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At least 163 records · Page 9

High Energy X-ray Applications for the Characterization of Metallic Uranium Alloys

Uranium-based metallic alloys are both candidates for fuels in high performance research and test reactors, as well as in fast spectrum reactors as nuclear transmutation fuels that can be utilized to burn long-lived minor actinides and fission products. Uranium-molybdenum (UMo) alloys are under development for the use in research and test reactors. Whereas, uranium-zirconium (U-Zr) alloys represent one of the types of fuels that are under consideration for use within the fast spectrum reactors. Both of these types of metallic fuels have been studied for over five decades in various types of reactors. Many of the previous studies had focused on performance-based aspects. However, recent advances in characterization tools and techniques, as well as short-term (low fluence) neutron irradiation facilities have contributed to a more in-depth understanding of nuclear fuel and material behavior following irradiation. This knowledge is crucial to the enhancement of current modeling and simulation techniques, particularly with respect to parameterization and validation. This paper focuses on the use of high energy x-rays to characterize metallic nuclear fuel. The specimens were composed of depleted uranium (DU) alloyed with either Zr or Mo, where DU-xZr (x = 10, 15, or 20 wt.%) and DU-yMo (y = 7 or 10 wt.%). The geometries of the specimens were 3 mm TEM disks that were ∼200 μm in thickness. The fuel alloys were initially prepared via an arc melting process. The samples were irradiated at the Advanced Test Reactor at Idaho National Laboratory (INL) using the hydraulic rabbit system. The hydraulic rabbit system allows for well-controlled, short term irradiations (less than one cycle), hence resulting in low fluences. The U-based alloys were irradiated to doses of 0.01 and 0.1 dpa. The irradiation temperature of the specimens ranged from 150 deg. C to 800 deg. C. Synchrotron characterization techniques can be used to provide insight into material microstructure ranging a multitude of spatial scales, from the atomic scale to the macroscale. High-energy x-rays at the National Synchrotron Light Source II (NSLS II) and the Advanced Photon Source (APS) have been utilized to understand the microstructural changes in these metallic alloys, specifically with respect to phase identification, phase fractions, chemical bonding, strain, and dislocation density through the use of diffraction and X-ray Absorption Spectroscopy (XAS). These experiments utilized a robot for specimen exchange during the diffraction measurements, allowing for remote handling of radioactive materials. This is an example of another recent advancement in characterization techniques that enables research with nuclear materials. Detailed results of the analyses of the microstructural changes are pending.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Transmission electron microscopy characterization of the fuel-cladding chemical interactions in HT9 cladded U-10Zr fuel

Fuel cladding chemical interaction (FCCI) is a key phenomenon needs to be better understood to establish the design basis for U-10Zr metallic fuel performance. Characterizing the microstructure and chemical composition of FCCI at micron and sub-micron scale is critically important toward a more mechanistic understanding of FCCI phenomenon and its potential effects on cladding integrity and metallic fuel performance. This paper, by using transmission electron microscopy, investigated the FCCI region in HT9 cladded U-10Zr fuel irradiated to 5.7% FIMA burnup at a peak inner cladding temperature of 615 °C in Fast Flux Test Facility (FFTF). Four distinct layers are identified in the FCCI region. The migration of Fe into the fuel side leads to the formation of several U-Zr-Fe ternary phases, including ?-Fe0.5Zr0.32U0.18, e-Fe0.3Zr0.4U0.3, and ?-Fe0.06Zr0.23U0.71, mingled with UFe2, U6Fe, and U phase at various Fe penetration depth up to ~ 150 µm. On the cladding side, grain coarsening and significant lanthanides infiltration along grain boundaries are observed. Laves phase, (Fe,Cr)2(Mo,W), which typically does not exist in fresh HT9, is identified in a wide radial range in the cladding. The typical HT9 martensitic lath structure and pre-existing M23C6 precipitates disappear, partially or completely, depending on the radial distance from the fuel-cladding interface. Those microstructural and compositional changes could cause mechanical degradation in the HT9 cladding. The present characterization results will improve the understanding of FCCI phenomenon and facilitate the development of microstructure-informed FCCI modeling for metallic fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Isolation of the Copper Redox Steps in the Standard Selective Catalytic Reduction on Cu-SSZ-13

Operando X-ray absorption experiments and density functional theory (DFT) calculations are reported that elucidate the role of copper redox chemistry in the selective catalytic reduction (SCR) of NO over Cu-exchanged SSZ-13. Catalysts prepared to contain only isolated, exchanged CuII ions evidence both CuII and CuI ions under standard SCR conditions at 473 K. Reactant cutoff experiments show that NO and NH3 together are necessary for CuII reduction to CuI. DFT calculations show that NO-assisted NH3 dissociation is both energetically favorable and accounts for the observed CuII reduction. The calculations predict in situ generation of Brønsted sites proximal to CuI upon reduction, which we quantify in separate titration experiments. Both NO and O2 are necessary for oxidation of CuI to CuII, which DFT suggests to occur by a NO2 intermediate. Reaction of Cu-bound NO2 with proximal NH4 + completes the catalytic cycle. N2 is produced in both reduction and oxidation half-cycles.

Environmental Molecular Sciences Laboratory↗

Shielding Analysis Capability of UNF-ST&DARDS

The Used Nuclear Fuel Storage, Transportation and Disposal Analysis Resource and Data System (UNF-ST&DARDS) is used to perform dose rate calculations for spent nuclear fuel (SNF) transportation packages based on the actual physical and nuclear characteristics (i.e., assembly design, burnup, initial enrichment, and cooling time) of the as-loaded SNF. Nuclear fuel data, transportation package model templates, and SNF canister loading map information residing within the tool facilitate automated generation of SCALE input files for radiation source term and dose rate calculations. Transportation package specific models developed for UNF-ST&DARDS dose rate analyses are described in detail. UNF-ST&DARDS dose rate analyses were performed in this paper for over 400 SNF canisters from 16 sites in their designated transportation casks. For simplicity, representative dose rate calculation results are presented as a function of time (i.e., selected calendar years between 2020 and 2100) for 73 SNF canisters in dry storage at four sites. For these canisters, the projected maximum dose rate values at 2 m from the lateral surfaces of the vehicle under normal conditions of transport (NCT) would vary between 1.9 and 11.5 mrem/h in 2020. Five SNF canisters will exceed the regulatory dose rate limit of 10 mrem/h at 2 m in 2020, and the analyzed SNF canisters will comply with regulatory dose rate limits by 2030. An analysis of the impact on the dose rate of fuel failure and reconfiguration during transportation indicated that the maximum dose rate for hypothetical accident conditions will be unaffected, and the NCT maximum dose rate at 2 m would have a maximum increase by a factor of 1.7 for a representative pressurized water reactor package and by a factor of 2.6 for a representative boiling water reactor package relative to intact fuel. Finally, analysis of the actual heat loading and the dose rate at 2 m from the lateral surface of the vehicle for the five SNF canisters exceeding the NCT regulatory dose rate limit of 10 mrem/h in 2020 showed that the dose rate could be more limiting with respect to regulatory requirements than the heat loading; i.e., the canister transportability date may be evaluated based on the transportation package’s external dose rate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Containment Analysis Capability of UNF-ST&DARDS

The Used Nuclear Fuel-Storage, Transportation & Disposal Analysis Resource and Data System (UNF-ST&DARDS) methodology to perform automated containment analyses for potential transportation packages based on canister loading map information is described in this paper, and its capability is illustrated with example results. The allowable leakage rate is calculated with the procedures provided in ANSI N14.5-2014 and NUREG/CR-6487, which were adapted for containment analysis of a transportation package containing fuel assemblies with different nuclear characteristics (e.g., initial enrichment, burnup, and cooling time) and clad integrity (intact or damaged). UNF-ST&DARDS applies different source term calculation methodologies for low-burnup fuel (LBF) (i.e., <45 GWd/tonne U) assemblies and high-burnup fuel (HBF) (i.e., ≥45 GWd/tonne U) assemblies. The LBF radionuclide activities are based on actual fuel assembly burnup, initial enrichment, and cooling time. Bounding radionuclide activities based on a fuel pellet burnup value of 65 GWd/tonne U and actual fuel assembly cooling time are used for HBF assemblies. The fraction of failed fuel rods and the release fractions for the contributors to releasable source terms recommended in NUREG-1617 are used in the containment analysis regardless of fuel assembly burnup. However, UNF-ST&DARDS supports different parameter values for LBF and HBF assemblies. Finally, the containment analysis methodology for as-loaded transportation packages is presented in detail, and the UNF-ST&DARDS containment analysis capability is illustrated with results for simulated transportation packages containing spent nuclear fuel canisters in dry storage at selected sites.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermo-hydrological and chemical (THC) modeling to support Field Test Design

This report summarizes ongoing efforts to simulate coupled thermal-hydrological-chemical (THC) processes occurring within a hypothetical high-level waste (HLW) repository in bedded salt. The report includes work completed since the last project deliverable, “Coupled model for heat and water transport in a high level waste repository in salt”, a Level 2 milestone submitted to DOE in September 2013 (Stauffer et al., 2013). Since the last deliverable, there have been code updates to improve the integration of the salt module with the pre-existing code and development of quality assurance (QA) tests of constitutive functions and precipitation/dissolution reactions. Simulations of bench-scale experiments, both historical and currently in the planning stages have been performed. Additional simulations have also been performed on the drift-scale model that incorporate new processes, such as an evaporation function to estimate water vapor removal from the crushed salt backfill and isotopic fractionation of water isotopes. Finally, a draft of a journal paper on the importance of clay dehydration on water availability is included as Appendix I.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Dynamics, thermodynamics, radiation, and cloudiness associated with cumulus-topped marine boundary layers

The overall goal of this project was to improve the understanding of marine boundary clouds by using data collected at the Atmospheric Radiation Measurement (ARM) sites, so that they can be better represented in global climate models (GCMs). Marine boundary clouds are observed regularly over the tropical and subtropical oceans. They are an important element of the Earth’s climate system because they have substantial impact on the radiation budget together with the boundary layer moisture, and energy transports. These clouds also have an impact on large-scale precipitation features like the Inter Tropical Convergence Zone (ITCZ). Because these clouds occur at temporal and spatial scales much smaller than those relevant to GCMs, their effects and the associated processes need to be parameterized in GCM simulations aimed at predicting future climate and energy needs. Specifically, this project’s objectives were to (1) characterize the surface turbulent fluxes, boundary layer thermodynamics, radiation field, and cloudiness associated with cumulus-topped marine boundary layers; (2) explore the similarities and differences in cloudiness and boundary layer conditions observed in the tropical and trade-wind regions; and (3) understand similarities and differences by using a simple bulk boundary layer model. In addition to working toward achieving the project’s three objectives, we also worked on understanding the role played by different forcing mechanisms in maintaining turbulence within cloud-topped boundary layers We focused our research on stratocumulus clouds during the first phase of the project, and cumulus clouds during the rest of the project. Below is a brief description of manuscripts published in peer-reviewed journals that describe results from our analyses.

54 ENVIRONMENTAL SCIENCES↗

Base Monolithic Fuel: Research, Development, and Qualification Plan

The Office of Global Threat Reduction Initiative within the U.S. DOE/National Nuclear Security Administration is working to convert research reactors globally from highly enriched uranium fuel to low-enriched uranium (LEU) fuel. Of the 200 candidate research reactors, over 80 reactors have been converted using LEU fuel developed in the 1980s. Additional reactor conversions using this fuel are currently underway. However, there is a small set of high performance research reactors which require a new high density LEU fuel for conversion, including six U.S. high performance research reactors (USHPRRs). This research, development, and qualification plan provides the general approach for the USHPRR team to move the selected base monolithic LEU through to licensing and use in the intended reactors. The plan includes the latest information on the perceived requirements for licensing and use of the fuel. It also includes the methods by which data will be collected to show that these requirements have been met.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Integral Experiment Request 209 (CED-2 Summary Report)

This report examines proposed Seven Percent Critical Experiment (7uPCX) experiments with fuel arrays larger than would be critical when fully reflected. In these experiments, the reactivity of the assembly will be controlled by varying the moderator/reflector level in the core tank. The analysis uses two configurations, each completely filling the 45x45 fuel rod array with fuel rods and water holes, as representative examples of the proposed experiments. The proposed configurations are compared to the experiments documented in LEU-COMP-THERM-078 [Reference 1] and to fully-reflected experiments with the same fully-loaded fuel arrays that are poisoned with boron in the moderator. The conclusion is drawn that the proposed experiments can be performed with acceptably low uncertainties given a calibrated moderator/reflector level measurement system.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Design of UO 2 -BeO Critical Experiment at Sandia [Poster]

The purpose of this proposal is to design a new integral critical experiment to investigate the effects of beryllium oxide and high assay low-enriched uranium fuels. this proposal considers using several existing resources at Sandia: (1) the Critical Experiments (SCX) facility and water tank, (2) spare UO 2 -BeO fuel for the Annular Core Research Reactor (ACRR), and 7uPCX fuel rods from previous benchmark experiments.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Degradation mechanisms in thermal-barrier coatings

The degradation mechanism in a thermal barrier-coating system subjected to prolonged heating in air as well as to thermal cycling was studied. Bond-coat oxidation was found to be the most important reason for degradation. The oxidation produced NiO as well as Al2O3 in one set of samples, but the variation in initial coating structure made it difficult to resolve systematic differences between isothermally heated and thermally cycled samples. However, the contribution to degradation from changes in substrate composition seemed less in the cycled sample.

Shinde, S. L.↗

Modeling Feedbacks Between Water and Vegetation in the Climate System

Not only is water essential for life on earth, but life itself affects the global hydrologic cycle and consequently the climate of the planet. Whether the global feedbacks between life and the hydrologic cycle tend to stabilize the climate system about some equilibrium level is difficult to assess. We use a global climate model to examine how the presence of vegetation can affect the hydrologic cycle in a particular region. A control for the present climate is compared with a model experiment in which the Sahara Desert is replaced by vegetation in the form of trees and shrubs common to the Sahel region. A second model experiment is designed to identify the separate roles of two different effects of vegetation, namely the modified albedo and the presence of roots that can extract moisture from deeper soil layers. The results show that the presence of vegetation leads to increases in precipitation and soil moisture in western Sahara. In eastern Sahara, the changes are less clear. The increase in soil moisture is greater when the desert albedo is replaced by the vegetation albedo than when both the vegetation albedo and roots are added. The effect of roots is to withdraw water from deeper layers during the dry season. One implication of this study is that the insertion of vegetation into the Sahara modifies the hydrologic cycle so that the vegetation is more likely to persist than initially.

Miller, James R.↗

Advanced Oxide Material Systems for 1650 C Thermal/Environmental Barrier Coating Applications

Advanced thermal and environmental barrier coatings (TEBCs) are being developed for low-emission SiC/SiC ceramic matrix composite (CMC) combustor and vane applications to extend the CMC liner and vane temperature capability to 1650 C (3000 F) in oxidizing and water-vapor-containing combustion environments. The advanced 1650 C TEBC system is required to have a better high-temperature stability, lower thermal conductivity, and more resistance to sintering and thermal stress than current coating systems under engine high-heat-flux and severe thermal cycling conditions. In this report, the thermal conductivity and water vapor stability of selected candidate hafnia-, pyrochlore- and magnetoplumbite-based TEBC materials are evaluated. The effects of dopants on the materials properties are also discussed. The test results have been used to downselect the TEBC materials and help demonstrate the feasibility of advanced 1650 C coatings with long-term thermal cycling durability.

Zhu, Dong-Ming↗

Geostationary Carbon Process Mapper (GCPM)

Geostationary Carbon Process Mapper (GCPM) is an earth science mission to measure key atmospheric trace gases related to climate change and human activity.Understanding of sources and sinks of CO2 is currently limited by frequency of observations and uncertainty in vertical transport. GCPM improves this situation by making simultaneous high resolution measurements of CO2, CH4, CF, and CO in near-IR, many times per day. GCPM is able to investigate processes with time scales of minutes to hours. CO2, CH4, CF, Co selected because their combination provides information needed to disentangle natural and anthropogenic sources/sinks. Quasi-continuous monitoring effectively eliminates atmospheric transport uncertainties from source/sink inversion modeling. will have one instrument (GeoFTS), hosted on a commercial communications satellite, planned for two years operation. GCPM will affordably advance the understanding of observed cycle variability improving future climate projections.

Carbon Process↗

Thermal Cycling of Stationary Superconducting Rotor Coils for the High Efficiency Megawatt Motor

The self-cooled, superconducting rotor included in the design of the High Efficiency Megawatt Motor (HEMM) can produce magnetic field strengths far higher than those produced using conventional approaches. However, the superconductivity properties of high-temperature superconducting coils can degrade as the coil is repeatedly thermally cycled, significantly impacting the HEMM’s performance. To explore ways to reduce this risk, NASA researchers fabricated and tested several coils of increasing complexity. The results of the testing campaign indicate that NASA can fabricate and test full-scale superconducting coils for the rotor of the HEMM that can reliably survive repeated thermal cycling with no or acceptably slow degradation.

Electrified Aircraft Propulsion↗