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DOE OSTI2024

First principles density functional theory study of tritium species adsorption on Ni(111) surface and diffusion in nickel-sublayer for tritium storage

The nickel-plated zircaloy-4 is used as a tritium ( 3 H) getter in the tritium-producing burnable absorber rods (TPBARs) to capture 3 H produced in the 6 Li-riched annular γ-LiAlO 2 pellet under neutron irradiation. The experimental data and our previous theoretical results showed that the 3 H species produced from the γ-LiAlO 2 pellet were mainly 3 H 2 and 3 H 2 O. These 3 H species diffuse from the surface of the LiAlO 2 pellet across vacuum to the nickel-plated zircaloy-4 getter and then further diffuse into the getter to chemically form metal hydrides. While a number of studies show that oxygen binds strongly as compared to 3 H on the nickel (Ni) layer, the detailed mechanism of 3 H species absorption and diffusion across the Ni plate and Ni/Zr interface are still unclear. By employing density functional theory calculations, here we explored the 3 H 2 and 3 H 2 O species adsorption and dissociation on the Ni(111) surface and diffusion into the Ni sublayer. Our results indicated that the 3 H 2 and 3 H 2 O dissociate on the Ni(111) surface. The NiO x and Ni(O 3 H) x could be formed in the Ni layer due to the higher oxygen (O) diffusion energy barrier and formation of Ni vacancy defects. The oxygen was found to be retained in the Ni layer from diffusing across the Ni–Zr interface. This was revealed by comparing the diffusion barriers for 3 H with O. 3 H was found to have nearly three times smaller diffusion barrier than for O, making 3 H comparatively easier to diffuse through the Ni layer. In conclusion, the obtained results provide guidelines for experimental measurements on 3 H retention behavior in TPBARs and may open further avenues to explore the impurity effects on 3 H diffusion and storage at the Ni/zircaloy interfaces.

Tafen, De Nyago [National Energy Technology Lab. (↗

DOE OSTI2025

Tritium adsorption and absorption on (100) and (001) surfaces of pure and tin defective zirconium

Zirconium alloys such as zircaloy-4 are used as tritium (T) getter materials in tritium-producing burnable absorber rods (TPBARs) due to their ability to capture T, thereby forming metal hydrides. Developing an understanding of T adsorption onto zircaloy prior to diffusion into the subsurface is relevant for rational tritium getter and TPBAR design, to improve material properties for nuclear applications. Herein, density functional theory calculations revealed the preferred binding sites for T adsorption on Zr(001) and Zr(100). The energy barriers of T transfer, along the surface and from the surface to the subsurface were computed. The adsorption properties of Zr(001) were found to be superior to those of Zr(100). Surface tin impurities were found to strongly repel T. The presence of subsurface and surface tin resulted in higher absorption energy barriers for both the forward and reverse processes. Based on the calculated energy barriers, a surface to surface T diffusion coefficient of 9.53 × 10 -10 m 2 s -1 is expected for pristine Zr(001). Finally, a surface to subsurface T diffusion coefficient on the order of 10 -13 m 2 s -1 is predicted in pristine Zr, decreasing to 10 -19 m 2 s -1 for the transfer with a subsurface tin impurity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Characterization of Fuel-to-Coolant Heat Transfer During Reactivity-Initiated Accidents Using Tightly Coupled Thermal Hydraulics and Fuel Thermomechanics

The reactivity-initiated accident (RIA) is a complex scenario with several tightly interacting physical phenomena. Accurately predicting fuel behavior during these transients is difficult due to limitations in the modeling of fuel-to-coolant heat transfer. Common approaches to simulate RIAs involve standalone calculations using either a fuel performance code or a thermal-hydraulic code. The complex interdependencies of thermal-hydraulic and fuel mechanical behavior suggest that a tight coupling between these codes may provide more accurate predictions of fuel-to-coolant heat transfer and cladding mechanical response. Here, RELAP5-3D and BISON are coupled in this paper to simulate RIAs, and a sensitivity analysis is performed to rank key thermal properties and two-phase heat transfer parameters relevant for fuel-to-coolant heat transfer and cladding failure mechanisms in UO 2 –Zircaloy-4 systems. Gas gap conductance, film boiling heat transfer uncertainty, pulse width, fuel-specific heat capacity, and cladding-specific heat capacity were identified as important parameters. Variations in figures of merit resulting from changes to pulse width and the material thermal properties indicate that time-dependent heat transfer rates are significant for safety-relevant mechanical parameters due to the time dependence of cladding ductility and pellet-cladding mechanical interaction loading. The results suggest that the thermal-hydraulic factors have a nonnegligible influence on the thermomechanical solution and vice versa. Tight coupling of both sets of physics is recommended to improve prediction of fuel behavior during RIAs. Highlights include the following: 1. The RELAP5-3D thermal-hydraulic code and the BISON fuel performance code are tightly coupled for simulation of RIA transients with energy depositions at the Zircaloy-4 cladding failure threshold. 2. Departure from nucleate boiling occurred for all simulated cases. Due to the ductility of fresh fuel, substantial ballooning occurred in most cases. 3. Gas gap conductance, fuel-specific heat capacity, cladding-specific heat capacity, transient pulse width, and film boiling heat transfer were the dominant thermal factors impacting the safety figures of merit at energy depositions.

Critical Heat Flux (CHF)↗

DOE OSTI2025

A Standardized Analysis Process Using Digital Image Correlation to Calculate In Situ Cladding Strain from Modified Burst Tests for Fuel Performance Code Validation

Historical data collection on nuclear fuel cladding materials has focused on generating a statistically significant amount of data to assess the material and its failure behavior. Furthermore, data generated to support material model and failure criteria development were previously posttest evaluations, so a large number of tests was required to gain new understanding. A way to expedite this process is to develop techniques capable of generating large, high-fidelity data sets from a single test with lower uncertainty or quantified uncertainty. One such example of this approach is Oak Ridge National Laboratory’s use of modified burst tests (MBTs) to analyze the mechanical behavior and failure conditions of cladding during a simulated reactivity-initiated accident (RIA). Each test incorporates digital image correlation (DIC) analysis techniques that are used to assess the accumulated strain in situ, as well as eventual cladding failure. This work has been fruitful in defining strain-to-failure conditions for materials like silicon carbide (SiC) fiber–reinforced/SiC matrix composite tubes (SiC/SiC), iron-chromium-aluminum (FeCrAl) alloy tubes, and chromium-coated Zircaloy-4 tubes. However, there are numerous DIC software available, including open-source and proprietary software. The different DIC software use various algorithms to process images and calculate displacement values. Using these different software and algorithms can lead to varying results, and perhaps larger-than-expected uncertainties. In the present study, previously published MBT data encompassing a variety of test conditions were reanalyzed with two different DIC software to assess the variance in the calculated strain results. The data consisted of SiC/SiC, FeCrAl, and chromium-coated Zircaloy-4 tubes. Plots of the calculated strains during the transient revealed good agreement between the two DIC software. The average root-mean-square errors between the two software was 0.20% strain, which is slightly larger than a previously reported error value for these tests. In conclusion, this variance in results is low enough that this analysis method can be used for code validation.

Reactivity-initiated accident↗

DOE OSTI2022

The Mechanical Response of High Burnup 17x17 PWR Fuel Rods Under Bending

As a part of the US Department of Energy Office of Nuclear Energy High Burnup Spent Fuel Data Project, Oak Ridge National Laboratory has performed 4pt-bend tests on a series of 17x17 PWR fuel rods that were discharged with rod average burnups between 50 and 60 GWd/MTU. The rods include four different kinds of fuel cladding: standard Zircaloy-4 (Zirc-4), low-tin (LT) Zirc-4, ZIRLO, and M5. Six rods of each type (combining Zirc-4 and LT Zirc-4 as one type) were tested to failure at room temperature and 200 oC. Three of each type experienced a full-length heat treatment cycle from RT to 400 oC to RT with an 8 hr soak at 400 oC to simulate the expected limiting vacuum drying condition, which potentially induces hydride reorientation and causes some annealing of irradiation damage in the cladding. Overall, the fuel rods show significant capacity to deflect in bending and exhibit non-linear deformation before failing. The calculated failure strains range from 1.5% to 3.8%. The simulated vacuum drying heat treatment had the largest effect on fuel rods with ZIRLO and M5 cladding. In both cases the heat treatment caused increases in the plastic strain at failure, suggesting some annealing of irradiation damage is occurring. The finite element modeling of the 4pt bending test assume the pellet is a collection of pellet wedge pieces. The results for the Zircaloy-4 rods suggest that the pellets are bonded to the cladding and friction controls the relative motion of the pellet wedge pieces.

Cantonwine, Paul↗

DOE OSTI2024

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↗

DOE OSTI2020

Phase Equilibria and Thermochemistry of Advanced Fuels: Modeling Burnup Behavior (Final Report)

Achieving the goal of developing advanced fuel concepts that meet the DOE objectives of being robust, demonstrating high performance, and are more tolerant of accident conditions than current fuel systems will require a thorough understanding of the thermophysical and thermochemical properties of the constituent materials. Non-oxide fuel systems are being explored under the Advanced Fuels Program that hold significant promise for improved performance and accident tolerance, including the uranium silicide-based system considered in the current work. Prospective cladding materials currently considered that contribute to improved accident tolerance include silicon carbide composites and ferritic alloys (Fe-Cr-Al base compositions). Thus, the effort developed thermochemical models and values, supported with targeted experiments, to evaluate the ferritic alloy and silicon carbide composite cladding systems in contrast to current zirconium alloy cladding. The developed detailed understanding will serve to aid in relatively early screening of candidate systems to avoid wasted effort, guide development of new fuel forms, and to provide a basis for predicting and modeling fuel performance. Major deliverables for the project included: Thermochemical assessment and models of phases in the U-Si and U-Si-N systems; thermochemical evaluation supported by experimental measurements of fuel-cladding interactions of silicide fuel with baseline zirconium, ceramic composite, and ferritic alloy cladding; thermochemical assessment and models of phases supported by experimental measurements for silicide fuel with key fission products provided in a dataset and reported in refereed publications. Within the project a significantly refined U-Si phase diagram was developed and reported that now includes homogeneity ranges for key phases, such at the U 3 Si 2 proposed fuel phase, and settles issues with regard to uncertainty in the stability of some phases. Computational efforts together with key experiments has determined phase formation in interactions between U 3 Si 2 and Zircaloy-4 cladding material, a ferritic FeCrAlY alloy of interest as an advanced cladding material, and silicon carbide, also of interest as a fiber-reinforced composite cladding. As expected, very significant reactions occur between U3Si2 and Zircaloy-4, with much less interaction at higher temperatures for the ferritic alloy, and finally interactions with SiC only in the region of contact. A potentially major issue is the stability of U 3 Si 2 fuel that has undergone significant burnup. The result is the loss of the uranium metal, liberating silicon, and the formation of concomitant fission product elements that either dissolve in the U 3 Si 2 phase or form independent, and possibly silicide phases. A combination of experimental determinations of phase formation of U 3 Si 2 reacted with representative fission products yttrium, gadolinium, cerium, zirconium, and molybdenum and first principles calculations has helped understand the fuel chemistry. The behavior of the U 3 Si 2 phase and the partitioning of silicon to possible fission product phases with burnup was thus determined, with significant dissolution in U 3 Si 2 of cerium, gadolinium, zirconium, and plutonium predicted along with independent phase formation of a U-Mo-Si ternary phase, yttrium silicide, and elemental selenium. It can be concluded that at significant burnup there will be a very minor amount of the U 3 Si 2 fuel phase that will decompose to a lower silicide or a uranium alloy as silicon preferentially forms a secondary phase.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

BISON BWR Fuel Modeling Capability: Material Models (FY2020)

Until this year the BISON fuel performance code has been developed primarily for pressurized water reactor (PWR), accident tolerant fuel (ATF), and advanced reactor (e.g., tri-structural isotropic (TRISO), metallic) analyses. The main focus of this work is to develop and document required material models that would aid predicting cladding failure with a specific hydride distribution to be investigated for boiling water reactor (BWR) applications in the next fiscal year. In terms of materials, the primary differences between a BWR and PWR is the use of gadolinia doping of the UO 2 fuel, the use of Zircaloy-2 for the cladding, and the addition of a liner on the inner surface of the cladding for improved pellet-clad mechanical interaction (PCMI)performance. The liner is typically made of pure zirconium or a lower tin content zirconium alloy (e.g. Zr-0.3%Sn). This work details the development and documentation of material and behavioral models for BWR analysis such as the addition of material and behavior models for gadolinia doped UO 2 , pure zirconium, Zr-0.3%Sn, and Zircaloy-2 as well as the ease-of-use additions to allow internal meshing capabilities to include liners. Another important aspect affecting cladding performance is hydrogen diffusion and hydride precipitation in the cladding. A model was added previously for non-lined, homogeneous claddings. In this work, instructions are provided on how to apply the model to BWR liner cladding. Representative experimental values are provided for the hydrogen diffusion parameters and precipitation-dissolution kinetics for typical liner materials of interest.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Sister Rod Destructive Examinations (FY20) Appendix A: Full Length Rod Heat Treatments (FHT)

As a part of the US DOE-NE High Burnup Spent Fuel Data Project, ORNL is performing destructive examinations (DEs) of high burnup (HBU) (>45 gigawatt days per metric ton uranium) spent nuclear fuel (SNF) rods from the North Anna Nuclear Power Station operated by Dominion Energy. The SNF rods, called the “sister rods,” are all HBU and include four different kinds of fuel rod cladding: standard Zircaloy-4, low-tin Zircaloy-4, ZIRLO®, and M5®. The DEs are being conducted to obtain a baseline of the HBU rod’s condition prior to dry storage and are focused on understanding overall SNF rod strength and durability. Both composite fuel and empty cladding are being tested. While the data generated can be used for multiple purposes, a primary goal for obtaining the post-irradiation examination data will support SNF dry storage licensing and relicensing activities.This report documents the status of the ORNL Phase 1 DE activities related to full length rod heat treatments (FHT) applied to selected sister rods in Phase 1 of the sister rod test program. The results of this work and detailed examinations are summarized in the Sister Rod DE Status Report.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Sister Rod Destructive Examinations (FY20) Appendix B: Segmentation, Defueling, Metallograhic Data and Total Cladding Hydrogen

As a part of the US DOE-NE High Burnup Spent Fuel Data Project, ORNL is performing destructive examinations (DEs) of high burnup (>45 gigawatt days per metric ton uranium) spent nuclear fuel (SNF) rods from the North Anna Nuclear Power Station operated by Dominion Energy. The SNF rods, called the “sister rods,” are all HBU and include four different kinds of fuel rod cladding: standard Zircaloy-4, low-tin Zircaloy-4, ZIRLO®, and M5®. The DEs are being conducted to obtain a baseline of the HBU rod’s condition prior to dry storage and are focused on understanding overall SNF rod strength and durability. Both composite fuel and empty cladding are being tested. While the data generated can be used for multiple purposes, a primary goal for obtaining the post-irradiation examination data and the associated measured mechanical properties is to support SNF dry storage licensing and relicensing activities.This report documents the status of the ORNL Phase 1 DE activities related to: rough segmentation, defueling, optical microscopy, and cladding total hydrogen measurements for 7 Phase 1 sister rods and outlines the DE tasks performed and the data collected to date. The results of these detailed examinations and others are summarized in the Sister Rod DE Status Report.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Post Examination of Candidate NpO 2 Targets for 238 Pu Production

Four targets composed of sintered NpO 2 pellets enclosed in Zircaloy cladding were irradiated in the High Flux Isotope Reactor for 2 to 4 cycles to determine if an oxide pellet and Zircaloy cladding would be usable candidates for 238 Pu production. The pellets were sintered to a high fraction of theoretical density (TD) and melt wires were placed in small holes that had been drilled in the center of selected pellets to determine if the pellet centers exceeded desirable operating temperatures. After irradiation, the targets were punctured to determine the internal target pressure and the fission gas release. None of the targets had excessive pressure, and fission gas release was in the range of 4 to 38%. The targets were then cut into segments for radiochemical analysis, and metallography (MET) mounts were created to examine the pellet microstructure and to search for the melt wires to determine if they had melted. Three of the four targets resulted in successful MET mounts; the two-cycle pellets were too friable to be handled. No signs of pellet melting were noted, and unfortunately, none of the melt wires could be recovered. The results indicate that this pellet/clad design offers a practical option for 238 Pu production.

36 MATERIALS SCIENCE↗

DOE OSTI2022

BISON Validation to In-Situ Cladding Burst Test and High Burnup LOCA Experiments

The process to develop and qualify nuclear fuels for commercial nuclear application requires fundamental material development, characterization, and design; out-of-pile testing on unirradiated materials; integral fuel rod irradiations, testing, and post irradiation examinations (PIEs); and transient analyses. The historical approach depends on the generation of large empirical datasets and series of integral fuel rod irradiations, and this approach ultimately takes approximately 20 years—or sometimes longer—to acquire data through extensive sequential testing. Thus, the qualification and eventual deployment of new fuel systems constitute a long and drawn-out process. However, recent technological advancements have provided researchers the opportunity to perform out-of-cell, in-situ measurements to assess material performance for the duration of the experiment. One such example of this capability is the use of digital image coordination and thermal imaging to assess Zircaloy cladding performance under a simulated loss-of-coolant accident (LOCA) transient condition. In general, the in-situ measurements provide high-fidelity strain, strain rates, and temperature surface maps. This is critical for the United States nuclear industry, which is actively developing a technical basis to support extending the peak rod average burnup from 62 to ~75 GWd/tU and the deployment of accident-tolerant fuel. However, the Nuclear Regulatory Commission, through their research information letter, outlined a number of technical issues for the industry to address before extending burnup. One topic of specific interest is understanding the cladding balloon and rupture geometry during the LOCA heatup phase. Leveraging these advanced in-situ capabilities, this work intends to use insitu data generated from a simulated LOCA in the Severe Accident Test Station at Oak Ridge National Laboratory to better understand high-temperature creep and its impact on Zircaloy balloon and rupture performance. This work used the BISON fuel performance code to compare BISON’s high-temperature creep model predictions to in-situ data and identify limitations and gaps within the model. Additionally, BISON will subsequently be used to simulate relevant high-burnup LOCA tests. The results will be analyzed and compared to the available post-test data in a manner consistent with the approach outlined in the Nuclear Regulatory Commission research information letter.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Improving Ductility of Hydride Embrittled Zirconium (Final Report)

One of the main limiting factors on the lifetimes of nuclear fuel rod claddings is the formation of hydrides and associated detrimental effects on mechanical properties. In this study, we examined the behavior of hydrides in zirconium and zircaloy-4 after tensile stress is applied to determine whether the more ductile γ-ZrH phase was stabilized by the mechanical stress. We did not find a significant increase in the ratio of γ-ZrH phase to δ-ZrH1.5 phases after tensile stress is applied in previously hydrided metals. Previous reports indicate that this stabilization does occur when zircaloy is stressed and hydrided simultaneously, indicating that the formation of the γ-ZrH phase may reverse upon relaxation or may require the stress in-situ during the hydriding process to form in significant quantities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Sister Rod Destructive Examinations (FY23) Appendix F3: Uncertainty and Conservative Bias in the Cyclic Integrated Reversible-Bending Fatigue Test

The development and application of the Cyclic Integrated Reversible-Bending Fatigue Tester (CIRFT) has been documented over the past 10 years. The CIRFT system was developed in collaboration with the U.S. Nuclear Regulatory Commission (NRC) to address the concern that high-burnup fuel rod fatigue performance was degraded compared to cladding-only behavior. Fatigue data measured by CIRFT on high-burnup fuel rods were then used by the NRC to develop a fatigue response curve for pressurized water reactor fuel rods with Zircaloy-4 cladding in NUREG-2224. Subsequently, CIRFT has been used in the sister rod project to test whether reoriented hydrides associated with vacuum drying influenced the fatigue lifetime, to extend the fatigue testing database to include fuel rods with ZIRLO cladding, and to add to the experience on both Zircaloy-4 and M5 cladding. These data will be used as a reference for subsequent characterization of fuel rods removed from the high-burnup demonstration cask to better understand the effects of long-term dry storage, which can be thought of as a multiyear elevated temperature anneal. The objective of fatigue testing is to provide data that can be used to develop a best-estimate fatigue curve and a conservative fatigue design curve that accounts for uncertainty and can be compared with actual transportation conditions. The process for defining a design fatigue curve for commercial used fuel rods was developed by Oak Ridge National Laboratory (ORNL) in FY22. One issue noted in the fatigue evaluation was that the calculated combined uncertainty in the strain amplitude values determined from the measured data was large. It was proposed then to directly measure the uncertainty in the strain amplitude to either validate the calculated combined uncertainty or update the uncertainty based on the measurement data. Thus, the purpose of this appendix is to document the measured uncertainty in the strain amplitude data. In the process, it was determined that there has been a conservative bias in the calculated strain amplitude that is small enough to be within the measurement uncertainty. This observation is discussed herein, and a case is made to continue to include the conservative bias in the data.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Evaluation of Mechanistic and Empirical Models against Existing FFRD and LOCA Experimental Databases

The desire of the nuclear industry to improve the economics of existing nuclear power plants has necessitated research into the potential of a phenomenon known as fuel fragmentation, relocation, and dispersal (FFRD). This phenomenon is possible during a loss-of-coolant accident (LOCA) at relatively high burnup. The Nuclear Energy Advanced Modeling and Simulation program has been developing simulation capabilities for FFRD and LOCA in the BISON fuel performance code for multiple years. This year, the effort has been focused on evaluating new lower length scale informed pulverization thresholds as well as updating and adding new empirical models for various phenomena. Models added or updated this year include a preliminary transient fission gas release model, new high-temperature Zircaloy creep models, a Zircaloy rupture opening area model, and a temperature-dependent emissivity during radiation from the fuel rod to the surrounding atmosphere. The models are verified through implementation tests to demonstrate code correctness after addition to BISON. The models are then assessed against a subset of the existing BISON validation suite for LOCA and FFRD cases. Two new cases, Studsvik Rods 192 and 193, have been added. The results indicate that the inclusion of a bubble pressure evolution model in the bubbles in the high-burnup structure has the largest impact compared to the 3D fracture criterion on reducing the calculated amount of pulverized fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Hydrogen and Deuterium Reactivity with Carbon Surface Impurities on the TPBAR Getter Ni Plate Studied in situ with Environmental XPS

Tritium for the U.S. Department of Energy’s Tritium Readiness Program is produced in tritium-producing burnable absorber rods (TPBARs) inserted into light-water nuclear reactors. The rods are stainless-steel-clad tubes with a permeation barrier coating and internal components. The internal components have been designed and selected to produce and retain tritium. The TPBAR incorporates a Ni-plated Zircaloy-4 getter tube to capture tritium and prevent it from reaching the rod cladding and permeating into the environment. The role of the Ni coating is to protect the Zircaloy-4 getter from oxidation while allowing for maximum tritium permeability. Ubiquitous surface impurities on the Ni, such as carbon, could limit its protective functionality and permeability if they exist in relatively large concentrations. The reactivity of impurity carbon with permeating tritium can also result in tritiated hydrocarbon impurities on the gas phase. The goal of this work is to determine quantitatively the chemical state and reactivity of potential Ni coating impurities in actual TPBAR getter samples. Using Environmental X-ray Photoelectron Spectroscopy (eXPS), a very sensitive gas/surface chemistry diagnostic, we reveal in situ the source and evolution of carbon on the Ni surface at different hydrogen and deuterium pressure conditions, and how carbon reactivity may result in hydrocarbon gas-evolution at application-relevant temperatures.

36 MATERIALS SCIENCE↗

NASA NTRS1979

Diffusion and phase change characterization by mass spectrometry

The high temperature diffusion of trace elements in metals and alloys was investigated. Measurements were made by high sensitivity mass spectrometry in which individual atoms were detected, and quantitative data was obtained for zircaloy-2, 304 stainless steel, and tantalum. Additionally, a mass spectrometer was also an analytical tool for determining an allotropic phase change for stainless steel at 955 C, and a phase transition region between 772 C and 1072 C existing for zircaloy-2. Diffusion rates were measured in thin (0.001" (0.0025 cm) and 0.0005" (0.0013 cm)) ribbons which were designed as high temperature thermal ion sources, with the alkali metals as naturally occurring impurities. In the temperature and pressure regime where diffusion measurements were made, the solute atoms evaporated from the ribbon filaments when the impurities diffused to the surface, with a fraction of these impurity atoms ionized according to the Langmuir-Saha relation. The techniques developed can be applied to many other alloys important to space vehicles and supersonic transports; and, with appropriate modifications, to the diffusion of impurities in composites.

Koslin, M. E.↗

DOE OSTI2021

Fatigue Test Result for High Burnup Pressurized Water Reactor Rods

The High Burnup Spent Fuel Data Project, sponsored by DOE-NE, is focused on understanding the effects of long-term storage and transportation on high burnup (HBU) (>45 gigawatt days per metric ton uranium) light water reactor fuel. The experiment includes 32 HBU spent nuclear fuel (SNF) assemblies that will be stored in a typical Independent Spent Fuel Storage Installation (ISFSI) and 25 sister rods - nine SNF rods that were removed from the fuel assemblies prior to insertion to the ISFSI and 16 SNF rods removed from similar HBU assemblies. The sister rods provide a baseline of the condition of the HBU rods prior to loading, drying, and long-term dry storage. Destructive examinations of the sister rods are focused on understanding overall SNF rod strength and durability. Both composite fuel and empty cladding will be tested to derive material properties. While the data generated can be used for multiple purposes, a primary goal of the sister rod PIE data and associated measured mechanical properties is to support existing fuel storage licensing and relicensing activities by addressing identified knowledge gaps, and enhance the technical basis for post-storage transportation, handling, and consolidation activities. Fatigue tests of HBU M5-clad, ZIRLO-clad, Zircaloy-4, and low tin Zircaloy-4 segments have been completed using ORNL’s Cyclic Integral Reversible Fatigue Tester (CIRFT). This is the first time ZIRLO-clad rods have been tested. Some of the segments were heat-treated to understand the effects of thermal transients such as those encountered during dry storage vacuum drying on the fatigue lifetime. This paper presents results of the fatigue tests obtained to date and discusses planned future tests.

Montgomery, Rose↗