A high-throughput investigation of Fe–Cr–Al as a novel high-temperature coating for nuclear cladding materials
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Bunn, Jonathan Kenneth↗
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Mechanical response and microstructure evolution from multiaxial stress relaxation in textured zircaloy nuclear cladding
Modern energy markets provide motivation for nuclear reactors to increase operational flexibility and load following capacity of existing reactor designs. The operational power changes result in fuel pellet expansion and contraction resulting in pellet-cladding mechanical interaction (PCMI) and high cladding stresses that are strongly related to stressed corrosion cracking (SCC) which can lead to fuel rod failure. This work aims to quantify the stress fields in cladding with a focus on multiaxial stress relaxation response from an imposed strain and the resulting microstructure changes in textured zircaloy claddings. Stress relaxation tests resulting in multiaxial stress fields are performed to measure the material response of Zircaloy-4 nuclear cladding. Multiple experiments using samples from the same piece of cladding are performed so samples with the same processing history may be removed at strategic points throughout mechanical testing for microstructure characterization. The microstructure evolution is analyzed with mechanical response to evaluate the static recovery impact on crystallographic texture and grain morphology. Experiments are performed at Idaho National Laboratory using an experimental device capable of applying internal pressure and independent axial load to commercial nuclear cladding at elevated temperatures with stress- or strain-controlled experimental capability. X-ray diffraction and electron backscatter diffraction are used for microstructure analysis. Rheological models are used to visualize the multiaxial stress-strain relationships and isolate elastic, plastic, and viscoplastic material properties for analysis.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Zirconium nanoparticle coating development for FCCI diffusion barrier in nuclear cladding
Fuel clad chemical interaction (FCCI) is a pervasive issue for metallic nuclear fuels. FCCI can damage cladding, reduce thermal efficiency, and compromise the structural integrity of the fuel rod. In this study, we evaluated the FCCI mitigation capabilities of electrophoretically-deposited Zr nanoparticle coatings on ferritic-martensitic stainless-steel cladding (HT9). Zr was deposited on the internal surface of 6 mm outer diameter cladding using electrophoretic deposition (EPD). Thickness varied among samples with similar EPD conditions. A uniformly coated sample was selected and sent to the Argonne Tandem Linac Accelerator System (ATLAS) to simulate the coating's behavior under irradiation conditions. Furthermore, the coating prevented FCCI in diffusion couple studies. Results of this study confirm that Zr could potentially make an effective FCCI barrier in metallic fuel rods but the deposition process needs improvement.
36 MATERIALS SCIENCE↗
Dynamic data-driven multiscale modeling for predicting the degradation of a 316L stainless steel nuclear cladding material
Here, we have developed a long short-term memory stacked ensemble (LSTM-SE) surrogate modeling approach that can provide rapid predictions of microstructural evolution and the resultant mechanical properties of American Iron and Steel Institute (AISI) 316L series stainless steel (316LSS) fuel cladding under conditions of varying temperature and radiation dose rate. To acquire training data, we developed and implemented a kinetic Monte Carlo (KMC) model to simulate precipitation kinetics of M 23 C 6 , γ', and G phases within SS316L cladding. Experimentally reported precipitation kinetics of SS316L in literature were linked to the kinetic parameters of the simulated precipitation in our KMC model. The model was then used to simulate microstructure evolution under synthetically generated treatments of varying temperature and radiation dose rate, for periods of up to 3000 hours. Changes in volume fraction, number density, and particle size of precipitates were recorded, and particle area fractions were correlated using statistical methods to develop the surrogate model. Simultaneously, the mechanical properties of the simulated microstructures were evaluated using microstructure-based finite element method (FEM) analysis to determine the elastic modulus, yield stress, ultimate tensile strength, and elongation to failure of the aged microstructures. Using this approach, our surrogate model can predict precipitation behavior within 0.25% volume fraction and mechanical properties within 6% relative error from the values predicted by the KMC and FEM models using 50 training simulations as input. The trained recurrent neural network-based model can return estimations of precipitation kinetics and mechanical properties ~1000 times faster than the physics-based codes. This work demonstrates, as a proof of concept, that reactor material service lifetimes under variable service conditions can be predicted for a statistics-based model from a practicably obtainable dataset.
36 MATERIALS SCIENCE↗
A microstructure-based wear model for grid-to-rod fretting of clad nuclear fuel rods
Not Available
Blau, Peter J.↗
Low temperature chemical processing of graphite-clad nuclear fuels
A reduced-temperature method for treatment of a fuel element is described. The method includes molten salt treatment of a fuel element with a nitrate salt. The nitrate salt can oxidize the outer graphite matrix of a fuel element. The method can also include reduced temperature degradation of the carbide layer of a fuel element and low temperature solubilization of the fuel in a kernel of a fuel element.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Coating of nuclear fuel cladding materials, method for coating nuclear fuel cladding materials
The invention provides a nuclear reactor cladding, wherein at least one layer of coating is deposited on the exterior surface of the cladding. A nuclear reactor cladding, wherein at least one layer of coating is deposited on the interior surface of the cladding. A method of coating a nuclear reactor cladding, with the steps of selecting the cladding and depositing at least one layer of a first coating on the cladding.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
STRUCTURAL MODELING TO SUPPORT POST-YIELD ACCEPTANCE CRITERIA FOR SPENT NUCLEAR FUEL CLADDING
Spent nuclear fuel (SNF) is evaluated for structural failure during storage and transportation scenarios. The U.S. Department of Energy’s Spent Fuel and Waste Science and Technology (SFWST) program has sponsored significant research in quantifying mechanical loads on SNF during storage and transportation scenarios using experimental and modeling methods. The SFWST program has also performed significant research on measuring the mechanical behavior of irradiated SNF as defueled cladding segments and cladding with fuel pellets to measure composite behavior. This paper considers some of the key material data from the Sibling Pin testing and uses structural modeling and analysis methods that have been informed by testing to consider post-yield acceptance criteria for SNF cladding structural analysis. Test data published by Oak Ridge National Laboratory (ORNL) and Pacific Northwest National Laboratory (PNNL) are the foundation for informing the material behavior of the models developed in this study. In particular, four-point bend (4PB) tests of fueled and defueled cladding segments provide significant information about the bending failure mode of SNF. ORNL’s 4PB test data is on fueled cladding segments, so the composite behavior of SNF is demonstrated. This paper describes PNNL’s coincident beam model that was developed to approximate the composite behavior of SNF. This paper also presents PNNL’s structural dynamic finite element models of a cask tip-over scenario, which is predicted to cause the strongest mechanical loads on SNF of all postulated storage and transportation scenarios. SNF bending loads predicted in the cask tip-over scenario and cladding acceptance criteria beyond yield are considered, with justification based on the Sibling Pin test data. ASME Boiler and Pressure Vessel code stress intensity limits are also considered. The ultimate goal of this work is to aid in the justification of structural acceptance criteria for SNF cladding beyond the cladding’s irradiated yield strength for use in structural analysis of all storage and transportation scenarios.
Klymyshyn, Nicholas A.↗
Radiolytic Gas Production from Aluminum Coupons (Alloy 1100 and 6061) in Helium Environments—Assessing the Extended Storage of Aluminum Clad Spent Nuclear Fuel
Corrosion of aluminium alloy clad nuclear fuel, during reactor operation and under subsequent wet storage conditions, promotes the formation of aluminium hydroxide and oxyhydroxide layers. These hydrated mineral phases and the chemisorbed and physisorbed waters on their surfaces are susceptible to radiation-induced processes that yield molecular hydrogen gas (H 2 ), which has the potential to complicate the long-term storage and disposal of aluminium clad nuclear fuel through flammable and explosive gas mixture formation, alloy embrittlement, and pressurization. Here, we present a systematic study of the radiolytic formation of H 2 from aluminium alloy 1100 (AA1100) and 6061 (AA6061) coupons in “dry” (~0% relative humidity) and “wet” (50% relative humidity) helium environments. Cobalt-60 gamma irradiation of both aluminium alloy types promoted the formation of H 2 , which increased linearly up to ~2 MGy, and afforded G-values of 1.1 ± 0.1 and 2.9 ± 0.1 for “dry” and “wet” AA1100, and 2.7 ± 0.1 and 1.7 ± 0.1 for “dry” and “wet” AA6061. The negative correlation of H 2 production with relative humidity for AA6061 is in stark contrast to AA1100 and is attributed to differences in the extent of corrosion and varying amounts of adsorbed water in the two alloys, as characterized using optical profilometry, scanning electron microscopy, Raman spectroscopy, and X-ray diffraction techniques.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Report Summarizing Boiling Transition (Dryout) Testing of FeCrAl Cladding
Nuclear fuel and cladding in a light water reactor must maintain integrity under all normal operational and anticipated operational occurrences. In a Boiling Water Reactor (BWR) some Anticipated Operational Occurrences (AOOs) and Anticipated Transients Without SCRAM (ATWS) events have been known to result in cladding damage due to dryout with conventional Zircaloy-2 claddings. This work presents an assessment of commercially-fabricated, accident tolerant iron-chromium-aluminum (FeCrAl) alloy C26M cladding in such events with regard to the ballooning failure mode for unirradiated cladding In the severe accident test station (SATS), an experiment has been developed to gauge accident tolerance of fuel cladding materials under simulated cyclic dryout conditions. Thermal cycling from 300°C to 650°C was implemented on C26M and Zircaloy-2 tubes. The C26M tube did not fail after 54 cycles. The Zircaloy- 2 tube run under the same parameters as the C26M tube failed during the fourth cycle, consistent with expectations from the literature. Due to thermal gradients present in the furnace, both tubes experienced a maximum temperature at ~780°C. Due to differences in tube geometry, the hoop stress of the C26M tube was significantly higher than that of the Zircaloy-2 tube, 76 MPa at the maximum peak temperature compared to 55 MPa at burst, respectively. The cyclic dryout experiments show an increased performance of C26M over Zircaloy-2 under simulated conditions, an indication of C26M possessing superior high temperature oxidation resistance, mechanical properties and potentially resistance to fatigue.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
3D printed features on nuclear fuel cladding for optimized heat transfer
A nuclear fuel cladding with improved thermomechanical properties is provided. The nuclear fuel cladding includes a double-walled construction having inner and outer hexagonal sidewalls. The inner sidewall and the outer sidewall are spaced apart from each other to form a cooling channel therebetween, and the inner sidewall surrounds a nuclear fuel and is spaced apart from the nuclear fuel by a small gap. Helical fins extend into the cooling channel to interconnect the inner sidewall and the outer sidewall. Resilient fingers extend toward the nuclear fuel through the small gap to comply with variations in the size of the nuclear fuel due to fabrication tolerances as well as thermal expansion and swelling of the nuclear fuel, for example UO 2 , when undergoing fission. The nuclear fuel cladding is formed according to an additive manufacturing process, for example laser powder bed fusion printing.
Petrie, Christian M.↗
Method of separating and recovering uranium from aluminum-clad metallic nuclear fuel
According to one aspect of the invention, a method for separating and recovering uranium from a nuclear fuel element. The method includes immersing a nuclear fuel element containing nuclear fuel and cladding in a molten metal. The nuclear fuel includes uranium. The cladding is selectively dissolved from the nuclear fuel element when immersed in the molten metal. The nuclear fuel is separated from the cladding. The method then includes loading the nuclear fuel into a permeable basket that is electrically configured as an anode of an electrolytic cell. There are also a molten salt electrolyte and a cathode in the electrolytic cell. Then, the method includes applying an electric charge across the electrolytic cell. The molten salt electrolyte selectively transfers uranium from the anode to the cathode.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Modeling Radiolysis and Chemical Reactions during Dry Storage of Aluminum-clad Spent Nuclear Fuel
After aluminum-clad spent nuclear fuel (ASNF) is removed from the reactor, it is initially stored in spent fuel pools, which are specially designed water-filled basins that provide temporary cooling to reduce the temperature of the fuel assemblies and provide radiation shielding. ASNF continues to generate heat due to the radioactive decay of elements within the fuel, which persists for many years post-shutdown as the residual radioactive products decay into more stable elements. During the wet storage period, an oxyhydroxide layer composed of boehmite/bayerite forms on the surfaces of the aluminum cladding from exposure to water in the pools. Road-ready packaging for long-term disposition of the ASNF involves dry storage in helium backfilled DOE standard canisters (DSCs). When the ASNF is removed from water storage and dried, most of the water is removed, but some physisorbed and chemisorbed water remains in the oxyhydroxide layers. This residual water can produce hydrogen when exposed to radiation from the ASNF during dry storage. Predicting hydrogen accumulation over time in the DSCs is critical for long-term storage considerations. Previous modeling efforts have developed coupled computational fluid dynamics (CFD)-chemical models to simulate temperature, pressure, and gas phase concentrations within the DSCs. These models use the thermal field predicted by CFD as input to a radiolysis model for the gas phase and the surface oxyhydroxide layer chemistry. Given the long storage period of the DSCs and the impracticality of long-term experiments, a simulation-based approach is necessary to assess chemical evolution within the canisters. This study advances the development of a modeling framework designed to simulate the chemical evolution of spent fuel canisters. Both thermal and radiation-driven reactions are considered, with radiation kinetics quantified using G-values. Sensitivity analysis identifies key parameters influencing species composition. Reaction pathway diagrams offer insight into dominant species formation routes, enabling more effective comparisons between model predictions and experimental observations, particularly regarding the production of hydrogen. Results show that the model predicts significant hydrogen gas production with minimal oxygen generation, primarily due to hydrogen formation via boehmite pathways. These findings underscore the importance of accurately characterizing surface-bound species and radiolysis kinetics. A deeper understanding of these mechanisms is critical for evaluating the long-term safety of nuclear waste storage.
12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
Drying and Analysis of Aluminum (Oxy)hydroxide Films for Dry Storage of Aluminum-Clad Spent Nuclear Fuels
In aluminum-clad spent nuclear fuels, an (oxy)hydroxide layer on the surface of the cladding hosts chemisorbed water formed during reactor and post-discharge exposure to water. Any residual water is susceptible to generating hydrogen via radiolysis, which can be a risk associated with dry fuel storage. Engineering-scale forced helium dehydration (FHD) and vacuum drying tests were conducted on mock-up fuel assemblies that included corroded aluminum surrogate plates to assess the removal of bulk and chemisorbed water. Thermogravimetric analysis was performed on samples of the surrogate plates, both undried control samples used to determine onset temperatures associated with a phase change occurring in the oxide layer and samples from drying tests used to determine the effectiveness of each drying method. Both vacuum drying and FHD processes were capable of removing bulk water. However, FHD was determined to provide additional drying capabilities, including partial removal of chemisorbed water from bayerite due to the higher temperatures during drying. In conclusion, the temperature threshold for partial dehydroxylation of the oxide layer was determined to be around 220°C, meaning any drying methods attempting to remove chemisorbed water must exceed 220°C.
chemisorbed water↗
In situ high-temperature 3D imaging of the damage evolution in a SiC nuclear fuel cladding material
Silicon carbide (SiC)-based nuclear fission fuel rod cladding has been considered as one of the possible designs for accident tolerant fuels. It is in the form of a SiC fibre reinforced SiC matrix composite tube (SiC f -SiC m ) with monolithic SiC outer and/or inner coating layers. This study focuses on the deformation and fracture processes in this material using in situ X-ray micro-computed tomography (XCT) at room temperature (RT) and 1200 °C in an inert gas environment in a C-ring compression loading configuration. Prior to testing, local properties and residual stresses were characterised using nanoindentation and Raman spectroscopy since they can impact the mechanical behaviour of the material. The 3D strain distribution, crack formation and propagation processes including the toughening mechanisms (e.g., crack deflection, micro-cracking, crack bridging and bifurcation) are investigated in the coating and underlying composites at RT and 1200 °C. There is no particular sequence which toughening mechanism occurs first – this is very different from the conventional toughening theory in ceramic-matrix composites under uniaxial tension loading. Indeed, no evidence of fibre pull-out or fibre fracture was observed in this SiC f -SiC m nuclear cladding material in the current C-ring compression configuration. The correlation between local measurements and bulk mechanical behaviour are discussed.
3D imaging↗
Review and Summary of Corrosion Behavior for Aluminum-Clad Spent Nuclear Fuel in Dry Storage
A description of the corrosion behavior of aluminum alloys used for cladding on aluminum-based, aluminum-clad nuclear fuel used in research reactors under potential dry storage conditions has been compiled. An evaluation is made of potential additional corrosion with water postulated to not be removed during drying. The relative humidity (RH) produced by typical dryness criteria for industrial spent nuclear fuel drying is expected to be low, particularly at high temperatures (17% RH at 20°C and lower at higher temperatures). Existing corrosion data suggests that negligible vapor-phase corrosion of aluminum is expected at such low humidity, even for nominally bare aluminum surfaces. That is, the predicted relative humidity from free water (e.g., 17% RH) is below the “critical” relative humidity (~40% RH at room temperature), below which no significant corrosion is observed for bare aluminum. Furthermore, reported room-temperature corrosion rates are very low even under saturated (100% RH) water vapor. Existing results showing significant vapor-phase corrosion corresponded specifically to conditions of high temper ed with high relative humidity. A relatively large reservoir of (chemically bound) water exists in the aluminum (oxy)hydroxide films on the SNF cladding surface. The estimated total could saturate the gas even at relatively high temperature if fully released; however, its release as molecular water is expected to only be plausible if the temperature during storage exceeds both the drying temperature and the threshold for thermal decomposition of the trihydroxides (~220°C). Therefore, the combination of high temperature and high relative humidity that could drive significant corrosion is considered implausible during sealed dry storage following an appropriate drying process, to include >220°C drying for canisters that may approach or exceed this temperature during storage. Vapor-phase testing of aluminum samples with an adherent (oxy)hydroxide layer, prepared in liquid water to resemble those on actual aluminum-clad spent nuclear fuel (ASNF), did not observe evidence of additional corrosion even at combined high-temperature (up to 180°C) and high-humidity (up to 100% RH) conditions. Instead, small net mass losses were observed for most specimens and attributed to dehydration of the samples, which had been air-dried only prior to testing. ASNF being moved to dry storage is expected to have an existing (oxy)hydroxide film, suggesting that the cladding will be less prone to additional corrosion than bare aluminum metal. If significant corrosion did occur during sealed storage, the overall extent and impact is expected to be small. Corrosion post-closure of a canister would not alter the total amount of hydrogen in the canister, so it would have no effect on the maximum H 2 release already assessed in existing bounding calculations. In addition, the total amount of water in a 25-µm dense bayerite film would consume a only ~8 µm additional aluminum metal on average, if fully consumed by oxidizing aluminum metal to Al 2 O 3 . These conclusions are consistent with ASNF-in-canister simulations to date, which included a reaction pathway for corrosion using kinetics from previous literature and believed to be conservative and predicted very low rates of corrosion.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Hydrothermal Corrosion of Latest Generation of FeCrAl Alloys for Nuclear Fuel Cladding
After the Fukushima nuclear disaster, the nuclear materials community has been vastly investing in accident tolerant fuel (ATF) concepts to modify/replace Zircaloy cladding material. Iron–chromium–aluminum (FeCrAl) alloys are one of the leading contenders in this race. In this study, we investigated FA-SMT (or APMT-2), PM-C26M, and Fe17Cr5.5Al over a time period of 6 months in simulated BWR environments and compared their performance with standard Zirc-2 and SS316 materials. Our results implied that water chemistry along with alloy chemistry has a profound effect on the corrosion rate of FeCrAl alloys. Apart from SS316 and Zirc-2 tube specimens, all FeCrAl alloys showed a mass loss in hydrogen water chemistry (HWC). FA-SMT displayed minimal mass loss compared to PM-C26M and Fe17Cr5.5Al because of its higher Cr content. The mass gain of FeCrAl alloys in normal water chemistry (NWC) is significantly less when compared to Zirc-2.
36 MATERIALS SCIENCE↗
Formation and characterization of hydride rim structures in Zircaloy-4 nuclear fuel cladding tubes
Zirconium alloy tubes used as nuclear fuel cladding are subject to oxidation and subsequent hydrogen pickup during their long service in commercial light water reactors. The hydrogen picked up in the cladding can precipitate as a brittle hydride rim feature on the cladding outer surface. Here, to better understand the effect of hydride rims on the fracture behavior of stress-relieved zirconium alloy cladding tubes, a procedure to produce these rim-like structures has been developed and is described herein. Extensive characterization of the ‘as hydrided’ tubes is performed. The hydrogen charging apparatus consists of a tube furnace with a quartz chamber that is connected to a vacuum pump as well as a bottle of pure hydrogen gas. The charging station uses a static charge of hydrogen as opposed to a flowing gas. The chief advantage of this approach is the ability to monitor the pressure drop in the hydriding chamber and correlate this pressure drop to a known rate of hydrogen pickup in the cladding tube. It was found that the hydrogen partial pressure, metal temperature, and surface treatment all clearly played a role in whether a hydride rim was formed. Extensive characterization of the hydride rims shows they consist of needle like platelets of δ phase hydrides (ZrH1.66) oriented in the circumferential direction with a radial spacing of several microns in a sandwich-like structure.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗