full-length fuel rods. The inconsistency investigated in this work showed that the differences between the BISON simulation and the experiment's cladding burst conditions arise from an incomplete characterization of the cladding surface temperature, detailed rodlet characterization, lack of cladding strain measurements, and uncertainty in the cladding creep and failure models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Produce ZrH Moderator Material

This reports complete Milestone M2.2.3 Produce zirconium hydride moderator material. In this milestone, we report the successful fabrication of FeCrAl alloys cladded zirconium hydride moderator. Different types of crucible designs were presented, including the basic design with bar cladding material, basic design with tube cladding material, and crucible design with position holding function. Mo and FeCrAl were used as the trial cladding materials. The welding techniques and procedures were reported and discussed. Totally three welding techniques were adopted in the development of moderator cladding, and they are electron beam welding (EBW), laser welding (LW), and gas tungsten arc welding (GTAW). After welding, all cladded crucibles were evaluated with two kinds of leak testing, the helium leak test for minor leakage and the bubble test for major leakage. Due to the concern of the poor neutronics performance, Mo was not ideal for future moderator cladding application. Therefore, detailed characterization of the Mo cladded zirconium hydride was not pursued. Instead, the characterization of FeCrAl cladded zirconium hydride was performed. We discussed two material conditions (i.e., as machined and pre-oxidized conditions) prior to the cladding process, evaluated thermal stability of cladded zirconium hydride moderator through directly measuring hydrogen release, and characterized the zirconium hydride following the thermal desorption measurement. The results showed pre-oxidized FeCrAl is capable of efficiently preventing hydrogen release from the moderator assembly.

36 MATERIALS SCIENCE↗

Probabilistic Failure Criterion of SiC/SiC Composites Under Multiaxial Loading

Owing to its excellent mechanical properties and stability under high temperature and neutron irradiation conditions, SiC/SiC composites have emerged as a promising material for light water reactors (LWRs) in the development of accident-tolerant fuel (ATF) systems. Structural integrity and retention of hermeticity are two crucial requirements for SiC/SiC claddings during normal operations, and both of them are closely related to the proportional limit stress (PLS) of the material. Understanding the behavior of SiC/SiC composites under multiaxial stress states and developing a probabilistic approach for evaluating the structural vulnerability are of paramount importance for reliability-based analysis and design of SiC/SiC composite claddings. So far, there has been very limited effort towards experimental and analytical investigations of probabilistic failure of SiC/SiC claddings. This critical knowledge gap motivates this research. A probabilistic failure criterion for SiC/SiC composites under multi-axial loading is developed, and this criterion is incorporated into reliability analysis of the structural integrity of SiC/SiC fuel cladding. The research consists of two parts: 1) experimental investigation of multiaxial failure behavior of SiC/SiC composites, and 2) theoretical modeling of time-dependent probabilistic failure of SiC/SiC cladding. In the experimental investigation, the PLS is determined through the examination of stress-strain response, the acoustic emission measurement, as well as the X-ray computed tomography. The theoretical framework is derived by combin- ing the finite weakest-link statistical model and the subcritical damage growth model. This theoretical model captures the time-dependent failure mechanism of the material, which has a major consequence for predicting the lifetime distribution of the cladding. Meanwhile, the model also predicts that the failure statistics of the cladding depends strongly on the cladding length. The results of the multiaxial experiments reveal the level of statistical variation of the PLS of SiC/SiC materials under different stress states. The theoretical model provides a robust analytical tool for extrapolation of small-scale laboratory test results to the behavior of full-scale claddings. These findings establish a scientific foundation for the development of reliability-based design of SiC/SiC fuel claddings, which will play an essential role in improving the structural safety and integrity of LWRs.

42 ENGINEERING↗

The effect of temperature and burnup on U-10Zr metallic fuel chemical interaction with HT-9: A SEM-EDS study

The fuel cladding chemical interaction (FCCI) between Uranium-Zirconium-based metallic fuel and cladding materials during in-pile service is one of the most constraining phenomena affecting the performance of this fuel system. In this study, we investigated the effect of temperature and burnup on the FCCI development in two U-10 wt.% Zr (U-10Zr) fuel samples with HT-9 cladding irradiated as part of the MFF-3 irradiation test in the Fast Flux Test Facility (FFTF). One sample achieved a burnup of 13.1 at.% and operated with an average inner cladding temperature of 530°C, while the other achieved a burnup of 8.5 at.% and was subjected to an average inner cladding temperature of 615°C. Automated scanning electron microscopy (SEM) back-scattered electron (BSE) imaging of entire fuel cross-sections and SEM energy dispersive x-ray spectroscopy (EDS) analysis on specific fuel-cladding interface regions successfully provided a comprehensive characterization of the depth and type of interaction happening under different irradiation conditions. Further, our analysis shows that FCCI development on both fuel and cladding side is strongly influenced by the inner cladding temperature and, to some extent, the formation and integrity of Zr-rich layers between the fuel and cladding, while the impact of burnup and power is negligible. Measured FCCI thicknesses were compared to BISON simulations using both an empirical model based upon legacy data from the Experimental Breeder Reactor II (EBR II) irradiations and a mechanistic model currently under development for the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program, showing satisfactory agreement. Nonetheless, this comparison supports the need for additional microstructural characterization in intermediate ranges of temperature, power, and burnups in prototypic-length pins.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Summary Report on Ion Irradiation Study of Ceramic Coating on Suppressing FCCI

Advanced cladding is critical for advanced nuclear reactors with an enhanced performance in radiation tolerance and neutron transparency. Using advanced cladding will ensure the adequate thermal conductivity and mechanical stability of the cladding base material, corrosion resistance, high-temperature coolant compatibility of the cladding surface, and chemical stability in the cladding inner wall against fuel cladding chemical interaction (FCCI). An innovative cladding with a three-layer structure (i.e., a modified surface, a clad base material, and a modified inner wall) promises to meet all these requirements. Initial research and development (R&D) regarding this innovative cladding seek to demonstrate the effectiveness of a thin ceramic coating in suppressing FCCI under ion irradiation to high dose. This United States (U.S.) Department of Energy (DOE)–Office of Nuclear Energy (NE) project report summarizes the results of recent ion irradiation studies of diffusion-couple samples with details of an ion irradiation experiment, the characterization of the interface microstructure of cerium (Ce)/titanium nitride (TiN)/oxide-dispersion strengthened (ODS), Ce/TiN/iron (Fe), Ce/ODS, and Ce/Fe samples irradiated with 80 million electron-volts (MeV) of xenon (Xe) ions to 100 displacements per atom (dpa) at 500?C using the Argonne Tandem Linac Accelerator System (ATLAS) facility at Argonne National Laboratory (ANL). The results of the ODS-substrate sample are encouraging and demonstrate the effectiveness of a thin ceramic coating on FCCI mitigation under irradiation. The results from an Fe-substrate sample revealed a complex microstructure, and the root cause is discussed.

36 MATERIALS SCIENCE↗

BWR Spent Nuclear Fuel Acquisition and Testing to Support DOE-NE High Burnup Spent Fuel Data Project

The Office of Spent Fuel and Waste Disposition (SFWD) within the US Department of Energy (DOE) Office of Nuclear Energy (NE) established the Spent Fuel and Waste Science and Technology (SFWST) campaign to conduct research and development (R&D) activities related to the storage, transportation, and disposal of spent nuclear fuel (SNF) and high-level radioactive waste. The SFWST program was created within SFWD to address issues of extended or long-term SNF storage and transportation. Some near-term objectives of SFWST are to use a science-based, engineering-driven approach to: Support the enhancement of the technical bases to support the continued safe and secure dry storage of SNF for extended periods; Support the enhancement of the technical bases for retrieving SNF after extended dry storage; Support the enhancement of the technical bases for transporting high burnup (HBU) fuel and transporting low burnup fuel and HBU fuel after dry storage DOE-NE, in partnership with the Electric Power Research Institute, developed the High Burnup Spent Fuel Data Project to perform a large-scale demonstration and laboratory-scale testing of HBU pressurized water reactor (PWR) fuels (exceeding 45 gigawatt-days per metric ton of uranium [GWd/MTU]). Under this project, 25 sister rods—which are rods that have the same design, power histories, and other characteristics—were removed from assemblies at the North Anna Nuclear Power Station and sent to Oak Ridge National Laboratory (ORNL) in January 2016. ORNL performed detailed nondestructive examination (NDE) on all 25 rods. The NDE consisted of visual examinations, gamma and neutron scanning, profilometry and rod length measurements, and eddy current examinations. After completing the NDE, 10 of the sister rods were delivered to Pacific Northwest National Laboratory (PNNL) in a NAC International, Inc. legal-weight truck cask in September 2018 for destructive examination (DE). To date, SFWD work has focused on the PWR fuel that is part of the Sister Rod Test program. No boiling water reactor (BWR) fuel has been tested in the program, and the data needs that were identified for the PWR fuel have not been collected for BWR fuel. The goal to obtain six to nine BWR rods and test them at ORNL will support closing this important data gap. BWR fuel comprises approximately 56% of the total fuel assemblies currently in storage at nuclear power plants in the United States. BWR nuclear fuel and cladding designs and manufacturing are significantly different from PWRs. Differences include the following: BWR fuel pellets are larger than PWR pellets; Variations of Zircaloy-2 (including liners) are used instead of the Zircaloy-4 cladding materials used in PWRs; Clad manufacturing and stress-relief processes are different between PWRs and BWRs; The fuel rod dimensions are different because larger rod diameters and thicker cladding are used in BWRs; BWR fuel typically has lower internal rod pressures and sees vastly different operating conditions than PWR fuel (i.e., two-phase flow); BWR assemblies are “canned,” meaning each assembly is surrounded by a metal fuel channel; BWR cladding is often composed of an inner pure Zr liner that has widely different mechanical properties than the Zircaloy-2 alloy and exhibits a stronger affinity for hydrogen; The BWR SNF generally has more total hydrogen in the cladding/liner than typical PWR fuel; The construction of the PWR and BWR assemblies is vastly different; BWR rods are solidly attached to the assembly nozzles and experience a much different vibration and shock load than PWR rods, which are “floating” within a grid system attached to guide tubes, and the rods sit loosely on the bottom end plates. These numerous differences will affect the way the BWR SNF responds under dry storage preparation processes (e.g., vacuum drying) and during transportation. The results collected in the PWR experimental program must be compared with a subset of similar data collected on BWR SNF to establish a technical basis for whether the larger PWR database is sufficient to bound the BWR SNF end-of-life conditions as is currently assumed for several fuel/clad properties. Changes that occur in both fuel types at HBU could exacerbate any mechanical property differences. As the fuel burnup increases, several changes occur that might affect the performance of the fuel, cladding, and assembly hardware in storage and transportation. These changes include increased cladding corrosion layer thickness, increased cladding hydrogen content, increased cladding creep strains, increased fission gas release, and the formation of the HBU structure at the surface of the fuel pellets. The Nuclear Regulatory Commission (NRC) limits the current maximum rod-averaged burnup to 62 GWd/MTU due to these changes and the lack of data at higher burnups.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multilayer Architecture Barriers for High Temperature Nuclear Applications

Innovative thin film multilayer metal/ceramic barrier coatings have been developed by Argonne National Laboratory to protect fuel cladding against different phenomena that can be encountered under the harsh operating conditions of advanced nuclear reactors. One phenomenon is Fuel-Cladding Chemical Interaction (FCCI), which can represent a challenge to the performance of steel-clad metallic fuels in sodium-cooled fast reactors (SFRs), especially when operating to high burnups at elevated cladding temperatures, and long fuel residence time. Another phenomenon is the corrosion of zirconium-based cladding under prototypic boiling water reactor (BWR) conditions and associated cladding during off normal conditions, including loss of coolant accidents (LOCA). This work provides details of the development and testing of a thin film (few microns) multilayer metal/ceramic (CrY/Y 2 O 3 ) coatings on steel cladding and its performance against FCCI. The coating architecture evolved through systematic mechanical testing, radiation tolerance assessments, and high-temperature diffusion studies from a preliminary multilayer concept to an optimized high-performance design. The optimized structure leverages stoichiometric Y 2 O 3 for its exceptional radiation stability, chemical inertness, and ultra-low fission product diffusivity (e.g., Ce diffusivity ~10 -20 m 2 /s in irradiated Y 2 O 3 at 650 °C). This is paired with ductile chromium-rich interlayers (Cr 95 Y 5 ), which significantly enhance fracture toughness and mechanical resilience. Design refinements, including increased ceramic layer thickness and optimized Cr–Y interlayer composition, eliminated fracture propagation and preserved coating integrity under extreme mechanical stress (>10× typical reactor conditions) and prolonged radiation exposure (~300 dpa). Those conditions are well beyond expected conditions during normal operations in SFR, and cover some of the transient conditions as well. In addition, the coating deposition was demonstrated to be applied uniformly to the inner surface of steel tubes representing prototypic SFR cladding. Another phenomenon under consideration in this work is the corrosion of zirconium-based cladding under prototypic boiling water reactor (BWR) conditions and associated off normal conditions including loss of coolant accident (LOCA). Another multilayer thin film coating is considered for mitigation of this phenomenon, where a coating of yttrium aluminum and yttrium aluminum ceramic/metal thin film coating. Preliminary results on the coating performance during high temperature thermal cycling (up to 1000 C) have shown promising performance of the coating. On-going optimization of the coating will continue in FY26.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗