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At least 811 records · Page 45

Modeling aerosol transmission spectra from n(λ) and k(λ) infrared optical constants measurements of organic liquids and solids

The effects of light scattering and refraction play significantly different roles for aerosols than for bulk materials, making it challenging to identify aerosolized chemicals using traditional spectral methods or spectral reference libraries. Due to a potentially infinite number of particle morphologies, sizes, and compositions, constructing a database of laboratory-measured aerosol spectra is not a practical solution. Here, as an alternative approach, the measured n / k optical vectors of two example organic materials (diethyl phthalate and D-mannitol) are used in combination with particle absorption / scattering theory (Mie theory and FDTD) and the Beer-Lambert law to generate a series of synthetic infrared transmission / scattered light spectra. The synthetic spectra show significant differences versus simple slab transmission spectra, even for small changes in particle size (e.g., 5 vs. 10 µm) for both single particles and ensembles, potentially serving as useful reference data for aerosol sensing. For spherical single particles with diameters of 1 to 10 µm, FDTD simulations predict changes in the magnitudes of spectral shifts and the shapes of the peaks vs. particle size with only small deviations from Mie theory predictions, yet reliably capture the direction of the shifts. Typical spectral peak shifts in the longwave infrared correspond to Δλ ∼0.20 µm (∼34 cm -1 ) when compared to corresponding slab transmission spectra. Additionally, synthetic spectra generated from the n / k values derived using two different methods (KBr pellet transmission and single-angle reflectance) are compared using the Mie theory model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Coupled Experimental and Simulation Approach to Investigate the Impact of Grain Growth, Amorphization, and Grain Subdivision in Accident Tolerant U 3 Si 2 Light Water Reactor Fuel

Triuranium disilicide (U 3 Si 2 ) is being considered as an alternative accident tolerant fuel (ATF) due to its higher thermal conductivity. However, there is uncertainty in its use due to a lack of irradiation data at light water reactor (LWR) conditions. In this project, we used an integrated experimental and simulation approach to answer two significant questions pertaining to U 3 Si 2 that were not investigated by the Fuel Cycle Research and Development (FCRD) and Nuclear Energy Advanced Modeling and Simulation (NEAMS) programs: (1) Will grain growth in the hotter portions of the fuel significantly impact U 3 Si 2 LWR fuel behavior? (2) Under what conditions do grain subdivision and amorphization occur in U 3 Si 2 and will either occur at LWR conditions? Our approach to answer these questions used in situ ion irradiation and annealing to investigate grain growth, grain subdivision, and amorphization, along with mesoscale simulations using the MARMOT tool. We found that while the grain boundary mobility of U 3 Si 2 is larger than that of UO 2 , grain growth in U 3 Si 2 fuel pellets will be less than in UO 2 and may be neglected due to the lower thermal conductivity and thus lower centerline temperature. We also found that amorphization will not occur in U 3 Si 2 above 600 K, such that it is not likely to occur at typical LWR operating conditions. Grain subdivision will occur at LWR conditions and will likely occur at lower burnups than in UO 2 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Separate Effects Validation for Subcooled Boiling in CTF

In 2010, the U.S. Department of Energy created its first Energy Innovation Hub, which is focused on developing high-fidelity and high-resolution modeling and simulation (M&S) tools for modeling of light water reactors (LWRs). This hub, the Consortium for Advanced Simulation of LWRs (CASL), has developed an LWR simulation tool called the Virtual Environment for Reactor Applications (VERA). The multi-physics capability of VERA is achieved through the coupling of single-physics codes, including CTF (the CASL version of Coolant Boiling in Rod Arrays— Three Field (COBRA-TF)), Michigan Parallel Characteristics Transport (MPACT), BISON, and Materials Performance and Optimization (MPO) Advanced Model for Boron Analysis (MAMBA). As part of its M&S efforts, CASL has identified various challenge problems, including Crud Induced Power Shift (CIPS), Crud-Induced Localized Corrosion (CILC), Pellet-Cladding Interaction (PCI), and Departure from Nucleate Boiling (DNB). This work addresses CASL milestone L2:VVI.P19.03, which focuses on uncertainty quantification of crud, which is relevant to both CIPS and CILC. This is achieved through an analysis and separate effects validation of the thermal hydraulic phenomenon known as subcooled boiling. As part of this work, various sources of experimental data are examined and compared to different options for empirical modeling of subcooled boiling. Through this analysis, a complete understanding of the underlying models and their implementation details are understood. A subset of these data are incorporated into a separate effects validation study of CTF. The Westinghouse Advanced Loop Tester (WALT) and Rohsenow experiments are modeled, and it is shown that the newly-implemented Gorenflo correlation is more accurate than the existing Chen and Thom correlations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Irradiation enhanced diffusion and diffusional creep in U₃Si₂

U₃Si₂ is a candidate as an advanced fuel for light water reactors (LWRs). Compared to UO₂, there are significant data gaps for the thermophysical and thermomechanical properties of U₃Si₂. Atomic scale simulations can help fill in those gaps, while also providing a more mechanistic understanding of the material properties. Creep is an important property for fuel performance as it influences the pellet-cladding gap, which in turn affects the temperature of the fuel (a key parameter in many other aspects of fuel behavior). In this work, we employed a DFT-informed cluster dynamics framework to predict point defect concentrations in U₃Si₂. The concentrations, diffusivities, and volumes of these defects were used to develop a diffusional creep model based on bulk (Nabarro-Herring) and grain boundary (Coble) diffusion processes. It was found that irradiation enhanced Nabarro-Herring creep is dominant at low temperatures, while Coble creep dominates for high temperatures. The model compares well against available experimental data and has been implemented in BISON. A demonstration case using simple power profiles has been carried out, showing that negligible creep occurs due to the low temperatures experienced by U₃Si₂, a consequence of its high thermal conductivity.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Non-destructive Examinations of ATF-2 Baseline Rodlets

This report contains the results of non-destructive examinations of Accident Tolerant Fuels 2 (ATF-2) rodlets irradiated in the Advanced Test Reactor (ATR) Loop 2A. The experiment is part of the U.S. Department of Energy Nuclear Technology Research and Development (NTRD) program’s Advanced Fuels Campaign (AFC). The rodlets were composed of UO2 pellets and Zr-4 cladding. The data have been collected to provide baseline PIE data to support future testing in TREAT and to have performance data against which the data of the ATF concepts can be compared directly. The analyses performed included: visual examinations, axial gamma scanning, neutron radiography and profilometry. All the data collected showed a performance consistent with expectations for this fuel system at low burnup.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Stability of zirconium hydride

This reports complete Milestone M2.2.1 Stability of zirconium hydride: Experimental investigation of the hydrogen concentration of encapsulated zirconium hydride before and after joining. In this milestone, we first report the successful fabrication of crack-free bulk zirconium hydride by using the ORNL static hydriding system. The fabricated hydride was characterized by using X-ray diffraction (XRD) and X-ray computed tomography (XCT). XRD results showed that the δ-phase zirconium hydride, α-zirconium, and ε-phase hydride were present. XCT confirmed the absence of the internal cracking. The hydrogen concentration was determined by the weight change before and after hydrogen loading, given the fact that the oxide phase was not found during XRD analysis. Two metallic cladding materials, i.e., molybdenum and FeCrAl, were selected to encapsulate the fabricated zirconium hydride pellets. Demonstration capsules were designed and machined. Mo crucible was successfully sealed by using a combination of electron beam welding and gas tungsten arc welding. Due to the undesired neutronics property of Mo, further investigation of this cladding material was not pursued. Electron beam welding and laser beam welding were employed to seal the FeCrAl capsules. XRD were performed on the zirconium hydride before and after the sealing. The results showed that the welding process has negligible impact on the hydrogen content in the FeCrAl-canned zirconium hydride. The presented work fulfilled the proposed work under this milestone and paves a pathway to fabricate single-phase zirconium hydride and to develop robust cladding materials to can bulk zirconium hydride.

36 MATERIALS SCIENCE↗

Status Report on Development of a Cask to Enable Pulsed Neutron Characterization of Irradiated Fuel

We present the design of a shielding cask that allows pulsed neutron characterization of irradiated fuel rodlets prior to their destructive examination in hot cells. The goal is to provide complementary and informative measurements that will inform subsequent hot cell PIE examinations by identifying typical and atypical regions with respect to microstructure, tomographic data, or isotope densities. Time-of-flight neutron diffraction has the potential to offer efficient, non-destructive and non-contact microstructural characterization of irradiated fuel pins with spatial resolution of 1 mm3 to 1 cm3 while for energy-resolved neutron imaging (and by extension tomography) a resolution of 100 μm was demonstrated. The potential results include crystallinity vs. amorphous volumes and microstructural information such as phase compositions and textures from the diffraction data as well as distances (e.g. pellet to cladding), cracks, and isotopic distributions of minor actinides, fission products as well as fission gas partial pressures e.g. in the plenum from energy resolved neutron imaging. The capability will identify regions of atypical behavior and provide cost effective bulk characterization of entire samples prior to destructive evaluation in hot cells. This effort is a collaboration between LANL, INL, ORNL, and UC Berkeley. A key facet of the initiative is the ability to cost effectively ship irradiated fuels from INL to the pulsed spallation neutron source at LANSCE. The irradiated fuel would be loaded in the custom designed cask (designated RaMHaM) at INL hot cells which then could be shipped in a BRR Type B shipment container between INL and LANL. No hot cell is required after the loading of the sample at INL in the pathway laid out in this report, greatly simplifying handling at LANL.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Center of Excellence Collaboration Projects: Second Wave

The NEAMS program aims to develop an integrated multi-physics simulation capability “pellet-to-plant” for the design and analysis of future generations of nuclear power plants. In particular, the Reactor Product Line code suite's multi-resolution hierarchy is being designed to ultimately span the full range of length and time scales present in relevant reactor design and safety analyses, as well as scale from desktop to petaflop computing platforms. In particular the NEAMS program is supporting the development of novel thermal-hydraulic codes. The Center of Excellence for Thermal Fluids Application in Nuclear Energy, launched in 2018, has as its key goals to serve as a front door to industry. The Center of Excellence for Thermal Fluids Applications in Nuclear Energy has recently launched a program to start collaborative efforts between the laboratories and industry with the objective of stimulating cooperation and increasing adoption of T/H tools developed under NEAMS by the industry-at-large. In particular, two industry partners agreed to participate in a second wave of short-term collaborations aimed at demonstrating the value of NEAMS tools to their designs. These are Framatome and TerraPower who proposed projects related to LWR (Light Water Reactor) and MSFR (Molten Salt Fast Reactor) designs respectively. In this report we present the results of these two collaborations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

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↗

Semi-Empirical Material Model for Hydrogen Uptake Kinetics by 1,4-bis(phenylethynyl)benzene (DEB)-based Getters

We report on development of a semi-empirical model describing the kinetics of H 2 /D 2 reaction with 1,4-bis(phenylethynyl)benzene (DEB)-based getters in pellet and powder form. The physical basis of the model is solid-state diffusion of DEB plus reaction of DEB with H atoms on the surface of nanometer-scale Pd catalyst particles. The purpose of this material model is to facilitate more accurate predictions of performance for DEB-based getter assemblies. These predictions will be accomplished by integrating the model presented here into finite element, reaction/diffusion simulations of getter assembly hydrogen uptake performance. As of Fall 2020, this integration is underway.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Assessment of Existing Transportation Packages for Use with HALEU

Commercial light water reactor operators and fuel vendors in the United States are pursuing changes to fuel that include increased 235 U enrichment. Economic studies generally anticipate maximum near-term fuel assembly designs with up to 8 wt.% 235 U. Many next-generation nuclear reactor designs require high-assay low-enriched uranium (HALEU) (19.75 wt.% > 235 U > 5 wt.%) fuel. One necessary element for the commercial-scale use of HALEU is the ability to safely transport large quantities of enriched fuel material in multiple forms. However, there is uncertainty as to whether subcriticality requirements can be satisfied with existing package designs and whether existing critical benchmark experiment data are sufficient to support criticality safety code validation for HALEU transportation applications. This study assesses the potential to use currently licensed transportation packages for the transportation of increased enrichment unirradiated U fuel forms. The assessment uses selected package designs that represent the five categories of fuel form-boiling water reactor pins and assemblies, pressurized water reactor pins and assemblies, UF 6 , U-metal and tristructural isotropic (TRISO) particles, and UO 2 pellets or powder-and focuses on demonstrating subcriticality and identifying benchmark critical experiments appropriate for use in criticality computer code validation. Key quantities of interest that relate to subcriticality are limiting conditions (e.g., optimum moderation), package or package array k eff , package capacity, and package transportation array size. The SCALE TSUNAMI-3D and TSUNAMI Indices and Parameters codes are used for sensitivity and uncertainty calculations and for identification of candidate critical benchmark experiments for code validation. The primary metric for identifying candidate benchmarks is the similarity coefficient, c k . For each fuel form category, a representative package is evaluated. Results provided for each package evaluation include enrichment and packaging limits (e.g., maximum transportation array size as a function of enrichment) and benchmark critical experiment similarity coefficients. Results indicate that there are viable means for increasing enrichments into the HALEU range across the spectrum of fuel forms with differing increase amounts available for different packages. Sources of subcriticality margin to offset increased enrichment reactivity include reduced transportation array size, reduced fissile mass, burnable absorber credit, and safety analysis margin harvesting. For all packages except the DN-30, numerous critical benchmark experiment candidates for validation were identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Control of the Plasma-Material Interface for Long Pulse Optimization in EAST Final Report

This final report describes the funded activity to understand and control the plasma-material interface to improve long pulse discharge control and performance on the EAST (Experimental Advanced Superconducting Tokamak) facility, located in Hefei, China. The primary focus of the research was long pulse recycling control via optimization of lithium (Li) delivery systems, including flowing liquid lithium plasma facing components (PFCs), because Li persists as the main wall conditioning technique. On EAST, lithium was primarily introduced using crucible evaporation, pellet injection, and gravitationally dropped powder. Overall, the introduction of lithium into the EAST plasma had strong and persistent effects on the ELM behavior during long pulse EAST discharges demonstrating overall improved performance. Additionally, a flexible impurity injection tool, a multi-chamber impurity powder dropper, was developed and deployed on EAST, to extend powder injection to elements other than Li. Finally, improvements to the Soft X-ray diagnostic system were introduced to improve measurements of impurity transport and electron temperature.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Doping effect of Al in LLZO

Lithium ion batteries have become a common use in most electronic devices and transportation. However, the use of liquid electrolytes poses a serious safe hazard due to their high flammability. The narrow operating temperature and voltage windows also limit further improvement of the energy density.Solid-state lithium batteries with the use of more stable and safer solid electrolyte have garnered much attention and could be the future choice for battery technology. A promising potential candidate for the solid electrolyte component is the garnet type Li 7 La 3 Zr 2 O 12 (LLZO) ceramic material since it possesses high ionic conductivity at room temperature and enables the use of high capacity lithium anode and high voltage/capacity cathodes.However, to form the stable cubic phase of LLZO and high densification,high sintering temperatures above 1100°C is typically required, which causes Lithium loss of the system.Many studieshave been taken to dop LLZO with various precursors such as Ga, Ta, and Al to stabilize the cubic structure and reduce calcination temperature, while the doping effect on sintering densification is still unclear. In this study Al doping along with ball milling were explored to stabilize the cubic phase of LLZO and improve densification, while reducing the amount of impurity phases. Samples were synthesized from the precursors Li 2 CO 3 , Al 2 O 3 , La 2 O 3 , and ZrO 2 by ball milling followed by heat treatment for 12 hours at 1000°C. XRD with Rietveld fitting was used to determine the two phases of LLZO (cubic, tetragonal) and other possible secondary phases. Furthermore,SEM with top and cross sectional views was conducted to investigate the morphology and microstructure of sintered pellets.

36 MATERIALS SCIENCE↗

Investigating bubble pressures in irradiated UO 2 for understanding fragmentation of high burnup structure

This report summarized work carried out to investigate mechanisms relevant to fragmentation of high burnup UO 2 fuel. High pressure bubbles that form in high burnup structure are thought to be responsible for fragmentation and pulverization, when exposed to a temperature ramp during a transient. The over-pressurization of the bubbles during normal operation is a pre-requisite for this mechanism to occur. Therefore, in this work we investigate the role of interstitials, produced through irradiation, in over-pressurizing the bubbles by using a combined molecular dynamics (MD) and cluster dynamics approach. Firstly, the energies for the annihilation of interstitials and vacancies at bubbles have been determined from MD as a function of bubble pressure. Secondly, these reaction energies have been implemented in the cluster dynamics code Centipede to determine the steady-state defect concentrations and bubble pressure under irradiation. It was found that there is a transition from low pressure bubbles, at high temperature, to high pressure bubbles, at low temperatures. This indicates the formation of over-pressurized bubbles in the low temperature periphery of the pellet, where high burnup structure forms. This result supports the hypothesis that over-pressurized bubbles form during steady-state operation and can then contribute to fragmentation during a transient. Future work will examine the influence of bubble pressure on Xe diffusion and study the impact of other sinks (e.g. grain boundaries and dislocations) that are relevant to high burnup structure. Ultimately, the goal is to provide predictions of the bubble pressure as a function of burnup that can be used to derive a more mechanistic fragmentation threshold for use in BISON.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Experimental investigation on the binary/ternary fluidization behavior of Geldart D type spherical LDPE, Geldart D type cylindrical wood and Geldart B type sand particles

The series of experiments have been performed on a 2.5-inch cylindrical bed made of acrylic with full optical access and multiple pressure ports at various heights of the bed. The material of interest includes in the investigation include Geldart type D cylindrical hardwood pellets, Geldart type D spherical LDPE, and Geldart type B sand particles. The wood particles have a diameter of around 6.6 mm and a length of 13.2 mm, corresponding to an aspect ratio of 1:2. The spherical LDPE particles and the sand particles have a Sauter Mean Diameter of 3.75 mm, and 0.5 mm, respectively. The experiment series involved the fluidization of the above-mentioned single particle type, as well as the fluidization of binary and ternary mixtures with varying superficial velocities.

20 FOSSIL-FUELED POWER PLANTS↗

Radiation Transport Simulation of the Sulfur Counting System in the Radiation Metrology Laboratory (RML)

At the request of staff members from the Radiation Metrology Laboratory (RML), a series of Monte Carlo radiation transport calculations were performed using two different models of the detector geometry of the RMLs sulfur counting system. The fraction of electrons from each β-decay of 32 P in the sulfur pellet that enter the window of the sulfur counting system was calculated with both MCNP and ITS. In addition, the differential energy distributions of the electrons entering the counting system window were computed. There was significant agreement between the integral and differential quantities calculated by the two transport codes. Summary tables are for the integral efficiency values are found in the body of the report.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Analysis of the 30B UF 6 Container for Use with Increased Enrichment

Commercial light-water reactor (LWR) operators and fuel vendors are pursuing advancements in fuel and reactor design that include increasing 235 U enrichment from low enrichment (<5 wt.% 235 U) to low-enriched uranium+ (LEU+) (10 wt.% > 235 U > 5 wt.%) and high-assay low-enriched uranium (HALEU) (20 wt.% > 235 U > 10 wt.%). These advancements will necessitate the ability to transport LEU+ and HALEU fuel materials. Assessment of Existing Transportation Packages for Use with HALEU(ORNL/TM-2020/1725) assesses the potential to use currently licensed transportation packages for the transportation of HALEU by evaluating a representative package for each uranium fuel form category (for example, oxide and/or metal in fuel assemblies, fuel pins, powder, pellets, and uranium hexafluoride [UF 6 ].) This report expands on the UF 6 analysis.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fundamental Studies of Tritium Diffusivity in Pure and Defective Zircaloy-4 Getters (Tritium Science Program FY2020 Report)

Zirconium (Zr) alloys are extensively used as tritium (T) getters in nuclear reactors due to their low absorption cross section to thermal neutron, good mechanical properties at high temperature and resistant to corrosion in different environmental conditions. Zr alloys have better thermal properties than many other refractory alloys including stainless steel. The nuclear characteristic is simulated, and T is produced in tritium-producing burnable absorber rods (TPBAR) by the irradiation of neutron flux in pressurized water reactor (PWR). T thus produced diffuses through the pellets and is captured by the getter where it chemically reacts with Zr to form metal hydride (ZrTx). These hydrides are brittle and affect adversely the mechanical properties of alloys. In addition to that, mismatch in the lattice structures after hydride formation creates a stress which needs to be considered in component design and their life evaluation. Therefore, understanding the behavior of T and its species becomes significant as fuel burnup is increased, which leads to increase in hydrogen pickup and oxide formation. The transport of T and its species in pure Zr alloys, and in alloys with certain alloying elements and defects are important to understand in order to enhance the performance of the materials.

36 MATERIALS SCIENCE↗