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At least 289 records · Page 16

Time Domain Thermoreflectance (TDTR) Studies of Microstructural Characterization of as-Fabricated and/or Irradiated TPBAR Components

Paddock et al. demonstrated for the first-time the measurement of thermal diffusivity from thin metal films using picosecond transient thermoreflectance in 1986. This project attempted to use a similar experimental setup based on a femtosecond time domain thermoreflectance (TDTR) to measure the damage to the crystal lattice of LiAlO 2 from irradiation in the reactor and production of tritium and helium. The TDTR is based on a pump-probe laser configuration where the pump laser is used to heat the sample and the probe laser is used to follow the thermal evolution created by the pump laser. The goal for this project is to measure the differences in thermal diffusivity between LiAlO 2 and the irradiated Li AIO 2 sample in a reactor. Unfortunately, COVID-19 restricted laboratory research time and the availability of researchers capable to conduct TDTR work. In addition, the ultrafast laser (Astrella 35fs laser) required to conduct the work was inoperable making this particulate work impossible to conduct in FY20 and FY21. The purpose of the thermal diffusion measurements with a TDTR setup is to probe the damage and disorder to the crystal lattice of pristine and irradiated samples. Since TDTR was not available for this work, a different approach using Raman and luminescence spectroscopy was used to characterize the crystal lattice damage in LiAlO 2 from irradiation.

07 ISOTOPE AND RADIATION SOURCES↗

Prediction of Probabilistic Shock Initiation Thresholds of Energetic Materials Through Evolution of Thermal-Mechanical Dissipation and Reactive Heating

The ignition threshold of an energetic material (EM) quantifies the macroscopic conditions for the onset of self-sustaining chemical reactions. The threshold is an important theoretical and practical measure of material attributes that relate to safety and reliability. Historically, the thresholds are measured experimentally. In this work, we present a new Lagrangian computational framework for establishing the probabilistic ignition thresholds of heterogeneous EM out of the evolutions of coupled mechanical-thermal-chemical processes using mesoscale simulations. Furthermore, the simulations explicitly account for microstructural heterogeneities, constituent properties, and interfacial processes and capture processes responsible for the development of material damage and the formation of hotspots in which chemical reactions initiate. The specific mechanisms tracked include viscoelasticity, viscoplasticity, fracture, post-fracture contact, frictional heating, heat conduction, reactive chemical heating, gaseous product generation, and convective heat transfer. To determine the ignition threshold, the minimum macroscopic loading required to achieve self-sustaining chemical reactions with a rate of reactive heat generation exceeding the rate of heat loss due to conduction and other dissipative mechanisms is determined. Probabilistic quantification of the processes and the thresholds are obtained via the use of statistically equivalent microstructure sample sets (SEMSS). The predictions are in agreement with available experimental data.

36 MATERIALS SCIENCE↗

In-situ visualization of the transition metal dissolution in layered cathodes

Transition metal dissolution in layered cathodes is one of the most intractable issues that deteriorates the battery performance and lifetime. It not only aggravates the structure degradation in cathode, but also damages the solid electrolyte interphase in anode and even induce the formation of lithium dendrites. In this work, we investigate the dissolution behaviors of polycrystalline and single-crystalline layered cathode via operando X-ray imaging techniques. The described cathode particle morphology appears to have a significant impact on the evolution of the dissolution dynamics. As a mitigation strategy, we reveal that doping with trace amount of Zr in the layered cathode could improve its robustness against the transition metal dissolution. Our finding provides valuable insights for designing the next-generation highly-stable layered battery cathodes.

25 ENERGY STORAGE↗

Self-Learning Kinetic Monte Carlo Simulations of Radiation Damage in Nuclear Fuels

Understanding how irradiation affects the thermo-physical and mechanical properties of nuclear materials, such as thermal conductivity degradation in fuels and embrittlement of structural components, is critical to the safety and efficiency of nuclear reactors. These effects are largely governed by the formation and evolution of atomic-scale point defects and defect clusters. Due to their small sizes, however, these defects are invisible under high-resolution scanning transmission electron microscopy. This project aims to fill this experimental knowledge gap by integrating density functional theory (DFT), machine learning interatomic potential (MLIP), and kinetic Monte Carlo (KMC) techniques to predict longtime evolution of irradiation-induced defects in nuclear fuels.

36 - MATERIALS SCIENCE↗

Irradiation-induced shift in the thermodynamic stability of phases and the self-healing effect in transformative high entropy alloys

Here, this work investigated Fe 40 Mn 20 Cr 15 Co 20 Si 5 high entropy alloy (CS-HEA), which exhibits transformation induced plasticity (TRIP) from γ-fcc → ε-hcp, as a probable candidate for nuclear applications. CS-HEA is an extensively-explored, low stacking fault energy alloy with superior strength, ductility, fatigue resistance, and corrosion resistance. This study delved into the effect of irradiation on the shift in thermodynamic stability of the phases and thus radiation tolerance. The evolution of phases, lattice parameters, and transformation volume, V γ→ε , were evaluated from X-ray diffraction experiments along with the mechanical response from nanoindentation. The alloy exhibited a recently-proposed novel self-healing mechanism possible due to the TRIP effect to minimize irradiation damage by restraining the γ-fcc → ε-hcp transformation via thermal aid; this self-healing mechanism was confirmed by transmission electron microscopy. The results were corroborated by a negative change in V γ→ε and a low |V γ→ε |, which is an important criterion for recovery of parent γ-fcc phase. Thus, this alloy was deemed a good radiation-tolerant candidate for nuclear application.

36 MATERIALS SCIENCE↗

A concurrent irradiation-mechanics multiscale coupling model

The vast majority of our current knowledge regarding the basic mechanisms controlling irradiation effect on mechanical properties is based almost entirely on the results of post-irradiation experiments or theoretical models. However, the concurrent effects of irradiation, mechanical stress, and thermal damage on the failure phenomena of materials and components remain largely unexplored due to its internal multiscale-multiphysics coupling nature. Here, we present here a concurrent irradiation-mechanics multiscale coupling model. The concurrent evolutions of nanoscale irradiation defect clusters, microscale dislocation configurations, and mechanical responses are well captured based on coupling cluster dynamics, discrete dislocation dynamics, and the finite element methods using an effective time marching scheme. Model predictions of defect densities and size are in general agreement with experimental observations. Irradiation hardening is shown to take place also in samples undergoing concurrent irradiation-mechanical loading, similar to samples tested post-irradiation. However, the occurrence of plastic flow localization and dislocation channel formation is not accompanied with apparent yield drop (softening) under concurrent irradiation-mechanical loading conditions, which is different from the post-irradiation case.

42 ENGINEERING↗

The effects of dose, dose rate, and irradiation type and their equivalence on radiation-induced segregation in binary alloy systems via phase-field simulations

Radiation-induced segregation is a phenomenon commonly observed in many alloys which consists of the redistribution of elements (solute or interstitial impurities) under irradiation. The onset and development of radiation-induced segregation can only occur when a sufficient flux of defects is sustained and defect sinks are present. Irradiation dose, dose rate, and particle types all affect defect flux. In this work, we employ a phase-field model to examine the effects of dose, dose rate, and type of incident particles on radiation-induced segregation behavior in a model binary alloy. The phase-field model takes into account the formation and evolution of point defects as well as defect clusters, the diffusion and clustering of alloy species, the presence of additional extrinsic defect sinks in the form of dislocations, and two different methods of radiation-damage insertion, which are intended to simulate either light-ion/electron irradiation via Frenkel pairs or heavy-ion irradiation in the form of cascades. Our results show a dose-rate and particle-type dependence on the amount of solute segregation. We show that the material systems exposed to higher dose rates are less subjected to solute segregation at equivalent doses. We also show that such dose-rate-dependence behavior is due to a delay of the incubation dose at which radiation-induced segregation effectively starts. Particle type and the presence of dislocations can accentuate this behavior. Our model predictions correlate with many experimental observations made over the years on radiation-induced segregation providing credence to the simulation results. The methodology presented in this study allows for a first-order prediction of the dose rate at which proxy irradiation experiments could be performed to approximate radiation-induced segregation behaviors seen in targeted irradiation conditions.

36 MATERIALS SCIENCE↗

Influence of Powder Characteristics and Processing Methods on Creep Performance of Powder Metallurgy Hot Isostatic Pressed SS316

The U.S. nuclear energy expansion goals are driving the demand for manufacturing routes that can rapidly produce large, complex, near net shape components. Powder metallurgy hot isostatic pressing (PM HIP) is an advanced manufacturing technique that can be economically scaled-up, while alleviating the supply chain challenges that forging and casting face in terms of cost and lead time constraints. This makes PM-HIP a viable technology to aid and accelerate large-scale part manufacturing for nuclear applications. However, large-scale qualification and deployment of this technology require a thorough understanding of the influence of powder feedstock quality, powder handling history, hot isostatic pressing (HIP) parameters, and subsequent heat treatment on microstructural evolution and elevated temperature mechanical performance. The present work focusses on 316 austenitic stainless steel (SS316) which is most commonly used in high temperature environments for nuclear applications Results from this study show that PM HIPed SS316 meets ASME tensile requirements at room temperature and at elevated temperature. However, creep performance of PM-HIPed SS316 remains inferior to its wrought counterpart, demonstrating that tensile performance alone is not a reliable metric for long duration high temperature integrity. Further, this report delineates powder derived microstructural features that govern creep damage, with key evidences pointing to “microstructural inheritance” from gas atomized powder feedstocks. Commercial SS316 powders of varying chemical compositions and recycling histories were studies, and the results showed large differences in elemental segregation, oxide surface layers and secondary phase distributions. Multi-scale characterization revealed segregation of chromium, molybdenum, manganese and silicon at the boundaries and the precipitation of manganese-, silicon-, and molybdenum-oxides. During HIP consolidation, these surface oxides transform into decorated prior particle boundaries (PPBs) and grain boundary inclusions that persist through conventional post-HIP solution annealing treatment. The retained oxides in post-HIP microstructures were found to influence grain growth, precipitation behavior, and ultimately creep cavitation and fracture. Such post-HIP heat treatments are therefore limited by a complex trade-off between grain growth, and oxide coarsening which aggravate creep damage by acting as nucleation sites for cavities. The objective of this work is to establish an integrated processing–structure–property framework for PM-HIP 316 stainless steel by investigating the influence of powder feedstock characteristics in pre- and post-HIP processing as well as to understand the significance of post-HIP heat treatment on microstructural evolution and creep properties. The results from this report emphasize the significance of powder feedstock integrity in improving creep performance of PM-HIPed SS316, by highlight the effect of rapid solidification, elemental segregation, oxide formation and powder recycling on microstructural defect inheritance following HIP consolidation. Rather than considering HIP processing, solution annealing, and mechanical performance independently, this report treats powder production, HIP consolidation, post-HIP thermal processing, and creep deformation as interconnected stages within a continuous metallurgical process. The resulting framework will provide a scientific basis for developing feedstock engineering strategies capable of improving long-term reliability of PM-HIP stainless steels and accelerating their qualification for advanced nuclear applications.

Ajjarapu, Pavan [Oak Ridge National Laboratory (OR↗

Contributions to the mechanistic understanding of the microstructural evolution in irradiated U-Mo dispersion fuel

Here, advanced microstructural characterization techniques, such as scanning electron microscopy (SEM) and scanning transmission electron microscopy - energy dispersive x-ray spectroscopy (STEM-EDS), were used to interpret the fuel microstructure evolution and fission products behavior in U-Mo dispersion fuel irradiated in the Advanced Test Reactor (ATR) as part of the European Mini-Plate Irradiation Experiment (EMPIrE) test. The larger as-fabricated fuel grain size achieved by heat-treating the U-Mo powder resulted in slower high burnup structure (HBS) development and reduced fission gas porosity. Slower HBS kinetics was observed at the fuel kernels’ periphery, which contained smaller and less fission gas bubbles at all fission densities (FDs) investigated and was attributed to a locally reduced damage density and fission products concentration, as corroborated with Monte Carlo simulations. The non-refined grains at the fuel kernel periphery hosted a perfectly ordered fission Gas Bubble Superlattice (GBS) up to 6.3 × 10 21 fissions/cm 3 . Nano-scale STEM-EDS analysis presented in this study provided useful information on the GBS characteristic morphology and evolution in U-Mo fuel. The concentration of fission gas in the GBS progressively increased with FD, pointing to an evolution of the nanobubble pressure status with irradiation. A possible connection between the GBS collapse and HBS onset is proposed for which there exists a threshold in the misorientation of the refined sub-grains above which the GBS stability during irradiation is no longer preserved, resulting in the GBS collapse.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Back to functional hydrides: Effects of neutron-irradiated microstructure on hydrogen retention in yttrium hydride

Functional hydrides are promising candidates for advanced nuclear reactors, particularly in portable or transportable applications, due to their high hydrogen-retention capabilities, enabling efficient neutron moderation, and compact reactor design. However, hydrogen mobility in hydrides at elevated irradiation temperatures poses significant technological challenges, necessitating a comprehensive understanding of their irradiation behavior. Furthermore, this study investigated the microstructural and chemical stability of neutron-irradiated yttrium hydrides to assess their hydrogen-retention capacity. A targeted literature review was also conducted to contextualize neutron-irradiation effects on functional hydrides with regards to structural stability and hydrogen retention. Experimental characterizations revealed that, at high temperatures, irradiated hydrides retained their phase stability, which was likely enhanced by irradiation-induced microstructure evolution. Notably, an amorphous yttrium and oxygen -rich surface layer was present at the free surface of the hydride. Its thickness decreased while a continuous crystalline Y-O-rich layer was formed with increasing neutron damage. Additionally, the number density of dislocation loops and cavities generally increased as a function of neutron dose. First-principles calculations of hydrogen behavior within yttrium vacancy clusters in yttrium hydrides demonstrated vacancy-size-dependent hydrogen stability and configuration, highlighting the role of vacancy geometry in regulating hydrogen retention. Thus, the presence of irradiation-induced dislocation loops and cavities were hypothesized to improve hydrogen retention. Collectively, these findings advance the understanding of hydride behavior under neutron irradiation as well as their technological readiness for portable or transportable nuclear reactors.

Defect clusters↗

Computational Elucidation of Mechanical Degradation in NMC Cathodes: Impact on Cell Performance

Next-generation lithium ion batteries are expected to demonstrate superior energy and power density with longer cycle life for successful electrification of the automobile, aviation, and marine industries. Adoption of lithium metal anodes with solid electrolytes can help to achieve that goal given that the dendrite-related issues are solved eventually. Another possibility is to use Ni-rich high-capacity NMC cathode materials with liquid and/or solid electrolytes, which presently experiences rapid capacity fade while charged to higher voltages. Several mechanical and chemical degradation mechanisms are active within these NMC-based cathode particles. Recent experimental research activities attempted to correlate the mechanical damage with the capacity fade experienced by Ni-rich LiNi x Mn y Co z O 2 (x+y+z = 1) (NMC) cathodes. Here, a computational framework is developed in this study capable of quantifying the evolution of inter primary particle and cathode/electrolyte interfacial fracture experienced by the poly- and single-crystalline NMC cathodes during charge/discharge operation. Influences of mechanical degradation on the overall cell capacity, while operating with liquid and/or solid electrolytes, are successfully characterized. Decreasing the size of the cathode primary particles, or the size of the single-crystalline cathodes, can mitigate the overall mechanical degradation, and subsequent capacity fade, experienced by NMC cathodes. The developed theoretical methodology can help the engineers and scientists to better understand the mechanical degradation mechanism prevalent in Ni-rich NMC cathodes and build superior lithium ion-based energy storage devices for the application in next-generation devices.

25 ENERGY STORAGE↗

Geologic Risk Assessment Activities at SECARB Cranfield, MS Site

Risk Assessment (RA) of RCSP Phase 3 sites is a DOE requirement and valuable to DOE’s program because this process encourage careful consideration of elements that could damage an individual project, or if severe ,damage credibility and public commercial acceptance of the sequestration process. Poor outcomes even from small projects can have negative consequences larger than the cost to the individual project. In addition, practice in risk assessment compared to project evolution is needed as part of the confidence-building toward future large scale, long term industrial activities.

01 COAL, LIGNITE, AND PEAT↗

Analysis of Radiological Release From Fueled Irradiation Experiments During Manual Handling (Slides)

Irradiation experiments are manually handled at the Advanced Test Reactor (ATR) by qualified operators using long handled tools. Standard handling evolutions include insertion and removal from the reactor vessel, transfer to/from a storage location or cask in the ATR canal, and handling/reconfigurations at a canal working tray. Such routine handling has the potential to result in mechanical damage to the experiment boundary which is credited to retain fission products. Since damage can occur due to operator error, this is an anticipated occurrence. This work determines the radiological consequences to receptors inside the ATR facility, as well as public receptors. Given the wide variety of fuel types tested at the ATR, a generic approach to the analysis is taken. The radiological inventory is determined to bound a variety of fuel types (e.g., ceramic and molten fuel matrices) and fission powers on the U-235 enrichment spectrum. The source term analysis considers different release fractions to bound different fuel types and burnups. The postulated handling events occur underwater; thus, retention of the released isotopic content is considered within the canal water column. Retention of radionuclides in the water column is determined using a modified approach of United States (US) Nuclear Regulatory Commission (NRC) Regulatory Guide (RG) 1.183. Radiological dose to the facility receptor is determined using a compartment release model. Dose to the public receptor is determined using atmospheric dispersion models using site specific atmospheric conditions with the use of the Radiological Safety Analysis Computer (RSAC) program version 7.2.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗

Diffusion-mediated chemical concentration variation and void evolution in ion-irradiated NiCoFeCr high-entropy alloy

High-entropy alloys (HEAs) are proposed as potential structural materials for advanced nuclear systems, but little is known about the response of matrix chemistry in HEAs upon irradiation. Here, we reveal a substantial change of matrix chemical concentration as a function of irradiation damage (depth) in equiatomic NiCoFeCr HEA irradiated by 3 MeV Ni ions. After ion irradiation, the matrix contains more Fe/Cr in depth shallower than ~900–1000 nm but more Ni/Co from ~900–1000 nm to the end of the ion-damaged region due to the preferential diffusion of vacancies through Fe/Cr. Preferential diffusion also facilitates migration of vacancies from high radiation damage region to low radiation damage region, leading to no void formation below ~900–1000 nm and void formation around the end of the ion-damaged region at a fluence of 5 × 10 16 cm -2 (~123 dpa, displacements per atom, peak dose under full cascade mode). As voids grow significantly at an increased fluence (8 × 10 16 cm -2 , 196 dpa), the matrix concentration does not change dramatically due to new voids formed below ~900–1000 nm.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Diffusion-mediated chemical concentration variation and void evolution in ion-irradiated NiCoFeCr high-entropy alloy

High-entropy alloys (HEAs) are proposed as potential structural materials for advanced nuclear systems, but little is known about the response of matrix chemistry in HEAs upon irradiation. Here, we reveal a substantial change of matrix chemical concentration as a function of irradiation damage (depth) in equiatomic NiCoFeCr HEA irradiated by 3 MeV Ni ions. After ion irradiation, the matrix contains more Fe/Cr in depth shallower than ~900–1000 nm but more Ni/Co from ~900–1000 nm to the end of the ion-damaged region due to the preferential diffusion of vacancies through Fe/Cr. Preferential diffusion also facilitates migration of vacancies from high radiation damage region to low radiation damage region, leading to no void formation below ~900–1000 nm and void formation around the end of the ion-damaged region at a fluence of 5 × 10 16 cm –2 (~123 dpa, displacements per atom, peak dose under full cascade mode). As voids grow significantly at an increased fluence (8 × 10 16 cm –2 , 196 dpa), the matrix concentration does not change dramatically due to new voids formed below ~900–1000 nm.

36 MATERIALS SCIENCE↗

Recent Studies on Void Shrinkage in Metallic Materials Subjected to In Situ Heavy Ion Irradiations

The continuous formation and growth of voids induced by radiations in metallic materials may lead to significant microstructure damage and degradation of mechanical properties. In sharp contrast to the void swelling commonly observed in irradiated metallic materials, nanovoids in nanoporous metallic materials are found to shrink during radiation and thus nanovoids enhance the radiation tolerance of metallic materials. This article reviews recent studies on size-dependent void shrinkage in metallic materials subject to in situ heavy ion irradiation. Furthermore, we demonstrate the capability of machine learning in identifying and tracking the evolution of nanovoids. Finally, the physical mechanisms of radiation induced void shrinkage revealed by simulation studies are briefly summarized.

36 MATERIALS SCIENCE↗

In Situ Micro-Pillar Compression to Examine Radiation-Induced Hardening Mechanisms of FeCrAl Alloys

Here, the effects of 5 MeV Fe 2+ ion irradiation at 300°C on the microstructure evolution and deformation behavior of a FeCrAl C26M alloy are presented. It has been found that dislocation loop density increases an order of magnitude from 1 dpa to 16 dpa irradiations, whereas, the dislocation loop size saturates with increasing damage. Micropillars, 600 nm in diameter and 1.3 µm in height, were fabricated and compressed inside grains with <001>, <011> and <111> crystallographic orientations, respectively. {112} <111> has been identified as the primary slip system in both unirradiated and irradiated alloy. The increase in yield stress after irradiation is observed with measurable variation along <001> and <011> vs. along <111>. By applying the Orowan dispersed barrier model, the increase of yield stress is found mainly due to the slip resistance of radiation generated defect loops. Detailed transmission electron microscopy (TEM) studies were performed to quantify the Burgers vector and the distribution of irradiation induced dislocations at elevated strains. It is revealed that localized shear instability is caused by avalanche slip events of ½<111> dislocations gliding out of tested pillars. Simultaneously, a large number of sessile/immobile <100> dislocations formed in the vicinity of slip band, leading to the hardening at elevated strains.

36 MATERIALS SCIENCE↗

2020 Annual Report of Available Drawdowns for Each Oil Storage Cavern in the Strategic Petroleum Reserve

The Department of Energy maintains an up-to-date documentation of the number of available full drawdowns of each of the caverns owned by the Strategic Petroleum Reserve (SPR). This information is important for assessing the SPR's ability to deliver oil to domestic oil companies expeditiously if national or world events dictate a rapid sale and deployment of the oil reserves. Sandia was directed to develop and implement a process to continuously assess and report the evolution of drawdown capacity, the subject of this report. A cavern has an available drawdown if after that drawdown, the long-term stability of the cavern, the cavern field, or the oil quality are not compromised. Thus, determining the number of available drawdowns requires the consideration of several factors regarding cavern and wellbore integrity and stability, including stress states caused by cavern geometry and operations, salt damage caused by dilatant and tensile stresses, the effect of enhanced creep on wellbore integrity, and the sympathetic stress effect of operations on neighboring caverns. A consensus has now been built regarding the assessment of drawdown capabilities and risks for the SPR caverns. The process involves an initial assessment of the pillar-to-diameter (P/D) ratio for each cavern with respect to neighboring caverns. A large pillar thickness between adjacent caverns should be strong enough to withstand the stresses induced by closure of the caverns due to salt creep. The first evaluation of P/D includes a calculation of the evolution of P/D after a number of full cavern drawdowns. The most common storage industry standard is to keep this value greater than 1.0, which should ensure a pillar thick enough to prevent loss of fluids to the surrounding rock mass. However, many of the SPR caverns currently have a P/D less than 1.0 or will likely have a low P/D after one or two full drawdowns. For these caverns, it is important to examine the structural integrity with more detail using geomechanical models. Finite-element geomechanical models have been used to determine the stress states in the pillars following successive drawdowns. By computing the tensile and dilatant stresses in the salt, areas of potential structural instability can be identified that may represent "red flags" for additional drawdowns. These analyses have found that many caverns will maintain structural integrity even when grown via drawdowns to dimensions resulting in a P/D of less than 1.0. The analyses have also confirmed that certain caverns should only be completely drawn down one time. As the SPR caverns are utilized and partial drawdowns are performed to remove oil from the caverns (e.g., for occasional oil sales authorized by the Congress or the President), the changes to the cavern caused by these procedures must be tracked and accounted for so that an ongoing assessment of the cavern's drawdown capacity may be continued. A proposed methodology for assessing and tracking the available drawdowns for each cavern was presented in Sobolik et al. (2018). This report includes an update to the baseline drawdowns for each cavern, and provides an initial assessment of the evolution of drawdown expenditure for several caverns

02 PETROLEUM↗