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DOE OSTI2023

3D Quantification of Elemental Gradients within Heterostructured Particles of Battery Cathodes

Heterogenous architectures with elemental gradients tailored within particles have been pursued to combat the instabilities limiting Ni-rich cathode materials for lithium-ion batteries. The growth of different compositional layers is accomplished during the synthesis of hydroxide precursors. However, the extent to which these concentration gradients are modified during high-temperature reactions is difficult to establish in their intact, spherical form. Here, we show the entire three-dimensional structure of a secondary particle can be resolved nondestructively with differential X-ray absorption spectroscopy (XAS) through transmission X-ray microscopy (TXM). The relationship between particle location and elemental content was fully quantified, with high statistical significance, for heterostructures possessing different compositional gradients in the precursors with 90:5:5 Ni:Mn:Co core compositions. Reduced elemental heterogeneity was observed after high-temperature synthesis, but gradients remained. In conclusion, the methodology presented should be used to guide synthesis while assuring that gains in electrochemical performance are linked to precise elemental distributions at the nanoscale.

25 ENERGY STORAGE↗

DOE OSTI2020

Uncertainty amplification due to density/refractive index gradients in background-oriented schlieren experiments

Here, we theoretically analyze the effect of density/refractive index gradients on the measurement precision of background-oriented schlieren (BOS) experiments by deriving the Cramer–Rao lower bound (CRLB) for the 2D centroid estimation process. A model is derived for the diffraction limited image of a dot viewed through a medium containing density gradients that includes the effect of the experimental parameters such as the magnification and f-number. It is shown using the model that nonlinearities in the density gradient field lead to blurring of the dot image. This blurring amplifies the effect of image noise on the centroid estimation process, leading to an increase in the CRLB and a decrease in the measurement precision. The ratio of position uncertainties of a dot in the reference and gradient images is shown to be a function of the ratio of the dot diameters and dot intensities. We termed this parameter the amplification ratio (A F ), and a methodology for reporting position uncertainties in tracking-based BOS measurements is proposed. The theoretical predictions of the dot position estimation variance from the CRLB are compared to ray tracing simulations, and agreement is obtained. The uncertainty amplification is also demonstrated on experimental BOS images of flow induced by a spark discharge, where it is seen that regions of high amplification ratio correspond to regions of density gradients. This analysis elucidates the dependence of the position uncertainty on density and refractive index gradient-induced distortion parameters, provides a methodology for accounting its effect on uncertainty quantification and provides a framework for optimizing experiment design.

42 ENGINEERING↗

NASA NTRS1975

Kinetics of boron deposition by the hydrogen reduction of boron trichloride

The chemical vapor deposition of boron filament is generally considered to be limited by the diffusion of the reactive species to the hot substrate. From concentration gradient considerations and from experimental measurements it is concluded that the product species (HCl) is more likely to be involved in limiting the deposition rate. Comparison of theoretically calculated and experimentally measured deposition rates show that the rate is generally partially limited by diffusion and partially by the surface reaction rate (desorption) of HCl. The relative amounts of surface reaction or diffusion rate impedance were determined as a function of temperature and gas velocity. The temperature coefficient for the desorption of HCl was found to be 52 Kcal/mole.

Mehalso, R. M.↗

DOE OSTI2014

Field of view extension and truncation correction for MR-based human attenuation correction in simultaneous MR/PET imaging

Purpose: In quantitative PET imaging, it is critical to accurately measure and compensate for the attenuation of the photons absorbed in the tissue. While in PET/CT the linear attenuation coefficients can be easily determined from a low-dose CT-based transmission scan, in whole-body MR/PET the computation of the linear attenuation coefficients is based on the MR data. However, a constraint of the MR-based attenuation correction (AC) is the MR-inherent field-of-view (FoV) limitation due to static magnetic field (B{sub 0}) inhomogeneities and gradient nonlinearities. Therefore, the MR-based human AC map may be truncated or geometrically distorted toward the edges of the FoV and, consequently, the PET reconstruction with MR-based AC may be biased. This is especially of impact laterally where the patient arms rest beside the body and are not fully considered. Methods: A method is proposed to extend the MR FoV by determining an optimal readout gradient field which locally compensates B{sub 0} inhomogeneities and gradient nonlinearities. This technique was used to reduce truncation in AC maps of 12 patients, and the impact on the PET quantification was analyzed and compared to truncated data without applying the FoV extension and additionally to an established approach of PET-based FoV extension. Results: The truncation artifacts in the MR-based AC maps were successfully reduced in all patients, and the mean body volume was thereby increased by 5.4%. In some cases large patient-dependent changes in SUV of up to 30% were observed in individual lesions when compared to the standard truncated attenuation map. Conclusions: The proposed technique successfully extends the MR FoV in MR-based attenuation correction and shows an improvement of PET quantification in whole-body MR/PET hybrid imaging. In comparison to the PET-based completion of the truncated body contour, the proposed method is also applicable to specialized PET tracers with little uptake in the arms and might reduce the computation time by obviating the need for iterative calculations of the PET emission data beyond those required for reconstructing images.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2021

Learning electric vehicle driver range anxiety with an initial state of charge-oriented gradient boosting approach

This manuscript focuses on the modeling of electric vehicle (EV) driver’s range anxiety, a fear that a vehicle does not have sufficient range, or state of charge (SOC) of the battery pack, to reach its destination and would strand its occupants. Despite numerous research studies on the modeling of charging behaviors, modeling efforts to understand at what battery percentages do EV drivers charge their vehicles, and what are the associated contributing factors, are rather limited. To this end, an ensemble learning model based on gradient boosting is developed. The model sequentially fits new predictors to new residuals of the previous prediction and, then, minimizes the loss when adding the latest prediction. A total of 18 features are defined and extracted from the multisource data, which cover information on driver, vehicles, stations, traffic conditions, as well as spatial-temporal context information of the charging events. The analyzed dataset includes 4.5-year’s charging event log data from 3,096 users and 468 public charging stations in Kansas City Missouri, and the macroscopic travel demand model maintained by the metropolitan planning organization. Here, the result shows the proposed model achieved a satisfactory result with a R square value of 0.54 and root mean square error of 0.14, both better than multiple linear regression model and random forest model. To reduce range anxiety, it is suggested that the priorities of deploying new charging facilities should be given to the areas with higher daily traffic prediction, with more conservative EV users or that are further from residential areas.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2021

Rational design of mechanically robust Ni-rich cathode materials via concentration gradient strategy

Mechanical integrity issues such as particle cracking are considered one of the leading causes of structural deterioration and limited long-term cycle stability for Ni-rich cathode materials of Li-ion batteries. Indeed, the detrimental effects generated from the crack formation are not yet entirely addressed. Here, applying physicochemical and electrochemical ex situ and in situ characterizations, the effect of Co and Mn on the mechanical properties of the Ni-rich material are thoroughly investigated. As a result, we successfully mitigate the particle cracking issue in Ni-rich cathodes via rational concentration gradient design without sacrificing the electrode capacity. Our result reveals that the Co-enriched surface design in Ni-rich particles benefits from its low stiffness, which can effectively suppress the formation of particle cracking. Meanwhile, the Mn-enriched core limits internal expansion and improve structural integrity. The concentration gradient design also promotes morphological stability and cycling performances in Li metal coin cell configuration.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Evolution of microstructure and microtexture during hot deformation in an advanced P/M nickel base superalloy

Highlights: • Microstructural evolution of PM superalloy sensitive to temperature and strain rate. • Highest DRX with finer grained structure at higher temperatures and strain rates. • Dominance of DDRX showed by serrated grain boundaries and misorientation gradient. • Weak microtextural evolution inclined towards [110] fiber compression texture seen. In the present study, the effect of hot deformation parameters on the microstructural evolution is investigated for an experimental powder metallurgy nickel superalloy. The hot isostatically pressed (HIPed) alloy is isothermally hot compressed at constant true strain rate over wide temperatures (1000 °C, 1050 °C, 1100 °C, 1150 °C) and strain rates (0.001 s{sup −1}, 0.01 s{sup −1}, 0.1 s{sup −1}, 1 s{sup −1}) regimes. Electron Back-Scattered Diffraction (EBSD) characterization of the hot deformed samples is carried out to evaluate the microstructural evolution, grain boundary characteristics, and microtextural behaviour. The strong dependence of dynamic recrystallization characteristics on the hot deformation conditions is divulged through EBSD derived colour inverse pole figure maps endorsed by grain/twin boundary characteristics and misorientation gradient. Dynamic recrystallization (DRX) is maximized at higher deformation temperatures, whereas limited DRX is observed at lower deformation temperatures, especially at higher strain rates. The dominance of discontinuous dynamic recrystallization (DDRX) is manifested through bulged/serrated grain boundaries resulting in the formation of necklace microstructure corroborated by grain boundary cumulative misorientation gradient. Although random microtexture is revealed in both deformed and recrystallized microstructures, the tendency towards the formation of 110 fiber compression texture is apparently evident.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Suppression of Deflecting Forces in Planar-Symmetric Dielectric Wakefield Accelerating Structures with Elliptical Bunches

Wakefield based accelerators capable of accelerating gradients two orders of magnitude higher than present accelerators offer a path to compact high energy physics instruments and light sources. However, for high gradient accelerators, beam instabilities driven by commensurately high transverse wakefields limit beam quality. It has been previously theoretically shown that transverse wakefields can be reduced by elliptically shaping the transverse sizes of beams in dielectric structures with planar symmetry. We report here experimental measurements that demonstrate reduced transverse wakefields for elliptical beams in planar symmetric structures which are consistent with theoretical models. Furthermore, these results may enable the design of gigavolt-per-meter gradient wakefield based accelerators that produce and stably accelerate high quality beams.

47 OTHER INSTRUMENTATION↗

NASA NTRS1978

An experimental study of three-dimensional turbulent boundary layer and turbulence characteristics inside a turbomachinery rotor passage

Three-dimensional boundary layer and turbulence measurements of flow inside a rotating helical channel of a turbomachinery rotor are described. The rotor is a four-bladed axial flow inducer operated at large axial pressure gradient. The mean velocity profiles, turbulence intensities and shear stresses, and limiting stream-line angles are measured at various radial and chordwise locations, using rotating triaxial hot-wire and conventional probes. The radial flows in the rotor channel are found to be higher compared to those at zero or small axial pressure gradient. The radial component of turbulence intensity is found to be higher than the streamwise component due to the effect of rotation. Flow near the annulus wall is found to be highly complex due to the interaction of the blade boundary layers and the annulus wall resulting in an appreciable radial inward flow, and a large defect in the mainstream velocity. Increased level of turbulence intensity and shear stresses near the midpassage are also observed near this radial location.

Anand, A. K.↗

DOE OSTI2013

X-ray driven channeling acceleration in crystals and carbon nanotubes

Acceleration of particles channeling in a crystal by means of diffracted x-rays via Bormann anomalous transmission was conceived for heavy ions and muons by Tajima and Cavenago [Phys. Rev. Lett. 59, 1440 (1987)], which potentially offers an appreciably high field gradient on the order of GV/cm. The theoretical model of the high gradient acceleration has been studied in two kinds of atomic structure, crystals and carbon nanotubes (CNTs), with analytic calculations and electromagnetic eigenmode simulations. A range of acceleration gradients and cutoffs of the x-ray power (the lowest power limit to overcome the Bremsstrahlung radiation losses) are characterized in terms of the lattice constants, unit cell sizes, and photon energies. The parametric analysis indicates that the required x-ray power can be reduced to an order of megawatt by replacing crystals with CNTs. Eventually, the equivalent dielectric approximation of a multi-wall nanotube shows that 250–810 MeV muons can be synchronously coupled with x-rays of 0.65–1.32 keV in the accelerating structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRSDate not supplied

Simulation and Modeling of Hypersonic Turbulent Boundary Layers Subject to Favorable Pressure Gradients due to Streamline Curvature

Direct numerical simulations (DNS) of favorable-pressure-gradient turbulent boundary layers are presented for a nominal freestream Mach number of 5, with the objective of assessing the limitations of the currently available Reynolds-averaged Navier-Stokes (RANS) models. The favorable pressure gradient is induced by the streamwise curvature of the two-dimensional, planar, convex measurement surface used during experiments at the Texas A&M University. The DNS data shows good comparison with the measured velocity profiles, strain rates, and some, but not all, of the Reynolds-stress components. The discrepancies between the predicted and the measured wall-normal as well as shear stress components are primarily attributed to the lower than actual values inferred from typical PIV measurements of turbulent boundary layers. The DNS data shows a zero or slightly negative Reynolds shear stress in the outer part of the boundary-layer, which is indicative of the decaying turbulent motion under a strong favorable pressure gradient. The DNS data is also compared with the results of RANS computations based on commonly used zero, one, and two equation eddy-viscosity models. The RANS models yield reasonable comparisons with the DNS-based skin friction under zero and weak pressure gradients, but significant discrepancies under a strong pressure gradient. The k-w SST model provided the best overall predictions of skin friction, except in the region where the flow transitions from a favorable to an adverse pressure gradient. While the RANS models examined herein also give good predictions of the Reynolds shear stress under a sufficiently weak pressure gradient, none of those models are able to appropriately capture the reduction in the Reynolds stresses when the flow was subjected to a strong pressure gradient. An a priori assessment of the turbulent heat-flux prediction based on the assumption of a constant turbulent Prandtl number with the DNS data shows that while the constant turbulent Prandtl number model is effective in predicting the wall-normal component of turbulent heat flux, it does not capture the turbulent heat transfer in the streamwise direction for all the pressure gradient cases. The failure of the constant turbulent Prandtl number model highlights a requirement for more advanced models of the turbulent heat flux.

turbulent boundary layers↗

DOE OSTI2022

Gradient porosity electrodes for fast charging lithium-ion batteries

The tendency of Li plating at the surface of thick graphite electrodes greatly limits their application in electrical vehicle (EV) batteries for fast charging applications. To address this concern, we proposed an innovative gradient porosity architecture to facilitate mass transport and suppress Li plating in the thick anodes for fast charging applications. This concept was approved through a thick 3-layered graphite electrode with the highest porosity in the top layer and the lowest porosity in the bottom layer, in contact with the current collector. Here, the gradient porosity structure in the 3-layered graphite electrodes was confirmed by electron microscopy and mercury porosimetry measurements. Used as the anodes of lithium-ion batteries, 3-layered graphite electrodes demonstrated unprecedentedly rate capability and durability superior to 1-layered electrodes. The post-mortem analysis on the cycled cells shows that 3-layered electrodes can significantly suppress Li plating at a high rate up to 4C, which might be responsible for the improved performance of the derived cells. The excellent electrochemical behaviors of 3-layered graphite electrodes are associated with the favored mass transport originating from the unique gradient porosity structure. This is consistent with theoretical studies showing that gradient porosity lowers the Li-ion concentration gradient in the electrolyte in the region close to the separator and slows down the process of reaching the Li plating threshold.

25 ENERGY STORAGE↗

NASA NTRS2019

Twentieth Century Redistribution in Climatic Drivers of Global Tree Growth

Energy and water limitations of tree growth remain insufficiently understood at large spatiotemporal scales, hindering model representation of interannual or longer-term ecosystem processes. By assessing and statistically scaling the climatic drivers from 2710 tree-ring sites, we identified the boreal and temperate land areas where tree growth during 1930–1960 CE responded positively to temperature (20.8 ± 3.7 Mio km2; 25.9 ± 4.6%), precipitation (77.5 ± 3.3 Mio km2; 96.4 ± 4.1%), and other parameters. The spatial manifestation of this climate response is determined by latitudinal and altitudinal temperature gradients, indicating that warming leads to geographic shifts in growth limitations. We observed a significant (P < 0.001) decrease in temperature response at cold-dry sites between 1930–1960 and 1960–1990 CE, and the total temperature-limited area shrunk by −8.7 ± 0.6 Mio km2. Simultaneously, trees became more limited by atmospheric water demand almost worldwide. These changes occurred under mild warming, and we expect that continued climate change will trigger a major redistribution in growth responses to climate.

Babst, Flurin↗

DOE OSTI2015

Improved DC Gun and Insulator Assembly

Many user facilities such as synchrotron radiation light sources and free electron lasers rely on DC high voltage photoguns with internal field gradients as high as 10 to 15 MV/m. These high gradients often lead to field emission which poses serious problems for the photocathode used to generate the electron beam and the ceramic insulators used to bias the photocathode at high voltage. Ceramic insulators are difficult to manufacture, require long commissioning times, and have poor reliability, in part because energetic electrons bury themselves in the ceramic causing a buildup of charge and eventual puncture, and also because large diameter ceramics are difficult to braze reliably. The lifetimes of photo cathodes inside high current DC guns exhibiting field emission are limited to less than a hundred hours. Reducing the surface gradients on the metals reduces the field emission, which serves to maintain the required ultrahigh vacuum condition. A novel gun design with gradients around 5 MV/m and operating at 350 kV, a major improvement over existing designs, was proposed that allows for the in-situ replacement of photo cathodes in axially symmetric designs using inverted ceramics. In this project, the existing JLAB CEBAF asymmetric gun design with an inverted ceramic support was modeled and the beam dynamics characterized. An improved structure was designed that reduces the surface gradients and improves the beam optics. To minimize the surface gradients, a number of electrostatic gun designs were studied to determine the optimum configuration of the critical electrodes within the gun structure. Coating experiments were carried out to create a charge dissipative coating for cylindrical ceramics. The phase II proposal, which was not granted, included the design and fabrication of an axially symmetric DC Gun with an inverted ceramic that would operate with less than 5 MV/m at 350 kV and would be designed with an in-situ replaceable photo-cathode.

43 PARTICLE ACCELERATORS↗

DOE OSTI2015

Searching for quantum optimal controls under severe constraints

The success of quantum optimal control for both experimental and theoretical objectives is connected to the topology of the corresponding control landscapes, which are free from local traps if three conditions are met: (1) the quantum system is controllable, (2) the Jacobian of the map from the control field to the evolution operator is of full rank, and (3) there are no constraints on the control field. This paper investigates how the violation of assumption (3) affects gradient searches for globally optimal control fields. The satisfaction of assumptions (1) and (2) ensures that the control landscape lacks fundamental traps, but certain control constraints can still prevent successful optimization of the objective. Using optimal control simulations, we show that the most severe field constraints are those that limit essential control resources, such as the number of control variables, the control duration, and the field strength. Proper management of these resources is an issue of great practical importance for optimization in the laboratory. For each resource, we show that constraints exceeding quantifiable limits can introduce artificial traps to the control landscape and prevent gradient searches from reaching a globally optimal solution. These results demonstrate that careful choice of relevant control parameters helps to eliminate artificial traps and facilitate successful optimization.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

RACORO continental boundary layer cloud investigations. Part I: Case study development and ensemble large-scale forcings

Observation-based modeling case studies of continental boundary layer clouds have been developed to study cloudy boundary layers, aerosol influences upon them, and their representation in cloud- and global-scale models. Three 60-hour case study periods span the temporal evolution of cumulus, stratiform, and drizzling boundary layer cloud systems, representing mixed and transitional states rather than idealized or canonical cases. Based on in-situ measurements from the RACORO field campaign and remote-sensing observations, the cases are designed with a modular configuration to simplify use in large-eddy simulations (LES) and single-column models. Aircraft measurements of aerosol number size distribution are fit to lognormal functions for concise representation in models. Values of the aerosol hygroscopicity parameter, κ, are derived from observations to be ~0.10, which are lower than the 0.3 typical over continents and suggestive of a large aerosol organic fraction. Ensemble large-scale forcing datasets are derived from the ARM variational analysis, ECMWF forecasts, and a multi-scale data assimilation system. The forcings are assessed through comparison of measured bulk atmospheric and cloud properties to those computed in 'trial' large-eddy simulations, where more efficient run times are enabled through modest reductions in grid resolution and domain size compared to the full-sized LES grid. Simulations capture many of the general features observed, but the state-of-the-art forcings were limited at representing details of cloud onset, and tight gradients and high-resolution transients of importance. Methods for improving the initial conditions and forcings are discussed. The cases developed are available to the general modeling community for studying continental boundary clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Monitoring and modulating ion traffic in hybrid lipid/polymer vesicles

Controlling the traffic of molecules and ions across membranes is a critical feature in a number of biologically relevant processes and highly desirable for the development of technologies based on membrane materials. In this study, ion transport behavior of hybrid lipid/polymer membranes was studied in the absence and presence of ion transfer agents. A pH-sensitive fluorophore was used to investigate ion (H + /OH - ) permeability across hybrid lipid/polymer membranes as a function of the fraction of amphiphilic block copolymer. It was observed that vesicles with intermediate lipid/polymer ratios tend to be surprisingly more permeable to ion transport than the pure lipid or pure polymer vesicles. Hybrid vesicle permeability could be further modulated with valinomycin, nigericin, or gramicidin A, which significantly expedite the dissipation of externally-imposed pH gradients by facilitating the transport of the rate-limiting co-ions (e.g. K + ) ions across the membrane. For gramicidin A, ion permeability decreased with increasing polymer mole fraction, and the method of introduction of gramicidin A into the membrane played an important role. Finally, strategies to incorporate biofunctional molecules and facilitate their activity in synthetic systems are highly desirable for developing artificial organelles or other synthetic compartmentalized structures requiring control over molecular traffic across biomimetic membranes.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2018

Fabrication of localised aluminium foam by a novel polymeric blowing agent

Highlights: • Polymeric blowing agent used to synthesize metallic foam for first time. • Localised region of a metallic part is foamed. • A novel semisolid route is used to control the pore size of the foams. • Heat-treatable foam with controllable absorption energy is obtained. - Abstract: Closed cell aluminium foams are highly pursued, due to their unique combination of properties. However, the current applicability of the aluminium foams is limited due to issues like high costs, density-gradient and brittleness of the cell walls, which are either related to use of metallic hydride as blowing agent or liquid-state processing. To address these issues, this study presents a first attempt to use polymer as a blowing agent to foam an aluminium alloy. A polymer is Poly (methyl hydro siloxane) was dispersed into an Al2024 sheet of 6 mm by Friction Stir Processing, in a localised region. This processed sample was pyrolysed at temperatures between solidus and liquidus (500–640 °C) of the alloy and at various durations (5–60 min) to foam the localised precursor. The density of resulting foams was measured by the Archemidies method and the resulting pore structures were characterised by Scanning Electron Microscopy (SEM) and micro X-ray Computed Tomography (CT). The results show that by as pyrolysis temperature increases relative density reaches a minimum of 0.65 at 560 °C. Beyond 590 °C, relative density increased from the optimum due to escape of foaming gasses. With increasing pyrolysis temperature, the pore size increased from few microns to several hundred microns. Further, quasi-static compression test was done on as processed, solutionized and aged foams. Due to increased strain hardening in aged samples energy absorbed during compression increased by 80% in the plateau region. Hence, polymeric a blowing agent can be used to synthesize heat-treatable foams with controllable absorption energy.

36 MATERIALS SCIENCE↗