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At least 595 records · Page 33

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NASA NTRS2016

Interfacial Structure and Capacitance of Li-doped Ionic Liquid Electrolytes from Molecular Simulations

Ionic liquids have been proposed as candidate electrolytes for high-energy density, rechargeable batteries, supercapacitors, and hybrid energy storage devices. Though Li-salt is often present in these systems, its influence on interfacial properties is largely uncharacterized. We, thereby, present an extensive computational analysis, supported by experimental comparisons, of the properties of a representative set of these electrolytesat an ideal carbon interface as a function of Li-salt doping and voltage. We have performed polarizable molecular (MD) dynamics simulations, using the APPLEP force field, to evaluate electric double layer (EDL) capacitance and distribution of Li+ in the EDL. Differential capacitance exhibits the characteristic camel profile and is insensitive to Li-doping. Li+ localizes in the second molecular layer of the EDL, which is a result of confinement from free energy barriers associated with ion layering. Joint MDelectronic structure computations show the electrochemical window of the electrolytes to be a weak function of Li-doping. Estimates of supercapacitor specific energy are made using the computed window and capacitance. The magnitude and trends in specific energy are in good agreement with experiment.

batteries↗

NASA NTRS2002

Local Conductance and Saturation Lengths of Atomic Wires Dipped in a Conducting Medium

We conclude that the conducting mode pi is the most likely responsible for conduction in experimental mercury-nanotube contacts. The total conductance approaches a saturation value as the dipping length is increased. There are two distinct regimes, strong and weak coupling, characterized by saturation conductances of 0 or 1G(sub o). We have calculated the partial conductance at each nanotube unit cell. The partial conductance exhibits oscillations due to reflection at the end of the tube.

OKeeffe, James↗

DOE OSTI2022

Evaluation of Horizon of Viability Optimization Engine for Sustained Power to Critical Infrastructure: Preprint

In the aftermath of increasingly frequent catastrophic events, a typical scenario is Critical Infrastructure (CI) units being supported by available backup sources with a weak power grid that can be intermittent or absent. Such a scenario is significantly challenging in the sense of reliable supply of power to CI units. In this article, an intelligent optimization scheme termed as Horizon of Viability (HoV) engine is developed to guarantee the viability of a sustained reliable supply of power to the CI units over a time-horizon. The proposed HoV engine generates a cost-optimal portfolio of the locally available generation sources and the loads over a time horizon using a mixed-integer convex programming problem. A Controller hardware-in-the-loop (CHIL) platform is developed to evaluate the control performance of the HoV engine. The experimental results corroborates the efficacy in maintaining the viability of the CI units after a grid interruption event. Further, the proposed HoV optimization scheme performs better compared to existing net-load management schemes in the literature.

disaster resiliency↗

DOE OSTI2023

The s process in massive stars, a benchmark for neutron capture reaction rates

A clear definition of the contribution from the slow neutron-capture process (s process) to the solar abundances between Fe and the Sr-Zr region is a crucial challenge for nuclear astrophysics. Robust s-process predictions are necessary to disentangle the contribution from other stellar processes producing elements in the same mass region. Nuclear uncertainties are affecting s-process calculations, but most of the needed nuclear input are accessible to present nuclear experiments or they will be in the near future. Neutron-capture rates have a great impact on the s process in massive stars, which is a fundamental source for the solar abundances of the lighter s-process elements heavier than Fe (weak s-process component). In this work we present a new nuclear sensitivity study to explore the impact on the s process in massive stars of 86 neutron-capture rates, including all the reactions between C and Si and between Fe and Zr. We derive the impact of the rates at the end of the He-burning core and at the end of the C-burning shell, where the 22 Ne(α,n) 25 Mg reaction is is the main neutron source. We confirm the relevance of the light isotopes capturing neutrons in competition with the Fe seeds as a crucial feature of the s process in massive stars. For heavy isotopes we study the propagation of the neutron-capture uncertainties, finding a clear difference of the impact of Fe and Co isotope rates with respect to the rates of heavier stable isotopes. The local uncertainty propagation due to the neutron-capture rates at the s-process branching points is also considered, discussing the example of 85 Kr. The complete results of our study for all the 86 neutron-capture rates are available online. Finally, we present the impact on the weak s process of the neutron-capture rates included in the new ASTRAL library (v0.2).

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

The role of ionic blockades in controlling the efficiency of energy recovery in forward bias bipolar membranes

Limited understanding exists about the operation of bipolar membranes (BPMs) in forward bias to convert protonic gradients into electrical work, despite their emerging role in many electrochemical devices. In these device contexts, the BPM is typically exposed to complex electrolyte mixtures, but their impact on polarization remains poorly understood. Here, for this work, we develop a mechanistic model explaining the forward bias polarization behaviour of BPMs in mixed electrolytes with different acidities/basicities. This model invokes that weak acids/bases accumulate in the BPM and impose an ionic blockade that inhibits the recombination of stronger acids/bases, resulting in a substantial neutralization overpotential. We demonstrate the utility of our model for fuel cells and redox flow batteries and introduce two materials design strategies for mitigating this inhibition. Lastly, we apply our findings to enhance the energy efficiency of carbonate management in CO 2 electrolysers. This work highlights how non-equilibrium local environments at membrane–membrane interfaces can define the efficiency of protonic-to-electrical energy conversion.

25 ENERGY STORAGE↗

DOE OSTI2024

Self-organization in collisionless, high- β turbulence

The magnetohydrodynamic (MHD) equations, as a collisional fluid model that remains in local thermodynamic equilibrium (LTE), have long been used to describe turbulence in myriad space and astrophysical plasmas. Yet, the vast majority of these plasmas, from the solar wind to the intracluster medium (ICM) of galaxy clusters, are only weakly collisional at best, meaning that significant deviations from LTE are not only possible but common. Recent studies have demonstrated that the kinetic physics inherent to this weakly collisional regime can fundamentally transform the evolution of such plasmas across a wide range of scales. Here, we explore the consequences of pressure anisotropy and Larmor-scale instabilities for collisionless, β $\gg$ 1, turbulence, focusing on the role of a self-organizational effect known as ‘magneto-immutability’. We describe this self-organization analytically through a high-β, reduced ordering of the Chew–Goldberger–Low-MHD (CGL-MHD) equations, finding that it is a robust inertial-range effect that dynamically suppresses magnetic-field-strength fluctuations, anisotropic-pressure stresses and dissipation due to heat fluxes. As a result, the turbulent cascade of Alfvénic fluctuations continues below the putative viscous scale to form a robust, nearly conservative, MHD-like inertial range. These findings are confirmed numerically via Landau-fluid CGL-MHD turbulence simulations that employ a collisional closure to mimic the effects of microinstabilities. We find that microinstabilities occupy a small (~5%) volume-filling fraction of the plasma, even when the pressure anisotropy is driven strongly towards its instability thresholds. We discuss these results in the context of recent predictions for ion-vs-electron heating in low-luminosity accretion flows and observations implying suppressed viscosity in ICM turbulence.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Breaking Beams: A Kinetic Treatment of the Filamentation and Forward Scatter of Laser Beams in Plasma (Abbreviated Final Report)

Precise and predictable propagation and deposition of laser energy in high energy density (HED) plasma is threatened by the breakup of the beam into filaments. Such filaments can be deflected and sprayed but also locally intensify the light, increasing the likelihood of other problematic interactions with the plasma. Adequately modeling, anticipating, and avoiding such processes in HED experiments requires a thorough understanding of the thresholds and nonlinear saturation mechanisms, particularly for the weakly collisional, high temperature plasmas achieved at the National Ignition Facility (NIF).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Breaking Beams: A Kinetic Treatment of the Filamentation and Forward Scatter of Laser Beams in Plasma

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Constraints on the IBEX Ribbon’s Origin from Its Evolution over a Solar Cycle

Abstract In 2009, the Interstellar Boundary Explorer (IBEX) discovered a narrow “ribbon” of energetic neutral atom emissions across the sky with properties correlated with the solar wind latitudinal structure and the interstellar magnetic field draped around the heliosphere. It is widely believed that the ribbon is formed from the escape of heliospheric ENAs into the local interstellar medium and their eventual return as secondary ENAs. However, there is no consensus on the rate of pitch angle scattering of these PUIs before they become secondary ENAs. We test two opposing limits of scattering rates (“weak” versus “strong”) by solving a time-dependent model of the ribbon that evolves with the solar cycle, and we compare them to IBEX observations over 2009–2019. First, we find that both models qualitatively reproduce the evolution of IBEX fluxes for most of the data set, with a few exceptions, although the strong (or “spatial retention”) scattering model greatly underestimates the observed fluxes. Regardless, time dependence of fluxes cannot distinguish these models. Second, the ribbon’s geometric properties, i.e., its center and radius, are significantly different between the models. The spatial retention model reproduces the observed ribbon centers as a function of energy and time slightly better than the weak scattering model, and the spatial retention model reproduces the observed ribbon radius over energy and time almost perfectly, whereas the weak scattering model compares poorly. Our analysis favors the spatial retention mechanism as the source of the IBEX ribbon, but it requires modification to increase the flux of ENAs observed at 1 au.

Zirnstein, E. J. (ORCID:0000000172400618)↗

NASA NTRS1972

Analysis of inner and outer zone: OGO-1 and OGO-2 electron spectrometer and ion chamber data

The dynamic processes governing the acceleration and loss of electrons in the radiation zones are investigated. The radial diffusion coefficient was determined for a McIlwain parameter between 1.6 and 2.2 for electrons having a first adiabatic invariant of 12 MeV/gauss. The coefficient is larger than earlier values and suggests that there exists a lower limit to the fluxes in the inner zone. The agreement between observed and calculated magnetic fields and particle fluxes is improved by using solar wind pressure as input to the magnetic field models. Changes in the plasma pressure can cause apparent local time asymmetries in particle flux. A comparison of the magnetic field models with observed location of the trapping boundary also indicates the need for including distributed currents within the magnetosphere. The high latitude trapping boundary is only weakly dependent on A sub p, and the trapping boundary data are improved by including in the models a stand-off distance which varies with the plasma pressure.

Pfitzer, K. A.↗

NASA NTRS1976

Omega navigation for general aviation

A 70-hour flight test evaluation of an Omega navigation system was performed using a Piper Cherokee 180, to determine the feasibility of Omega for worldwide general aviation navigation. Measurements were made of position accuracy, noise phenomena, and signal to noise ratio. It was found that Omega accuracy is essentially insensitive to local geography, but that there are isolated local interference phenomena associated with radio transmitters, although the strongest noise source observed was due to the onboard power source for the VHF comm/nav radio. An occurrence of lane jumps was observed when attempting to navigate with one weak station.

Hollister, W. M.↗

NASA NTRS1979

Finite beta effects on the drift-cyclotron instability

The effects of finite plasma beta and strong plasma inhomogeneities on the microinstability resulting from the unstable coupling of ion-cyclotron oscillations and an ion drift wave are examined. A local electromagnetic, kinetic dispersion equation, which takes into account finite orbit modifications of both ions and electrons as well as the effects of strong inhomogeneities on the ions and permits the continuous tracking of the instability from the weak gradient regime to the strong gradient regime, is derived and solved numerically. Finite beta is shown to increase the frequency and reduce the growth rate of the instability, but not completely stabilize it due to electromagnetic effects. When plasma inhomogeneity is sufficiently strong, finite beta reduces the growth rate of the large k sub y band of a given harmonic more than the small k sub y band; however, the most unstable bands remain the same as in the case of zero beta. Implications of these results for the Tandem Mirror Experiment are discussed.

Gladd, N. T.↗

NASA NTRS1987

Absolute instability of the Gaussian wake profile

Linear parallel-flow stability theory has been used to investigate the effect of viscosity on the local absolute instability of a family of wake profiles with a Gaussian velocity distribution. The type of local instability, i.e., convective or absolute, is determined by the location of a branch-point singularity with zero group velocity of the complex dispersion relation for the instability waves. The effects of viscosity were found to be weak for values of the wake Reynolds number, based on the center-line velocity defect and the wake half-width, larger than about 400. Absolute instability occurs only for sufficiently large values of the center-line wake defect. The critical value of this parameter increases with decreasing wake Reynolds number, thereby indicating a shrinking region of absolute instability with decreasing wake Reynolds number. If backflow is not allowed, absolute instability does not occur for wake Reynolds numbers smaller than about 38.

Hultgren, Lennart S.↗

NASA NTRS1999

Bidirectional Reflectance of a Macroscopically Flat, High-Albedo Particulate Surface: An Efficient Radiative Transfer Solution and Applications to Regoliths

Many remote sensing applications rely on accurate knowledge of the bidirectional reflection function (BRF) of surfaces composed of discrete, randomly positioned scattering particles. Theoretical computations of BRFs for plane-parallel particulate layers are usually reduced to solving the radiative transfer equation (RTE) using one of existing exact or approximate techniques. Since semi-empirical approximate approaches are notorious for their low accuracy, violation of the energy conservation law, and ability to produce unphysical results, the use of numerically exact solutions of RTE has gained justified popularity. For example, the computation of BRFs for macroscopically flat particulate surfaces in many geophysical publications is based on the adding-doubling (AD) and discrete ordinate (DO) methods. A further saving of computer resources can be achieved by using a more efficient technique to solve the plane-parallel RTE than the AD and DO methods. Since many natural particulate surfaces can be well represented by the model of an optically semi-infinite, homogeneous scattering layer, one can find the BRF directly by solving the Ambartsumian's nonlinear integral equation using a simple iterative technique. In this way, the computation of the internal radiation field is avoided and the computer code becomes highly efficient and very accurate and compact. Furthermore, the BRF thus obtained fully obeys the fundamental physical laws of energy conservation and reciprocity. In this paper, we discuss numerical aspects and the computer implementation of this technique, examine the applicability of the Henyey-Greenstein phase function and the sigma-Eddington approximation in BRF and flux calculations, and describe sample applications demonstrating the potential effect of particle shape on the bidirectional reflectance of flat regolith surfaces. Although the effects of packing density and coherent backscattering are currently neglected, they can also be incorporated. The FORTRAN implementation of the technique is available on the World Wide Web, and can be applied to a wide range of remote sensing problems. BRF computations for undulated (macroscopically rough) surfaces are more complicated and often rely on time consuming Monte Carlo procedures. This approach is especially inefficient for optically thick, weakly absorbing media (e.g., snow and desert surfaces at visible wavelengths since a photon may undergo many internal scattering events before it exists the medium or is absorbed. However, undulated surfaces can often be represented as collections of locally flat tilted facets characterized by the BRF found from the traditional plane parallel RTE. In this way the MOnte Carlo procedure could be used only to evaluate the effects of surface shadowing and multiple surface reflections, thereby bypassing the time-consuming ray tracing inside the medium and providing a great savings of CPU time.

Mishchenko, Michael I.↗

NASA NTRS2010

A Meteorological Overview of the TC4 Mission

The TC4 mission in Central America during summer 2007 examined convective transport into the tropical Upper Troposphere/Lower Stratosphere (UTLS) and the evolution of cirrus clouds. The tropical tropopause layer (TTL) circulation is dominated by the Asian monsoon anticyclone and westward winds that stretch from the western Pacific into the Atlantic. During TC4, TTL westward flow over Central America was stronger than normal. Incidence of cold clouds over the Central American region was the third lowest out of 34 years sampled. The major factor was an incipient La Nina, specifically anomalously cold temperatures off the Pacific Coast of South America. Weakness in the low level Caribbean jet caused a shift in the coldest clouds from the Caribbean to the Pacific side of Central America. The character of tropopause temperature variability was that of upward propagating waves generated by local and nonlocal convection. These waves produced tropopause temperature variations of 3 K, with peak-to-peak variations of 8 K. At low levels in Central America, flow from the Sahara desert predominated; further south, the air came from the Amazon region. Convectively influenced air in the upper troposphere came from Central America, the northern Amazon region, the Atlantic ITCZ, and the North American monsoon. In the TTL, Asian and African convection affected the observed air masses. North of 10N in the Central American TTL, African and Asian convection may have contributed as much to the air masses as Central and South American convection. South of 8N, Asian and African convection had far less impact.

Pfister, L.↗

NASA NTRS2016

Magnetospheric Multiscale Observations of Magnetic Reconnection Associated with Kelvin-Helmholtz Waves

The four Magnetospheric Multiscale (MMS) spacecraft recorded the first direct evidence of reconnection exhausts associated with Kelvln-Helmholtz (KH) waves at the duskside magnetopause on 8 September 2015 which allows for local mass and energy transport across the flank magnetopause. Pressure anisotropy-weighted Walen analyses confirmed in-plane exhausts across 22 of 42 KH-related trailing magnetopause current sheets (CSs). Twenty-one jets were observed by all spacecraft, with small variations in ion velocity, along the same sunward or antisunward direction with nearly equal probability. One exhaust was only observed by the MMS-1,2 pair, while MMS-3,4 traversed a narrow CS (1.5 ion inertial length) in the vicinity of an electron diffusion region. The exhausts were locally 2-D planar in nature as MMS-1, 2 observed almost identical signatures separated along the guide-field. Asymmetric magnetic and electric Hall fields are reported in agreement with a strong guide-field and a weak plasma density asymmetry across the magnetopause CS.

Eriksson, S.↗

DOE OSTI2026

Anion-dependent phase behavior of methylimidazolium-based ionic liquids mixed with water: Correlation between local molecular structure and mesoscale behaviors

The mesoscopic phase behavior of decylmethylimidazolium (C 10 mim) ionic liquids (ILs) bearing three monovalent anions—thiocyanate (SCN − ), nitrate (NO 3 − ), and chloride (Cl − )—mixed with water at relatively high IL contents (50–95 wt%) was investigated. Small-angle and wide-angle X-ray scattering (SAXS/WAXS) were employed to follow the evolution of both local and mesoscale structures across this composition range. In the absence of water, C 10 mimSCN and C 10 mimCl behaved as disordered liquids, whereas C 10 mimNO 3 spontaneously formed a hexagonally ordered cylindrical mesophase and displayed a sticky-solid macroscopic appearance. Upon addition of water, C 10 mimSCN remained a viscous liquid and only weakly ordered lamellar domains were observed. This limited ordering is attributed to the lack of hydrogen bonding and weak interaction energy between SCN − anions and C 10 mim + cations. In contrast, the trigonal-planar NO 3 − and point-like Cl − anions promoted the formation of well-defined hexagonal mesophases up to 35–45 wt% water. The formation of hydrogen bonding of the two anions with imidazolium ring protons likely enabled the creation of compact ion clusters that effectively exclude water molecules from the immediate vicinity of the IL aggregates. These findings demonstrate that the interaction energy between ion pairs dictate IL-water interactions and therefore control the transition from disordered liquids to ordered mesophases in IL/water mixtures with high IL contents. In conclusion, the combined SAXS/WAXS analysis reveals a correlation between local intermolecular structure and the emergence of mesoscopic order, providing a systematic framework for tailoring mesoscale structures in alkylimidazolium-based IL/water systems.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Uniformity Is Key in Defining Structure–Function Relationships for Atomically Dispersed Metal Catalysts: The Case of Pt/CeO 2

Catalysts consisting of atomically dispersed Pt (Pt iso ) species on CeO 2 supports have received recent interest due to their potential for efficient metal utilization in catalytic convertors. However, discrepancies exist between the behavior (reducibility, interaction strength with adsorbates) of high surface area Pt iso /CeO 2 systems and of well-defined surface science and computational model systems, suggesting differences in Pt local coordination in the two classes of materials. Here, we reconcile these differences by demonstrating that high surface area Pt iso /CeO 2 synthesized at low Pt loadings (<0.1% weight) exhibit resistance to reduction and sintering up to 500 °C in 0.05 bar H 2 and minimal interactions with CO—properties previously seen only for model system studies. Alternatively, Pt loadings >0.1 weight % produce a distribution of sub-nanometer Pt structures, which are difficult to distinguish using common characterization techniques, and exhibit strong interactions with CO and weak resistance to sintering, even in 0.05 bar H 2 at 50 °C—properties previously seen for high surface area materials. This work demonstrates that low metal loadings can be used to selectively populate the most thermodynamically stable adsorption sites on high surface area supports with atomically dispersed metals. Further, the site uniformity afforded by this synthetic approach is critical for the development of relationships between atomic scale local coordination and functional properties. Comparisons to recent studies of Pt iso /TiO 2 suggest a general compromise between the stability of atomically dispersed metal catalysts and their ability to interact with and activate molecular species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗