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DOE OSTI2018

On visualizing material flow and precipitate evolution during probeless friction stir spot welding of an Al-Li alloy

Highlights: • Severe thermal cycle and deformation refined grains and intermetallic particles in SZ. • T{sub 1} phases fully dissolved in SZ followed by re-precipitation of GP zone and δ′ phases. • The predominant flow direction remained in spiral-like pattern during P-FSSW. • Local abrasion existed in the lap-weld interface due to flow difference, forming joining. - Abstract: The precipitate evolution and material flow visualization during probeless friction stir spot welding (P-FSSW) of an Al-Li alloy has been investigated experimentally and numerically in this work. Due to severe heat input during welding, the main strengthening phases of T{sub 1} fully dissolved in the stir zone followed by the re-precipitation of GP zone and δ′ phases, assisted with the refinement of the intermetallic particles and grains. The history of material flow was three-dimensionally visualized with a tracer, studied with X-ray tomography. The experiments and the simulation results provided a consistent interpretation of a circumferential material flow which moved inwards radially near the top surface. Upward flow in the bottom sheet improved with dwell time, causing the interface to bend. Local abrasion between the two sheets due to flow difference led to the disruption of oxide layer, and formed a connection at the interface.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Development of molecular dynamics potential for uranium silicide fuels

The use of uranium-silicide (U-Si) in place of uranium dioxide (UO{sub 2}) is one of the promising concepts being proposed to increase the accident tolerance of nuclear fuels for light water reactors. First-principles based density functional theory (DFT) electronic structure calculations may provide the most reliable information. However, it is probably not possible to obtain kinetic information such as amorphization under irradiation directly from DFT simulations due to size and time limitations. Thus, a more feasible way may be to employ molecular dynamics (MD) simulation. Unfortunately, so far no MD potential is available for U-Si to discover the underlying mechanisms. Here, we present our recent progress in developing a U-Si potential. The development is based on the Tersoff type potentials for single element U and Si. The Si potential is taken from the literature and a Tersoff type U potential is developed in this project. With the primary focus on the U{sub 3}Si{sub 2} phase, some other U-Si systems such as U{sub 3}Si are also included as a test of the transferability of the potentials for binary U-Si phases. Based on the potentials for unary U and Si, two sets of parameters for the binary U-Si system are developed using the Tersoff mixing rules and the cross-term fitting, respectively. The cross-term potential is found to give better results on the enthalpy of formation, lattice constants and elastic constants than those produced by the Tersoff mixing potential, with the reference data taken from either experiments or DFT calculations. In particular, the results on the formation enthalpy and lattice constants for the U{sub 3}Si{sub 2} phase and lattice constants for the high temperature U{sub 3}Si (h-U{sub 3}Si) phase generated by the cross-term potential agree well with experimental data. Reasonable agreements are also reached on the elastic constants of U{sub 3}Si{sub 2}, on the formation enthalpy for the low temperature U{sub 3}Si (m-U{sub 3}Si) and h-U{sub 3}Si phases, and on the lattice constants of m-U{sub 3}Si phase. All these phases are predicted to be mechanically stable. The unary U potential is also tested for three metallic U phases (α, β, γ). The potential is found capable to predict the cohesive energies well against experimental data for all three phases. It matches reasonably with previous experiments on the lattice constants and elastic constants of αU. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Enthalpies of formation and phase stability relations of USi, U 3 Si 5 and U 3 Si 2

U–Si intermetallic compounds have drawn great attention due to their potential application as nuclear fuels. However, the thermodynamic properties and phase equilibria of this binary system from ambient to high temperature conditions are not fully understood. Via high temperature oxidative drop calorimetry and detailed characterization of the initial and final phases, we have experimentally determined the standard enthalpies of formation of USi and U 3 Si 5.07 at 298 K to be –43.2 ± 6.2 and –43.8 ± 9.0 kJ/mol·atom, respectively. The energetics of the tetragonal USi (t-USi, space group I 4/ mmm ) phase has also been calculated with Density Functional Theory (DFT) for the first time. Combining the obtained formation enthalpies with the heat capacities measured previously, we assessed the thermodynamic stability of t-USi relative to a phase assemblage of two other U–Si phases, U 3 Si 5.07 and U 3 Si 2 , from ambient temperature to 1200 K. The tetragonal USi is thermodynamically more stable than U 3 Si 5.07 + U 3 Si 2 , which supports previously published phase diagram (H. Okamoto and T. Massalski, 1990 [1]): specifically, at least one stable USi phase exists when the U content is 50 at.%. In conclusion, further thermodynamic and phase equilibrium studies are needed for a more comprehensive understanding of the U–Si system across broader compositional and temperature ranges.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Research Needs for Uranium-Zirconium- Based Metallic Fuels

The purpose of this report is to summarize the needs and present recommendations related to the future direction for U-Zr-based metallic fuel research (including binary U-Zr and ternary U-Pu-Zr alloys). These needs and recommendations were determined by subject matter experts from various institutions during a two-day workshop held at the University of Florida in November, 2019. During open-floor discussions, the highest priority gaps in our understanding of U-Zr-based fuels were down-selected, and near- and long-term needs that directly impact the implementation of these metallic fuels were identified. The identified near-term needs include investigation of the following phenomena: i) swelling and fission gas release, ii) fuel-cladding chemical interaction, iii) phase evolution/constituent redistribution, and iv) thermal properties of the fuels. The long-term needs are: i) investigation of fuel creep and plasticity and ii) fission product (lanthanide) transport. In addition, there was general agreement that all institutions and subject matter experts would benefit from an open-source metallic fuels database with thermophysical property and microstructural data, along with fuel operation/irradiation history, which should be regularly updated with vetted information from new experimental and computational investigations and used to advance metallic fuels research and development. Finally, we recommend that metallic fuel research should be ongoing and that fuel qualification and fuel optimization should be equally prioritized; research combining experiments with modeling and simulation has the largest potential impact.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

The synthesis and air oxidation behavior of U-Si-Al and U-Si-B compositions

Uranium silicide intermetallic compounds are currently under investigation by the DOE-NE Advanced Fuels Campaign as candidate accident tolerant nuclear fuel concepts for light water reactors. While many U-Si compounds offer benefits compared to reference UO{sub 2} in terms of heavy metal density and thermal conductivity, they have been shown to display poor resistance to oxidizing atmospheres above 400 Celsius degrees. The general oxidation behavior of all U-Si compounds is oxidation of uranium; formation of UO{sub 2} followed by U{sub 3}O{sub 8} leads to rapid pulverization of the material. It is hypothesized that introducing an additional compositional degree of freedom by exploring U-Si-X (X=Al or B) ternary systems may provide the means to design a candidate nuclear fuel which optimizes the benefits of each binary. Phase analysis and preliminary oxidation testing were performed on four compositions containing alloying additions to U{sub 3}Si{sub 2} and U{sub 3}Si{sub 5}. Aluminum additions to U{sub 3}Si{sub 2} were observed to increase the oxidation resistance by delaying the onset of oxidation during synthetic air ramp testing. U{sub 3}Al{sub 2}Si{sub 3} delayed the onset of oxidation to T>650 C. degrees. During a 10 hour isothermal hold at 400 C. degrees in air the compound gained very little mass, indicating that it could be stable at reactor operating temperatures. Further analysis of this material is necessary to determine its oxidation behavior in steam and determine the specific mechanism that is providing the delayed oxidation. Boron additions to U{sub 3}Si{sub 5} do not appear to provide any additional oxidation resistance to the compound as tested in this work. The 1.67 at.% addition of B produced primarily single-phase composition. Melting and sintering studies followed by further compositional and thermal analyses are required to advance this composition as a candidate composite fuel additive. Lastly, the nominally U{sub 3}BSi{sub 4} composition produced a multi-phase system which provided no additional oxidation resistance following either a synthetic air ramp oxidation test or a pre-passivation isothermal hold at 800 C. degrees.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1998

The Coronae of Moderate-Mass Giants in the Hertzsprung Gap and the Clump

We have used the Roentgensatellit (ROSAT), the Extreme Ultraviolet Explorer (EUVE), and the Hubble Space Telescope (HST) to measure X-ray and ultraviolet emissions of moderate-mass (APPROX. 2-3 solar mass) giants in the Hertzsprung gap (spectral types early F to mid-G) and the post-helium flash "clump" (approx. G8-K0). Our motivation was to document the evolution of hot coronae (T greater than 10(exp 6)K) along the post-main-sequence trajectories traveled by such stars in order to gain insight concerning the "X-ray deficiency" of the F-GO giants and the strong braking of stellar rotation at the red edge of the Hertzsprung gap. With few exceptions, Hertzsprung gap and clump giants observed by ROSAT PSPC show hot (T approx. 10(exp 7)K) coronal energy distributions, regardless of any X-ray deficiency, EUVE spectra of gap star 31 Com (G0 111) indicate a broad coronal emission measure hump at approx. 10(exp 7.2)K, while the active clump giant beta Ceti (K0 III) displays a sharp peak at approx. 10(exp 6.8)K, as seen previously in the mixed clump/gap binary Capella (alpha Aur: G8 III + G0 III). The gap giants upsilon Peg (F8 III) and 24 UMa (G4 III) have EUV emissions of intermediate temperature (approx. 10(exp 7.0)K). The stars 31 Com, psi(sup 3) Psc (G0 III), and beta Cet exhibit redshifted transition zone (TZ: approx. 10(exp 5)K) lines in HST GHRS spectra, as reported earlier in Procyon (alpha CMi: F5 IV-V) and Capella G0. Such redshifts on the Sun are thought to signify flows in magnetic loops. beta Cas (F2 III)-a rare soft coronal source among the gap stars-displays blueshifts of C iv and 0 iv], although emissions at cooler and hotter temperatures are near the photospheric velocity. The remarkably broad line profiles of the fastest rotating gap giants suggest that the 10(exp 5) K "subcoronal " emission zones extend to h approx. R(sub *) above the photosphere, about 50 scale heights. In contrast to the TZ line redshifts, the upper chromospheric emissions (e.g., Mg II and Si III) of 31 Com and upsilon(sup 3) Psc have blueshifted cores. Blue-asymmetric peaks in the solar Mg a lines are thought to indicate dynamical heating in the chromosphere. Observations of the H(sub I) Ly(alpha) feature of 31 Com taken 9 months apart reveal striking profile changes, reminiscent of those noted previously in the Ly(alpha) blue peak of the Capella G0 star. We used the far-ultraviolet diagnostics, in combination with ROSAT X-ray photometry and EUVE high-excitation line strengths, to constrain physical models of the stellar outer atmospheres. Quasi-static magnetic loops can simulate the empirical coronal emission measures of the giant stars, but the inferred pressures for sensible loop lengths conflict with direct measurements of subcoronal densities. Furthermore, the high rate of emission at approx. 10(exp 5) K cannot be explained by thermal conduction down the legs of hot quasi-static loops. On the other hand, the possible existence of elongated (l - R(sub *) emission structures on the gap giants leads to a speculative scenario to explain the X-ray deficiency. It is based on the increased importance of the dynamical filling phase ("explosive evaporation") of the loop life cycle; conductive cooling, yielding TZ emissions at the footpoints, when the heating is interrupted; and the possibility for transitions between " hot " and " cool " energy balance solutions owing to dynamical suspension and centrifugal trapping of the cooling gas. The long loops might represent a vestigial global " magnetosphere " inherited from the main-sequence phase, which ultimately is disrupted near approx. G0 by the deepening convective envelope and growth of a more solar-like dynamo. Coronal emissions might be boosted temporarily as the X-ray deficiency is removed but soon would be quenched by wind braking previously inhibited by the magnetospheric "dead zone."

Ayres, Thomas R.↗

DOE OSTI2017

Sodium Pumping via Condensation within a Non-Wetting Porous Structure

The sodium thermal electrochemical converter (Na-TEC) is a heat engine that generates electricity via the isothermal expansion of sodium ions through a beta”-alumina solid-electrolyte. The transfer of liquid sodium from a low-pressure condenser to a high-pressure evaporator is necessary to complete the thermodynamic cycle for this conversion process. A unique sodium capillary pump for the Na-TEC is proposed, whereby low-pressure sodium vapor is condensed within a non-wetting (i.e. contact angle > 90o) stainless steel porous structure. Due to the curvature of the non-wetting liquid-vapor interface, the liquid adjacent to the interface is at a higher pressure than the vapor. This is in contrast to traditional wicks, where the liquid adjacent to the interface has a lower pressure. Thus, the curvature created at this non-wetting condensation interface supplies a directed force upon the liquid sodium that effectively “pushes” it towards a high pressure region, whereas a traditional capillary wick “pulls” the liquid. Porous structures made of stainless steel 316 are commercially available, and this material is non-wetting to sodium at the relevant temperature range of the Na-TEC condenser (500K – 673K). An experimental set-up is used to measure several interfacial and transport properties of the condensed sodium within this porous structure. These properties include the temperature dependent Laplace pressure generated at the phase change interface and the permeability of the porous structure. Liquid sodium is in contact with the porous structure and is progressively pressurized with argon gas until the sodium “breaks through” and the liquid begins to flow. This break-through pressure is determined when electrical contact is established between the flowing liquid metal and a set of electrodes cemented along the flow path. The velocity of the flowing sodium can also be measured with these electrodes, and the permeability is then determined by fitting velocity data to the classical Darcy law. These interfacial properties are then applied to a conjugate heat transfer model, which treats the coupled momentum and thermal transport processes within the non-wetting porous structure as sodium vapor is condensed. Due to the low mass flowrates in the Na-TEC (< 0.1 mg/s), higher order friction terms are neglected and the classical Darcy’s law is used for non-isothermal, compressible sodium vapor flow. At lower temperatures, the sodium vapor density becomes sufficiently small and there is a transition from classic Poiseuille flow (Kn < 0.1) to Knudsen flow (Kn > 10). Furthermore, transport due to binary diffusion is considered for situations where there is a substantial presence of non-condensable argon inside the sodium vapor plenum. Initial modeling results showing expected mass flowrates, temperature profiles, and liquid-vapor interface locations are presented for various physical conditions. Finally, the main design features of an experimental set-up used to demonstrate this capillary pumping is described in detail, including the method used to measure the low sodium mass flowrates. Initial experimental results demonstrating sodium pumping for a range of temperatures (800K – 1100K) will be presented and compared against the model predictions. A pump curve used to gauge the performance of this pumping mechanism is also created.

14 SOLAR ENERGY↗

NASA NTRS2016

Disk-Wind Connection During the Heartbeats of GRS 1915+105

Disk and wind signatures are seen in the soft state of Galactic black holes, while the jet is seen in the hard state. Here we study the disk-wind connection in the Rho class of variability in GRS 1915+105 using a joint NuSTAR-Chandra observation. The source shows 50 s limit cycle oscillations. By including new information provided by the reflection spectrum and using phase-resolved spectroscopy, we find that the change in the inner disk inferred from the blackbody emission is not matched by reflection measurements. The latter is almost constant, independent of the continuum model. The two radii are comparable only if the disk temperature color correction factor changes, an effect that could be due to the changing opacity of the disk caused by changes in metal abundances. The disk inclination is similar to that inferred from the jet axis, and oscillates by approx.10 deg. The simultaneous Chandra data show the presence of two wind components with velocities between 500 and 5000 km s(exp. −1), and possibly two more with velocities reaching 20,000 km s(exp. −1) (approx. 0.06 c). The column densities are approx. 5 × 10(exp. 22) cm(exp. −2). An upper limit to the wind response time of 2 s is measured, implying a launch radius of less than 6 × 10(exp. 10) cm. The changes in wind velocity and absorbed flux require the geometry of the wind to change during the oscillations, constraining the wind to be launched from a distance of 290-1300 r (sub g) from the black hole. Both data sets support fundamental model predictions in which a bulge originates in the inner disk and moves outward as the instability progresses.

accretion↗

NASA NTRS2002

Outbursts In Symbiotic Binaries (FUSE 2000)

During the past year, we made good progress on analysis of FUSE observations of the symbiotic binary Z And. For background, Z And is a binary system composed of a red giant and a hot component of unknown status. The orbital period is roughly 750 days. The hot component undergoes large-scale eruptions every 10-20 yr. An outburst began several years ago, triggering this FUSE opportunity. First, we obtained an excellent set of ground-based optical data in support, of the FUSE observations. We used FAST, a high throughput low resolution spectrograph on the 1.5-m telescope at Mt. Hopkins, Arizona. A 300 g/ mm grating blazed at 4750 A, a 3 in. slit, and a thinned Loral 512 x 2688 CCD gave us spectra covering 3800-7500 A at a resolution of 6 A. The wavelength solution for each spectrum has a probable error of +/- 0.5 A or better. Most of the resulting spectra have moderate signal-to-noise, S/.N approx. greater than 30 per pixel. The time coverage for these spectra is excellent. Typically, we acquired spectra every 1-2 nights during dark runs at Mt. Hopkins. These data cover most of the rise and all of the decline of the recent outburst. The spectra show a wealth of emission lines, including H I, He I, He II, [Fe V11], and the Raman scattering bands at 6830 A and 7088 A. The Raman bands and other high ionization features vary considerably throughout the outburst. These features will enable us to correlate variations in the FUSE spectra with variations in the optical spectra. Second, we began an analysis of FUSE spectra of Z And. We have carefully examined the spectra, identifying real features and defects. We have identified and measured fluxes for all strong emission lines, including the O VI doublet at 1032 A and 1038 A. These and several other strong emission lines display pronounced P Cygni absorption components indicative of outgrowing gas. We will attempt to correlate these velocities with similar profiles observed on optical spectra. The line velocities - together with line variations - will yield physical parameters for the expanding shell of gas in the outer atmosphere of the hot component. We also worked on several diagnostic tools, including upgrades to photoionization programs developed by the PI and others. We plan to use these tools to derive electron densities and temperatures front intercombination and forbidden lines observed on optical and FUSE spectra. Preliminary results indicate a large electron density, n(sub e) is greater than or = 10(exp 10)/cc and a modest electron temperature, T(sub e) approx. 20,000 K. We see no evidence for shocked gas as observed in some other symbiotics. However, we have yet to include several important lines of [Fe VII] and [Ne V] in the analysis. Inclusion of these lines will yield an improved estimate of the electron temperature in the gas. Finally, we have one additional FUSE spectrum planned for acquisition during this cycle. These data will provide important information concerning the state of the system farther along in its decline. Once we have this spectrum in hand, we plan to complete our analysis and publish our results.

Kenyon, Scott J.↗

DOE OSTI2015

On the [C ii]–SFR relation in high redshift galaxies

After two Atacama Large Millimeter/submillimeter Array (ALMA) observing cycles, only a handful of [C ii] 158 μm emission line searches in z > 6 galaxies have reported a positive detection, questioning the applicability of the local [C ii]–star formation rate (SFR) relation to high-z systems. To investigate this issue we use the Vallini et al. (V13) model,based on high-resolution, radiative transfer cosmological simulations to predict the [C ii] emission from the interstellar medium of a z ≈ 7 (halo mass M{sub h} = 1.17 × 10{sup 11} M{sub ⊙}) galaxy. We improve the V13 model by including (a) a physically motivated metallicity (Z) distribution of the gas, (b) the contribution of photodissociation regions (PDRs), and (c) the effects of cosmic microwave background (CMB) on the [C ii] line luminosity. We study the relative contribution of diffuse neutral gas to the total [C ii] emission (F{sub diff}/F{sub tot}) for different SFR and Z values. We find that the [C ii] emission arises predominantly from PDRs: regardless of the galaxy properties, F{sub diff}/F{sub tot} ≤ 10%, since at these early epochs the CMB temperature approaches the spin temperature of the [C ii] transition in the cold neutral medium (T{sub CMB} ∼ T{sub s}{sup CNM} ∼ 20 K). Our model predicts a high-z [C ii]–SFR relation, consistent with observations of local dwarf galaxies (0.02 < Z/Z{sub ⊙} < 0.5). The [C ii] deficit suggested by actual data (L{sub Cii} < 2.0 × 10{sup 7} L{sub ⊙} in BDF3299 at z ≈ 7.1) if confirmed by deeper ALMA observations, can be ascribed to negative stellar feedback disrupting molecular clouds around star formation sites. The deviation from the local [C ii]–SFR would then imply a modified Kennicutt–Schmidt relation in z > 6 galaxies. Alternatively/in addition, the deficit might be explained by low gas metallicities (Z < 0.1 Z{sub ⊙}).

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

In situ monitoring of microstructure evolution during thermal processing of uranium-zirconium alloys using laser-generated ultrasound

In this study, laser-generated ultrasound was used to monitor microstructure evolution during thermal processing of as-cast, polycrystalline binary uranium-zirconium metallic fuel alloys with compositions of U-20wt.%Zr (U-20Zr), U-50wt.%Zr (U-50Zr) and U-80wt.%Zr (U-80Zr). Ultrasonic waveforms were recorded during heating and cooling the samples from room temperature to >973 K and back. A phase transition temperature for all three compositions was estimated from the temperature at which an abrupt and rapid reduction in ultrasonic velocities was observed. Microstructural features on the length scale of tens of micrometers were inferred from the observation of scattering of ultrasonic waves by elastic heterogeneities above ~823 K in U-20Zr, while a hysteresis in the ultrasonic velocities of U-80Zr upon cooling was attributed to a partial retention of the high temperature phase following thermal annealing. The U-50Zr alloy exhibited a reversible viscoelastic response above 933 K, as evidenced by the observation of high frequency attenuation of the shear component of the waveforms at high temperature. Ultrasonic measurements were supplemented by in situ transmission electron microscopy (TEM). The TEM images revealed that the δ-U-Zr matrix in the three compositions underwent a spinodal decomposition above ~823 K into nanoscale regions. The ultrasonic measurements revealed larger, micron-scale structure evolution in the U-20Zr alloy at the same temperature. This large-scale structure is associated with heterogeneous regions having different Zr content. Our findings show the potential heating rate dependence of microstructural evolution in U-Zr alloys and highlight differences in the thermomechanical response and associated length scales during thermal annealing between single- and dual-phase compositions. These results demonstrate the utility of laser ultrasonics to rapidly and efficiently scan phase boundaries and monitor micrometer-scale structure evolution in metallic fuel alloys.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS2016

Spectral and Temporal Properties of the Ultra-Luminous X-Ray Pulsar in M82 from 15 Years of Chandra Observations and Analysis of the Pulsed Emission Using NuSTAR

The recent discovery by Bachetti et al. of a pulsar in M82 that can reach luminosities of up to 10(exp 40) erg s(exp -1), a factor of approximately 100 times the Eddington luminosity for a 1.4 solar mass compact object, poses a challenge for accretion physics. In order to better understand the nature of this source and its duty cycle, and in light of several physical models that have been subsequently published, we conduct a spectral and temporal analysis of the 0.58 keV X-ray emission from this source from 15 years of Chandra observations. We analyze 19 ACIS observations where the point-spread function (PSF) of the pulsar is not contaminated by nearby sources. We fit the Chandra spectra of the pulsar with a power-law model and a disk blackbody model, subjected to interstellar absorption in M82. We carefully assess for the effect of pile-up in our observations, where four observations have a pile-up fraction of 10, which we account for during spectral modeling with a convolution model. When fitted with a power-law model, the average photon index when the source is at high luminosity (LX greater than 10(exp 39) erg s(exp -1) is equal to gamma 1.33 +/-.0.15. For the disk blackbody model, the average temperature is T(sub in) 3.24 +/- 0.65 keV, the spectral shape being consistent with other luminous X-ray pulsars. We also investigated the inclusion of a soft excess component and spectral break, finding that the spectra are also consistent with these features common to luminous X-ray pulsars. In addition, we present spectral analysis from NuSTAR over the 3-50 keV range where we have isolated the pulsed component. We find that the pulsed emission in this band is best fit by a power-law with a high-energy cutoff, where gamma is equal to 0.6 +/- 0.3 and E(sub C) is equal to 14(exp +5) (sub -3)) keV. While the pulsar has previously been identified as a transient, we find from our longer-baseline study that it has been remarkably active over the 15-year period, where for 9/19 (47%) observations that we analyzed, the pulsar appears to be emitting at a luminosity in excess of 10( exp (39) erg s (exp −1), greater than 10 times its Eddington limit.

individual (M82) - stars: neutron X rays; binaries↗

DOE OSTI2025

3D pore structure reconstruction of fluff region in top of EBR-II irradiated fuel by X-ray micro-computed tomography

Metallic fuels comprised of U-Zr binary and U-Pu-Zr ternary alloys are a promising fuel candidate for sodium-cooled fast reactors and possess many advantages over ceramic fuels such as higher uranium density and improved thermal conductivity. Fluff is a highly porous structure forming at the top of metallic fuel slugs during irradiation and was extensively observed in past sodium-cooled fast reactor (SFR) experiments such as Idaho National Laboratory’s Experimental Breeder Reactor II (EBR-II). Previous investigations have shown that fluff is rich in fissile atoms and hence could have neutronics implications, but its formation mechanisms are not understood. In this work, two cube-shaped lift outs were taken from the fluff and bulk fuel regions of a high burnup U-19Pu-10Zr composition EBR-II fuel slug and characterized by micro computed tomography (Micro-CT) and energy dispersive x-ray spectroscopy (EDS). This was used to characterize differences in microscale porosity and composition between fluff and bulk fuel, and to support or oppose postulated fluff formation mechanisms. Surface EDS showed minimal differences between the elemental compositions of the fluff and fuel cubes. However, three-dimensional (3D) pore analysis from the tomography scans showed significant differences between the fluff and fuel cube pore size distributions at the microscale level. The high porosity and irregular pore distribution seen in macroscale fluff was also present within the micro-scale fluff cube, having a much higher porosity than the fuel cube which was concentrated in a few large pore networks. In conclusion, these results indicate support for a creep driven mechanism of fluff formation.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2018

Development and Rigorous Validation of Modules for Predicting Organic Aerosol CCN Activity from Molecular Properties

The indirect interaction of anthropogenic aerosols with clouds (aerosol indirect forcing) represents one of the main uncertainties in climate projections, and reducing this uncertainty requires improved understanding of the aerosol life cycle, including atmospheric aging and the ability to nucleate cloud droplets or crystals. A key parameter that links the chemical properties of aerosol to its nucleating properties, and ultimately to aerosol indirect forcing, is its hygroscopicity (ability to uptake water). One way to compare and systematize the ability of various chemical compounds or particle types to nucleate cloud drops is via the hygroscopicity parameter κ, which can be used directly in global models to simulate aerosol indirect forcing. In this project we further investigated the relationships between the chemical composition of organic aerosol particles, which are known to be important components of atmospheric particulate matter, and their ability to serve as cloud condensation nuclei (CCN). In particular, we isolated the role of viscosity on κ by applying methods similar to those we used previously in our DOE/ASR research. Our motivation for the focus on viscosity was through its link to particle phase state. Particle phase affects water uptake on timescales relevant to the laboratory and also likely relevant to atmospheric processes, with reduced apparent hygroscopicities for semisolid and solid particles, compared with liquid particles. Water uptake itself affects viscosity, an important feedback that we explored in this project. The objectives of the project were as follows: (1) measure the effects of molecular structure, temperature, and relative humidity on the viscosity of organic aerosol formed via controlled laboratory experiments, (2) measure the effects of organic aerosol viscosity on water uptake and CCN activity above and below water saturation, (3) further develop the κ parameterization of organic aerosol hygroscopicity to include viscosity/phase, and (4) experimentally validate the κ parameterization for organic aerosol with chemical composition ranging from relatively simple to complex. It was proposed that particle viscosity exerts a kinetic control on equilibrium water uptake. High viscosity was expected to delay water uptake based on diffusional limitations. This would manifest itself in reduced observed CCN activity or κ. Understanding the interplay between water content and viscosity (composition control on particle viscosity) and between viscosity and equilibrium water content (diffusional control on water uptake) were the overall science objectives of this grant. Targeted experiments were carried out to test the kinetic control hypothesis. These experiments included studies that explicitly measured the equilibration time scale of water uptake, and experiments that tested the role of viscous particle coatings on the observed CCN activity. From the combined work, it is concluded that mass transfer limitations by glassy organic particles are unlikely to affect cloud droplet activation near laboratory temperatures. This implies that viscosity does not need to be included in parameterizations that link particle chemical composition and κ. A parameterization to predict κ through the UNIFAC group contribution method was developed with previous ASR funding. As planned, this computational module was further developed and validated here through targeted laboratory studies. The computational module has been made available as free software under the GNU public license. A database of κ-values to aid model development has been compiled and is available online via an open access model. In conducting this work, significant effort was made to understand how aerosol composition, including the associated aerosol water content, affects viscosity. This included a study detailing the influence of functional group composition on organic aerosol viscosity. We identified a strong link between volatility and viscosity. Functional groups responsible for low vapor pressure also promote high viscosity. Specifically, carboxylic acid and hydroxyl groups were identified as major contributors to high viscosity. Several studies were carried out to characterize the link between composition and the glass-to-liquid phase transition. Compositions tested include models of organic/inorganic particles and models of complex organic aerosol formed through secondary processes. A simple computational model to predict the amorphous phase diagram was developed and tested. Excellent agreement between model and measurements was obtained for organic/inorganic mixtures. The computational model is simple enough to be included in global model simulations. However, constraints of input parameters such as the Gordon-Taylor constant for binary mixtures for a wide range of complex mixtures have not yet been fully evaluated. Combined, the performed work provides new constraints on the amorphous phase state of organic aerosols.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Geothermal Risk Reduction via Geothermal/Solar Hybrid Power Plants. Final Report

There are numerous technical merits associated with a renewable geothermal-solar hybrid plant concept. The performance of air-cooled binary plants is lowest when ambient temperatures are high due to the decrease in air-cooled binary plant performance that occurs when the working fluid condensing temperature, and consequently the turbine exhaust pressure, increases. Electrical power demand is generally at peak levels during periods of elevated ambient temperature and it is therefore especially important to utilities to be able to provide electrical power during these periods. The time periods in which air-cooled binary geothermal power plant performance is lowest generally correspond to periods of high solar insolation. Use of solar heat to increase air-cooled geothermal power plant performance during these periods can improve the correlation between power plant output and utility load curves. While solar energy is a renewable energy source with long term performance that can be accurately characterized, on shorter time scales of hours or days it can be highly intermittent. Concentrating solar power (CSP), aka solar-thermal, plants often incorporate thermal energy storage to ensure continued operation during cloud events or after sunset. Hybridization with a geothermal power plant can eliminate the need for thermal storage due to the constant availability of geothermal heat. In addition to the elimination of the requirement for solar thermal storage, the ability of a geothermal/solar-thermal hybrid plant to share a common power block can reduce capital costs relative to separate, stand-alone geothermal and solar-thermal power plant installations. The common occurrence of long-term geothermal resource productivity decline provides additional motivation to consider the use of hybrid power plants in geothermal power production. Geothermal resource productivity decline is a source of significant risk in geothermal power generation. Many, if not all, geothermal resources are subject to decreasing productivity manifested in the form of decreasing production fluid temperature, flow rate, or both during the life span of the associated power generation project. The impacts of geothermal production fluid temperature decline on power plant performance can be significant; a reduction in heat input to a power plant not only decreases the thermal energy available for conversion to electrical power, but also adversely impacts the power plant efficiency. The impact of resource productivity decline on power generation project economics can be equally detrimental. The reduction in power generation is directly correlated to a reduction in revenues from power sales. Further, projects with Power Purchase Agreement (PPA) contracts in place may be subject to significant economic penalties if power generation falls below a specified default level. While the magnitude of PPA penalties varies on a case-by-case basis, it is not unrealistic for these penalties to be on the order of the value of the deficit power sales such that the utility may purchase the power elsewhere. This report evaluates the use of geothermal/solar-thermal hybrid plant technology for mitigation of resource productivity decline, which has not been a primary topic of investigation in previous analyses in the open literature.

14 SOLAR ENERGY↗

DOE OSTI2023

FY23 Progress Report on Viscosity and Thermal Conductivity Measurements of Molten Salts

As presented in this report, thermal conductivity and viscosity measurements were performed on key chloride pseudo-binary molten salt systems of relevance to molten salt reactor developers. Thermal conductivity measurements were conducted with a variable gap technique, in which a known heat flux is driven across a molten salt specimen and the temperature difference is measured, allowing calculation of the thermal conductivity. This is achieved by establishing a small gap between the bottom of a cylindrical inner containment, which houses electrical heating elements, and an outer containment, which houses cooling channels; the gap size can be varied by compression of a formed bellows. A new calibration scheme was developed herein, involving a correction factor to the heat flux based on He measurements at various temperatures. Furthermore, the data processing methodology was improved to minimize the impact of radiative heat transfer in the calculation of salt specimen thermal conductivity from the temperature difference measurements. Viscosity measurements were conducted with a rolling ball viscometer, in which a ball rolls some known distance in an angled tubular crucible, and the terminal velocity can be used to calculate the viscosity of the salt. The measurement can be performed in a quartz crucible, with which a standard camera can be used to track the ball, or in a metal crucible, with which x-ray radiography is required to track the ball. A new custom x-ray system was made and dedicated to the rolling ball viscometer to enable high throughput automated measurements with salts which require containment with metal. Both systems have been integrated with a ventilation stack which allows for off-gassing of radioactive material, enabling future measurements with U-bearing salts. The thermal conductivity measurements performed herein were with NaCl-KCl (44 mol% NaCl). This salt system was measured in the previous fiscal year, however the thermal conductivity values obtained were comparatively low, and so the system was remeasured with the aforementioned calibration scheme and improved post-processing techniques. The newly obtained thermal conductivity values for NaCl-KCl (44 mol% NaCl) indicate good agreement with kinetic theory and ab-initio models (within 5–10 %). The viscosity measurements performed herein were with three different compositions of NaCl-KCl: 75, 50, and 25 mol% NaCl; a new calibration scheme was applied to account for variable flow effects in the laminar regime. The results show reasonable agreement with literature (5–20 %, depending on the temperature, composition, and study); however, literature values are likely higher than true values based on pure end-member measurements performed in the comparative studies. The measurements conducted herein do show a trend such that viscosity increases with increasing NaCl concentration, which agrees well with one of two comparative studies. In general, the measurements conducted herein gives confidence in the capability to use these systems to accurately measure thermal conductivity and viscosity of actinide-bearing salts within the next fiscal year.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗