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At least 379 records · Page 21

Brittle failure analysis and modeling of high-burnup PWR fuel cladding alloys

The aim of this research is the development of methods for predicting mechanical behavior and identification of limiting conditions to prevent brittle failure of high-burnup (HBU) pressure water reactor (PWR) fuel cladding alloys. A finite element (FE) model of the ring compression test (RCT) was created to analyze the failure behavior of zirconium-based alloys with radial hydrides during the RCT. An elastic-plastic material model describes the zirconium alloy. The stress-strain curve needed for the elastic-plastic material model was derived by inverse finite element analyses. Cohesive zone modeling is used to reproduce sudden load drops during RCT loading. Based on the failure mechanism in non-irradiated ZIRLO (R) claddings, a micro-mechanical model was developed that distinguishes between brittle failure along hydrides and ductile failure of the zirconium matrix. Two different cohesive laws representing these types of failure are present in the same cohesive interface. The key differences between these constitutive laws are the cohesive strength, the stress at which damage initiates, and the cohesive energy, which is the damage energy dissipated by the cohesive zone. Statistically generated matrix-hydride distributions were mapped onto the cohesive elements and simulations with focus on the first load drop were performed. Computational results are in good agreement with the RCT results conducted on high-burnup M5 (R) samples. It could be shown that crack initiation and propagation strongly depend on the specific configuration of hydrides and matrix material in the fracture area.

Simbruner, Kai↗

Hydride Reprecipitation in Prototypical 17x17 PWR Fuel Rods after Simulated Vacuum Drying Conditions

Light water reactor (LWR) fuel rod cladding picks up hydrogen as it oxidizes in reactor. Once the hydrogen concentration exceeds the solubility limit, zirconium hydride platelets precipitate, generally in the circumferential direction. In preparation for dry storage, elevated temperatures can dissolve some of the circumferential hydrides, which during cooling can then reprecipitate in a direction perpendicular to the hoop stress (radially). From 2019 to 2024, ORNL published a series of reports that included metallographic observations of cladding after a thermal transient to 400°C followed by slow cooling. The simulated dry storage process was performed on three full-length 17x17 PWR fuel rods at their as-discharged rod internal pressure. There were two important observations from the metallographic examinations of these heat-treated rods: (1) the propensity for hydride reorientation is strongly influenced by nearby as-discharged precipitated hydrides, (2) the radial hydrides observed near the cladding inner diameter were often associated with cracks in the pellet. Subsequent modeling using the BISON fuel performance code that considered the effects of pellet cracks and pellet-cladding bonding observed in high-burnup fuel support the conclusion that pellet cracks enhance the local hoop stress in the cladding creating preferential sites for hydride reorientation, and that the influence of the pellet cannot be ignored in accurate fuel rod performance predictions.

Montgomery, Rose [ORNL] (ORCID:0000000286038936)↗

Bond Strength of Plasma Sprayed Zr Diffusion Barrier on U-Mo Fuels

The United States government is continually committed to strengthening nuclear security and nonproliferation for reducing the threat of radioactive materials acquisition by terrorists. To meet this important mission, the US Department of Energy and National Nuclear Security Agency's (NNSA) Office of Material Management and Minimization (M{sup 3}) Reactor Conversion Program (CONVERT) seeks to minimize the use of highly enriched uranium (HEU) in civilian applications through work with governments and facilities around the world to convert research reactors to the use of non-weapons-usable low enriched uranium (LEU) fuels. Each reactor converted not only eliminates the need for HEU at civilian sites, but also reduces the amount of HEU being manufactured, stored, and transported, where the nuclear material is most vulnerable. In instances where suitable LEU fuels do not exist for the conversion of particular reactors, CONVERT contributes to development of new LEU fuels. Currently, the CONVERT Program is committed to development of a high-density U-Mo fuel that will be able to convert high performance research reactors, while establishing an efficient and economic fabrication capability to manufacture the fuel. To that end, Los Alamos National Laboratory (LANL) has been tasked with development of a method to affix zirconium (Zr) metal fuel diffusion barrier via plasma spraying, which will prevent a reaction between the U-Mo fuel and the 6061 aluminum cladding. A successful diffusion barrier requires adequate Zr layer thickness, uniform coverage, sufficient bonding at the Zr/fuel and Zr/aluminum cladding interface, and maintenance of the original nuclear fuel properties i.e. physical dimensions, alloy composition and dispersion, crystallographic phase concentration, neutronics, etc. This work outlines development of the Zr plasma spray processing techniques, parameters affecting the diffusion barrier/nuclear fuel bond strength, and characterization of the Zr diffusion barrier. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High Temperature Fuel Cladding Chemical Interactions Between TRIGA Fuels and 304 Stainless Steel

High-temperature fuel-cladding chemical interactions (FCCI) between TRIGA (Training, Research, Isotopes, General Atomics) fuel elements and the 304 stainless steel (304SS) are of interest to develop an understanding of the fuel behavior during transient reactor scenarios. TRIGA fuels are composed of uranium (U) particles dispersed in a zirconium-hydride (Zr-H) matrix. In reactor, the fuel is encased in 304-stainless-steel (304SS) or Incoloy 800 clad tubes. At high temperatures, the fuel can readily interact with the cladding, resulting in FCCI. A number of FCCI can take place in this system. Interactions can be expected between the cladding and the Zr-H matrix, and/or between the cladding and the U-particles. Other interactions may be expected between the Zr-H matrix and the U-particles. Furthermore, the fuel contains erbium-oxide (Er-O) additions. Interactions can also be expected between the Er-O, the cladding, the Zr-H and the U-particles. The overall result is that very complex interactions may take place as a result of fuel and cladding exposures to high temperatures. This report discusses the characterization of the baseline fuel microstructure in the as-received state (prior to exposure to high temperature), characterization of the fuel after annealing at 950C for 24 hours and the results from diffusion couple experiments carries out at 1000C for 5 and 24 hours. Characterization was carried out via scanning electron microscopy (SEM) and transmission electron microscopy (TEM) with sample preparation via focused ion beam in situ-liftout-technique.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Determination of the hydrogen heat of transport in Zircaloy-4

During operation in a nuclear reactor, Zr-based nuclear fuel cladding is subject to waterside corrosion which can lead to hydrogen ingress. Here, the hydrogen that enters the material will migrate to colder spots and precipitate as zirconium hydrides if the hydrogen content exceeds the hydrogen terminal solid solubility in the material. Since a temperature gradient is established in the radial direction of the cladding during operation, the hydrides can preferentially precipitate at the colder outer surface of the cladding. Other gradients can also occur in the longitudinal and azimuthal directions of the cladding tube. As a consequence, hydrogen redistributes itself in response to the concentration and temperature gradients present in the sample. The response of the hydrogen in solid solution to temperature gradients is governed by the heat of transport Q* as a function of temperature, so it can be used in the BISON code. A set of experiments was set up to determine the heat of transport (Q*), in which a uniformly hydrided Zircaloy-4 sample is annealed under a fixed temperature gradient at a range of temperatures, and the resulting hydrogen distribution is analyzed to determine Q*. The results are discussed in terms of existing literature.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Oxidation and Hydrogen Uptake in Zirconium, Zircaloy-2 and Zircaloy-4: Computational Thermodynamics and Ab Initio Calculations

Zirconium-based alloys Zircaloy-2 and Zircaloy-4 are widely used in nuclear industry as cladding materials for BWRs and PWRs, respectively. Over more than 60 years these materials displayed a very good combination of properties such as low neutron absorption, creep behavior, stress-corrosion cracking resistance, reduced hydrogen uptake, corrosion, and/or oxidation, especially in the case of Zircaloy-4. However, over the last couple of years energetic efforts were undertaken to improve their oxidation resistance during off-normal temperature excursions, as well as to further improve upon the already achieved levels of mechanical behavior and reduced hydrogen uptake. In order to facilitate the development of such novel materials, it is very important to achieve not only engineering control, but also scientific understanding of the underlying material degradation mechanisms, both in working conditions and in storage of spent nuclear fuel. This paper strives to contribute to these efforts by constructing the thermodynamic models of both alloys, constructing of the respective phase diagrams, and oxidation mechanisms. A special emphasis was placed upon the role of zirconium suboxides in hydrogen uptake reduction and the atomic mechanisms of oxidation. To that end, computational thermodynamics calculations were conducted concurrently with first-principles atomistic modeling.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling of Some Physical Properties of Zirconium Alloys for Nuclear Applications in Support of UFD Campaign

Zirconium-based alloys Zircaloy-2 and Zircaloy-4 are widely used in the nuclear industry as cladding materials for light water reactor (LWR) fuels. These materials display a very good combination of properties such as low neutron absorption, creep behavior, stress-corrosion cracking resistance, reduced hydrogen uptake, corrosion and/or oxidation, especially in the case of Zircaloy-4. However, over the last couple of years, in the post-Fukushima Daiichi world, energetic efforts have been undertaken to improve fuel clad oxidation resistance during off-normal temperature excursions. Efforts have also been made to improve upon the already achieved levels of mechanical behavior and reduce hydrogen uptake. In order to facilitate the development of such novel materials, it is very important to achieve not only engineering control, but also a scientific understanding of the underlying material degradation mechanisms, both in working conditions and in storage of used nuclear fuel. This report strives to contribute to these efforts by constructing the thermodynamic models of both alloys; constructing of the respective phase diagrams, and oxidation mechanisms. A special emphasis was placed upon the role of zirconium suboxides in hydrogen uptake reduction and the atomic mechanisms of oxidation. To that end, computational thermodynamics calculations were conducted concurrently with first-principles atomistic modeling.

42 ENGINEERING↗

Structure of the pellet-cladding interaction layer of a high-burnup Zr-Nb-O nuclear fuel cladding

Here, structure of the pellet/cladding-interaction (PCI) layer of a high-burnup nuclear fuel with niobium-bearing cladding was investigated using modern transmission electron microscopy (TEM) techniques. Morphology of the PCI consisted of uniform zirconia layer on the cladding side and finger-like features towards to the ceramic fuel. The PCI layer showed a complex microstructure that constitutes three distinct zirconia layers formed by two zirconia phases. From cladding to fuel, monoclinic, tetragonal, and another tetragonal phase were determined via TEM diffraction patterns and precession electron diffraction (PED) using ASTAR microscopy platform (AMP). Characterizations showed that monoclinic and tetragonal phases close to the cladding were crack-free, but the tetragonal layer adjacent to the fuel contained cracks and pores. Presence of the monoclinic layer suggested that its formation involved the gaseous diffusion of oxygen below threshold dose of fission product damage before the fuel/cladding contact occurred. Furthermore, high-resolution TEM revealed compound phase of (U,Zr)O 2 at fringes of zirconia fingers on the fuel side.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Interface stability of ultrasonic additively manufactured Zircaloy-4 during hydrothermal corrosion

Simulated pressurized water reactor conditions (330 °C, 15.6 MPa, ~20 ppb oxygen) without irradiation were used to investigate the hydrothermal corrosion behavior of ultrasonic additively manufactured Zircaloy-4 up to 1000 h. X-ray computed tomography allowed for visualization of defects from processing and their progression after corrosion experiments. The specimens were found to have clear variability in the mass change data, compared to typical wrought Zircaloy-4 specimens. The variation in the mass change after exposure was attributed to weld defects connected to the specimen surface which allowed ingress of oxidant into the samples. Defects visualized by computed tomography were found via metallography and characterized. In conclusion, ultrasonic additively manufactured Zircaloy-4 was found to have comparable corrosion behavior as wrought Zircaloy-4 for specimens which did not have clear surface defects along weld interfaces.

36 MATERIALS SCIENCE↗

U-10Mo/Zr Interface Modeling using a Microstructure-Based FEM Approach

The U-10Mo in low enrichments (LEU) has been identified as the most promising alternative to the current highly enriched uranium (HEU) used in the United States’ fleet of high performance research reactors (USHPRRs). The nominal configuration of the new LEU U-10Mo plate fuel comprises a U-10Mo fuel foil enriched to slightly less than 20% U-235 (0.08” to 0.02” thick), a thin Zr interlayer/diffusion barrier (25 m thick) and a relatively thick outer can of 6061 aluminum. Currently, the Zr interlayer is clad by hot roll bonding. Previous studies and observations revealed a thinning of the zirconium (Zr) layer during this fuel fabrication process, which is not desirable from the fuel performance perspective. Coarse UMo grains, dendritic structures, Mo concentration segregation, carbides, and porosity are present in the as-cast material and can lead to a nonuniform UMo/Zr interface. The purpose of the current work is to investigate the effects of these microstructural parameters on the Zr coating variation. A microstructure-based finite-element method model was used in this work, and a study on the effect of homogenization on the interface between U-10Mo and Zr was conducted. The model uses actual backscattered electron–scanning electron microscopy microstructures, Mo concentrations, and mechanical properties to predict the behavior of a representative volume element under compressive loading during the rolling process. The model successfully predicted the experimentally observed thinning of the Zr layer in the as-cast material. The model also uses results from a homogenization model as an input, and a study on the effect of different levels of homogenization on the interface indicated that homogenization helps decrease this thinning. This model can be considered a predictive tool representing a first step for model integration and an input into a larger fuel fabrication performance model.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Understanding Manufacturing Scale-Up of Plasma Sprayed Zr Barrier Coatings on U-10Mo Fuels

The United States government is committed to further strengthening nuclear security and nonproliferation in order to reduce the threat of terrorists acquiring nuclear material. To meet this important mission, the US Department of Energy/National Nuclear Security Agency's Office of Material Management and Minimization (M{sup 3}) Reactor Conversion Program minimizes the use of highly enriched uranium (HEU) in civilian applications by working with governments and facilities around the world to convert research reactors to the use of non-weapons-usable low-enriched uranium (LEU) fuels. Each reactor converted not only eliminates the need for HEU at civilian sites, but also reduces the amount of HEU being manufactured, stored, and transported, where it is at its most vulnerable. In instances where suitable LEU fuels do not exist for particular reactors to convert, the M{sup 3} Reactor Conversion Program (CONVERT) contributes to the development of new LEU fuels. Currently, the M{sup 3} Reactor Conversion Program is committed to developing a high-density U-Mo LEU fuel that will be able to convert high performance research reactors while establishing an efficient and economic fabrication capability to make the fuel. To that end, Los Alamos National Laboratory (LANL) has been tasked with developing a method to affix a Zirconium fuel diffusion barrier via plasma spraying that will prevent a reaction between the U-Mo fuel and the aluminum cladding. This report discusses the transitions from development of the plasma spray deposition process to a scientific understanding of pseudo-production conditions and quantification of coating layer properties, characterization, reproducibility, etc. Understanding quality assurance and its applications to experiment work is non-trivial; statistical analysis of various measurement techniques not only improve quality, but will allow for scale up of manufacturing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Uranium Zirconium Alloy Dissolution

This Special Instructions provides a standard method to dissolve irradiated or unirradiated UZr alloys. The scope of this procedure was developed to facilitate total dissolution of UZr solid samples with and without cladding materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Secondary creep behavior of Zr-4 claddings under LOCA conditions

The thermo-mechanical behavior of Zircaloy-4 fuel rods under Loss-Of-Coolant Accident (LOCA) conditions in water cooled reactors is investigated. A custom experimental setup is dedicated to the high-temperature creep ballooning study of 90 mm long cladding samples. Creep tests were performed under an inert environment (argon), for temperatures from 750 to 850 C. degrees and internal pressures ranging from 1 to 5 MPa. During its operating life, Zr-4 cladding is submitted to oxidation and hydriding. These parameters strongly influence the creep behavior of Zirconium alloys at high temperatures. A first campaign on as-received Zr-4 was performed. Creep-rates are computed using 2-Dimensional Digital Image Correlation (2D-DIC) and are correlated to local temperatures measured using Near Infra-Red thermography. As-received Zr-4 behavior laws are determined using Finite Element Model Updating (FEMU). Norton exponents and activation energies are determined for thermal-mechanical conditions of the performed tests. The results show that the effect of applied stress on the Norton exponent is evidenced in the study for both α-phase and (α + β)-phase domains. The determined stress exponent magnitudes are very consistent with literature data depending on the thermomechanical test conditions. The activation energy parameter is very sensitive to the thermo-mechanical conditions and remains valid within a limited temperature and stress ranges to the authors' knowledge. The beginning of the (α + β)-phase domain is clearly identified with the activation energy increase. Finally, steady-state creep is accurately modeled depending on ballooning thermo-mechanical conditions.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Reduced yield stress for zirconium exposed to iodine: Reactive force field simulation

Iodine-induced stress-corrosion cracking (ISCC), a known failure mode for nuclear fuel cladding, occurs when iodine generated during the irradiation of a nuclear fuel pellet escapes the pellet through diffusion or thermal cracking and chemically interacts with the inner surface of the clad material, inducing a subsequent effect on the cladding’s resistance to mechanical stress. To complement experimental investigations of ISCC, a reactive force field (ReaxFF) compatible with the Zr-I chemical and materials systems has been developed and applied to simulate the impact of iodine exposure on the mechanical strength of the material. The study shows that the material’s resistance to stress (as captured by the yield stress of a high-energy grain boundary) is related to the surface coverage of iodine, with the implication that ISCC is the result of adsorption-enhanced decohesion.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Proton beam power limits for stationary water-cooled tungsten target with different cladding materials

The proton beam power limit for a solid-tungsten spallation target is largely determined by beam induced thermomechanical structural loads and decay heat power deposition, while its lifetime is limited by radiation damage and fatigue life of the target materials. In this paper, we studied the power limits of a stationary water-cooled solid tungsten target concept. Tantalum clad tungsten was considered as a reference case. Being a low activation material, zircaloy 2 cladding option was studied and its decay heat driven power limit was compared with the reference case. Zirconium alloys have proven operations records in spallation target and nuclear fission environments, supported by materials data obtained from post irradiation examinations. Recent study also demonstrated feasibility of diffusion bonding zirconium to tungsten using vanadium foil inter layer. Particle transport simulations code FLUKA was used to calculate energy deposition and decay heat power deposition in the target, based on the beam parameters technically feasible at the Second Target Station of the Spallation Neutron Source at Oak Ridge National Laboratory. The energy deposition data were used for flow, thermal, and structural analyses to determine the beam intensity limit on the target concept studied. The decay heat deposition data were used to calculate the transient temperature evolution in the tungsten volumes in a loss of coolant accident (LOCA) scenario to determine its beam power limit. For a 1.3 GeV proton beam, the power limit on a stationary target was 400 kW for a tantalum clad target model and 800 kW for a zircaloy 2 clad target model.

Lee, Yong Joong↗

Pellet cladding mechanical interaction as a potential failure mechanism during a control rod drop accident in a boiling water reactor

Boiling water reactors (BWRs) represent approximately one-third of the operating fleet in the United States, contributing significantly towards the global effort in reducing carbon emissions. Even though most of the operating fleet has been in operation for quite some time, continued advancements in new nuclear fuel (such as accident tolerant fuel) or operating regimes (such as power up-rates and higher burnup operation) necessitates similar advancements in modeling and simulation capabilities. Bison, a component of the Virtual Environment for Reactor Applications (VERA), is a high-fidelity fuel performance code able to explore the fuel performance of a wide variety of fuel types in one-, two-, and three-dimensions. Until recently, the code had not been used for analyses of BWRs. Modeling capabilities have been added for Gd-bearing UO{sub 2} and pure zirconium liners. New models have been added based upon the U.S. Nuclear Regulatory Commission (NRC) guide-lines for hydrogen pickup in Zircaloy-2 claddings and pellet-clad mechanical interaction (PCMI) failure during a reactivity insertion accident (RIA), known as a rod drop accident (CRDA) in BWRs. Implementing and/or improving Bison modeling capabilities extended its analytical reach to areas beyond its original intended purpose. This paper demonstrates one of these capabilities as a proof of concept. Recently developed models enable Bison to provide an alternate approach for cladding integrity determination in CRDA evaluations, which currently use bounding conservative estimates. As part of this demonstration, NRC guidance on hydrogen-pickup and PCMI failure models were utilized in this research. Even though more research is needed in establishing right inputs and process in this area, this paper demonstrates Bison's ability to determine cladding integrity in a CRDA evaluation. This first of a kind demonstration is a proof of concept in this area, which could potentially be extended to a number of other areas where a more accurate cladding integrity determination would be needed. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

First-principles investigation of lanthanides diffusion in HCP zirconium via vacancy-mediated transport

The diffusion of lanthanide fission products plays an important role in the growth of the fuel-cladding chemical interaction (FCCI) region in metallic fuels. The use of a Zr interdiffusion barrier may mitigate the transport of lanthanides from the fuel to the cladding, but the efficacy of such a liner is not yet known. In this paper, the stability and vacancy-mediated diffusion of La, Ce, Pr, and Nd in hexagonal close-packed (HCP) Zr is investigated via density functional theory (DFT) calculations and self-consistent mean field (SCMF) analysis. DFT is used to calculate the formation, binding, and migration energies of vacancies and vacancy-solute pairs. The DFT energetics are used in the KineCluE code to calculate the Onsager transport coefficients. La is found to be the fastest diffusing species in HCP Zr and experiences an almost isotropic diffusion behavior. The other three species (Ce, Pr, and Nd) demonstrate anisotropic diffusion where the diffusion in the basal planes is significantly faster than that along the c-axis. Further, the calculated lanthanide diffusivities in HCP Zr are fitted to an Arrhenius relation and the activation energies and prefactors are reported for the first time. Furthermore, the vacancy drag and the segregation tendencies were analyzed using the calculated off-diagonal transport coefficients. According to our vacancy-mediated diffusion model, lanthanides are expected to be enriched at vacancy sinks at low temperatures, while at high temperatures, lanthanides are depleted at sinks and will preferably diffuse into the bulk. The enrichment/depletion transition temperature depends on the diffusion direction (basal or axial) and hence will be controlled by the grain texture and orientation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The influence of cladding on fission gas release from irradiated U-Mo monolithic fuel

The monolithic uranium-molybdenum (U-Mo) alloy has been proposed as a fuel design capable of converting the world’s highest power research reactors from use of high enriched uranium to low enriched uranium. However, a zirconium (Zr) diffusion barrier must be used to eliminate interactions that form during fabrication and are enhanced during irradiation between the U-Mo monolith and aluminum alloy 6061 (AA6061) cladding. One aspect of fuel development and qualification is to demonstrate appropriate understanding of the extent of fission product release from the fuel under anticipated service environments. An exothermic reaction has previously been observed between the AA6061 cladding and Zr diffusion layer. In this paper, two fuel segments with different irradiation history were subjected to specified thermal profiles under a controlled atmosphere using a thermogravimetric/differential thermal analyzer coupled with a mass spectrometer inside a hot cell. Samples from each segment were tested with cladding and without cladding to investigate the effect, if any, that the exothermic reaction has on fission gas release mechanisms. Measurements revealed there is an instantaneous effect of the cladding/Zr exothermic reaction, but not necessarily a cumulative effect above approximately 973 K (700 oC). The mechanisms responsible for fission gas release events are discussed.

cl↗