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All sources NASA NTRS DOE OSTI

DOE OSTI2020

Diffusion and migration in polymer electrolytes

Mixtures of neutral polymers and lithium salts have the potential to serve as electrolytes in next-generation rechargeable Li-ion batteries. The purpose of this review is to expose the delicate interplay between polymer-salt interactions at the segmental level and macroscopic ion transport at the battery level. Since complete characterization of this interplay has only been completed in one system: mixtures of poly(ethylene oxide) and lithium bis(trifluoromethanesulfonyl)imide (PEO/LiTFSI), we focus on data obtained from this system. We begin with a discussion of the activity coefficient, followed by a discussion of six different diffusion coefficients: the Rouse motion of polymer segments is quantified by D seg , the self-diffusion of cations and anions is quantified by D self,+ and D self,- , and the build-up of concentration gradients in electrolytes under an applied potential is quantified by Stefan-Maxwell diffusion coefficients, D 0+ , D 0- , and D +- . The Stefan-Maxwell diffusion coefficients can be used to predict the velocities of the ions at very early times after an electric field is applied across the electrolyte. The surprising result is that D 0- is negative in certain concentration windows. A consequence of this finding is that at these concentrations, both cations and anions are predicted to migrate toward the positive electrode at early times. We describe the controversies that surround this result. Knowledge of the Stefan-Maxwell diffusion coefficients enable prediction of the limiting current. We argue that the limiting current is the most important characteristic of an electrolyte. Excellent agreement between theoretical and experimental limiting current is seen in PEO/LiTFSI mixtures. What sequence of monomers that, when polymerized, will lead to the highest limiting current remains an important unanswered question. It is our hope that the approach presented in this review will guide the development of such polymers.

25 ENERGY STORAGE↗

DOE OSTI2020

Efficient lasing in mixtures of helium and fluorine in diffuse discharges formed by runaway electrons

The parameters of stimulated lasing in diffuse discharges formed in mixtures of helium and fluorine in a strongly inhomogeneous electric field are investigated. Lasing is obtained in the visible and VUV spectral regions on the transitions of fluorine atoms and molecules. It is shown that lasing in He – F{sub 2} mixtures at a wavelength of 157 nm continues for several half-periods of the discharge current. Due to the homogeneity of the diffuse discharge, the maximum lasing efficiency of the F{sub 2} laser is 0.15 %, which corresponds to the efficiency of this type of lasers pumped by pre-ionised transverse volume discharges. (paper)

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Correcting Magnetic-Field Diffusion Effects in Beam Position Monitors

Beam position monitors (BPMs) provide timeresolved measurements of the current and centroid position of high-current electron beams in linear induction accelerators (LIAs). The data from some types of BPMs can be influenced by magnetic field diffusion into the surrounding metal. We derive an estimate of the correction factor from first principles, and show how it is applied in practice to nearly eliminate the effect from the data.

43 PARTICLE ACCELERATORS↗

NASA NTRS1995

Diffusion lengths in irradiated N/P InP-on-Si solar cells

Indium phosphide (InP) solar cells are being made on silicon (Si) wafers (InP/Si) to take advantage of both the radiation-hardness properties of the InP solar cell and the light weight and low cost of Si wafers compared to InP or germanium (Ge) wafers. The InP/Si cell application is for long duration and/or high radiation orbit space missions. InP/Si cells have higher absolute efficiency after a high radiation dose than gallium arsenide (GaAs) or silicon (Si) solar cells. In this work, base electron diffusion lengths in the N/P cell are extracted from measured AM0 short-circuit photocurrent at various irradiation levels out to an equivalent 1 MeV fluence of 1017 1 MeV electrons/sq cm for a 1 sq cm 12% BOL InP/Si cell. These values are then checked for consistency by comparing measured Voc data with a theoretical Voc model that includes a dark current term that depends on the extracted diffusion lengths.

Wojtczuk, Steven↗

DOE OSTI2021

Using Computationally-Determined Properties for Machine Learning Prediction of Self-Diffusion Coefficients in Pure Liquids

The ability to predict transport properties of liquids quickly and accurately will greatly improve our understanding of fluid properties both in bulk and complex mixtures, as well as in confined environments. Such information could then be used in the design of materials and processes for applications ranging from energy production and storage to manufacturing processes. As a first step, we consider the use of machine learning (ML) methods to predict the diffusion properties of pure liquids. Recent results have shown that Artificial Neural Networks (ANNs) can effectively predict the diffusion of pure compounds based on the use of experimental properties as the model inputs. In the current study, a similar ANN approach is applied to modeling diffusion of pure liquids using fluid properties obtained exclusively from molecular simulations. A diverse set of 102 pure liquids is considered, ranging from small polar molecules (e.g., water) to large nonpolar molecules (e.g., octane). Self-diffusion coefficients were obtained from classical molecular dynamics (MD) simulations. Since nearly all the molecules are organic compounds, a general set of force field parameters for organic molecules was used. The MD methods are validated by comparing physical and thermodynamic properties with experiment. Computational input features for the ANN include physical properties obtained from the MD simulations as well as molecular properties from quantum calculations of individual molecules. Furthermore, fluid properties describing the local liquid structure were obtained from center of mass radial distribution functions (COM-RDFs). Feature sensitivity analysis revealed that isothermal compressibility, heat of vaporization, and the thermal expansion coefficient were the most impactful properties used as input for the ANN model to predict the MD simulated self-diffusion coefficients. The MD-based ANN successfully predicts the MD self-diffusion coefficients with only a subset (2 to 3) of the available computationally determined input features required. A separate ANN model was developed using literature experimental self-diffusion coefficients as model targets. Although this second ML model was not as successful due to a limited number of data points, a good correlation is still observed between experimental and ML predicted self-diffusion coefficients.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Alcove formation in dissolving cliffs driven by density inversion instability

We demonstrate conditions that give rise to cave-like features commonly found in dissolving cliffsides with a minimal two-phase physical model. Alcoves that are wider at the top and tapered at the bottom, with sharp-edged ceilings and sloping floors, are shown to develop on vertical solid surfaces dissolving in aqueous solvents. As evident from descending plumes, sufficiently large indentations evolve into alcoves as a result of the faster dissolution of the ceiling due to a solutal Rayleigh–Bénard density inversion instability. In contrast, defects of size below the boundary layer thickness set by the critical Rayleigh number smooth out, leading to stable planar interfaces. Furthermore, the ceiling recession rate and the alcove opening area evolution are shown to be given to first-order by the critical Rayleigh number. By tracking passive tracers in the fluid phase, we show that the alcoves are shaped by the detachment of the boundary layer flow and the appearance of a pinned vortex at the leading edge of the indentations. The attached boundary layer past the developing alcove is then found to lead to rounding of the other sides and the gradual sloping of the floor.

58 GEOSCIENCES↗

DOE OSTI2020

The Effect of Proton Conductivity of Fe–N–C–Based Cathode on PEM Fuel cell Performance

A model–based impedance spectroscopy is used to determine proton conductivity, oxygen transport parameter, double layer capacitance and oxygen reduction reaction (ORR) Tafel slope in the Fe–N–C cathode catalyst layer (CCL) of a PEM fuel cell. Experimental spectra of two cells differing by the membrane thickness only are processed using a physics–based model for PEMFC impedance. The spectra have been measured in the range of current densities from 25 to 800 mA cm -2 . The ORR Tafel slope of both the cells shows almost linear growth with the current density. In one of the cells, the CCL proton conductivity σp strongly decays at the current density of 100 mA cm -2 ; this decay is accompanied by the step growth of the double layer capacitance. Other minor variations of proton conductivity and double layer capacitance with the cell current occur also in a counterphase; presumed origin of this effect is discussed. The oxygen diffusion coefficient in the cathode exhibits explosive growth with the cell current. We attribute this effect to formation of temperature and pressure gradients in the CCL due to strongly non–uniform distribution of ORR rate in the electrode.

25 ENERGY STORAGE↗

NASA NTRS1992

Kinetics of intercalation of lithium into NbSe3 and TiS2 cathodes

Titanium disulfide and niobium triselenide are two well-studied candidate materials for positive electrodes in rechargeable lithium cells. A comparative study of the kinetics of intercalation of lithium in both the cathodes is made here based on various electrochemical techniques, i.e., linear polarization, potentiodynamic polarization, and ac impedance under different experimental conditions such as prismatic or disk configuration of fresh, partially discharged, or cycled electrode. Further, the diffusion coefficients of lithium ions in these cathodes are estimated under these conditions using conventional techniques, i.e., ac impedance, chronocoulometry, chronoamperometry, and current pulse relaxation. Based on the values of the diffusion coefficients, the applicability of these methods for the determination of diffusion coefficients is discussed.

Ratnakumar, B. V.↗

NASA NTRS2001

Experimental and Computational Study of Trapped Vortex Combustor Sector Rig with Tri-pass Diffuser

The Trapped Vortex Combustor (TVC) potentially offers numerous operational advantages over current production gas turbine engine combustors. These include lower weight, lower pollutant emissions, effective flame stabilization, high combustion efficiency, excellent high altitude relight capability, and operation in the lean burn or RQL (Rich burn/Quick mix/Lean burn) modes of combustion. The present work describes the operational principles of the TVC, and provides detailed performance data on a configuration featuring a tri-pass diffusion system. Performance data include EINOx (NO(sub x) emission index) results for various fuel-air ratios and combustor residence times, combustion efficiency as a function of combustor residence time, and combustor lean blow-out (LBO) performance. Computational fluid dynamics (CFD) simulations using liquid spray droplet evaporation and combustion modeling are performed and related to flow structures observed in photographs of the combustor. The CFD results are used to understand the aerodynamics and combustion features under different fueling conditions. Performance data acquired to date are favorable in comparison to conventional gas turbine combustors. Further testing over a wider range of fuel-air ratios, fuel flow splits, and pressure ratios is in progress to explore the TVC performance. In addition, alternate configurations for the upstream pressure feed, including bi-pass diffusion schemes, as well as variations on the fuel injection patterns, are currently in test and evaluation phases.

Hendricks, Robert C.↗

NASA NTRS1987

Diffuse and specular characteristics of leaf reflectance

In this paper, the evolution of current understanding of the mechanisms of leaf reflectance is reviewed. The use of measurements of polarized reflectance to separate leaf reflectance into diffuse and specular components is discussed. A section on the factors influencing leaf reflectance - leaf structure and physiological disturbances - is included along with discussion on the manner in which these influences are manifested.

Grant, Lois↗

NASA NTRS2009

The Chandra M10l Megasecond: Diffuse Emission

Because MIOl is nearly face-on, it provides an excellent laboratory in which to study the distribution of X-ray emitting gas in a typical late-type spiral galaxy. We obtained a Chandra observation with a cumulative exposure of roughly 1 Ms to study the diffuse X-ray emission in MlOl. The bulk of the X-ray emission is correlated with the star formation traced by the FUV emission. The global FUV/Xray correlation is non-linear (the X-ray surface brightness is roughly proportional to the square root of the FUV surface brightness) and the small-scale correlation is poor, probably due to the delay between the FUV emission and the X-ray production ill star-forming regions. The X-ray emission contains only minor contributions from unresolved stars (approximates less than 3%), unresolved X-ray point sources (approximates less than 4%), and individual supernova remnants (approximates 3%). The global spectrum of the diffuse emission can be reasonably well fitted with a three component thermal model, but the fitted temperatures are not unique; many distributions of emission measure can produce the same temperatures when observed with the current CCD energy resolution. The spectrum of the diffuse emission depends on the environment; regions with higher X-ray surface brightnesses have relatively stronger hard components, but there is no significant evidence that the temperatures of the emitting components increase with surface brightness.

Kuntz, K. D.↗

NASA NTRS1991

A technique to measure the thermal diffusivity of high Tc superconductors

High T(sub c) superconducting electrical current leads and ground straps will be used in cryogenic coolers in future NASA Goddard Space Flight Center missions. These superconducting samples are long, thin leads with a typical diameter of two millimeters. A longitudinal method is developed to measure the thermal diffusivity of candidate materials for this application. This technique uses a peltier junction to supply an oscillatory heat wave into one end of a sample and will use low mass thermocouples to follow the heat wave along the sample. The thermal diffusivity is calculated using both the exponential decay of the heat wave and the phase shift to the wave. Measurements are performed in a cryostat between 10 K and room temperature.

Powers, Charles E.↗

NASA NTRS1981

Application of aerial photography to the study of small scale upper ocean phenomena

The industrial waste dumped 180 n. miles south of Galveston was monitored in July 1977 by water sampling, hydrographic measurements, acoustic tracking on board two vessels, and by aerial photography. The plume of the waste diffused vertically and horizontally. Photodensitometry of aerial photos of the plume showed lateral dispersion of the plume in agreement with two other methods: acoustic tracking of the waste suspensoid and transmissometer sampling. In addition, the method showed small scale features like the lateral and longitudinal variations in the photodensity, indicating the waste concentration. This waste concentration showed periodic changes in its axial distance, with the spectral peak at about 160 m wave length. It shows a sharp increase at the windward edge of the plume as do the acoustic records. This phenomenon is explained in terms of the shearing current near the surface together with vertical diffusion. The periodic change along the axis is explained in terms of the Langmuir circulation and in terms of internal ship waves.

Ichiye, T.↗

NASA NTRS2006

Hybrid MD-Nernst Planck Model of Alpha-hemolysin Conductance Properties

Motivated by experiments in which an applied electric field translocates polynucleotides through an alpha-hemolysin protein channel causing ionic current transient blockade, a hybrid simulation model is proposed to predict the conductance properties of the open channel. Time scales corresponding to ion permeation processes are reached using the Poisson-Nemst-Planck (PNP) electro-diffusion model in which both solvent and local ion concentrations are represented as a continuum. The diffusion coefficients of the ions (K(+) and Cl(-)) input in the PNP model are, however, calculated from all-atom molecular dynamics (MD). In the MD simulations, a reduced representation of the channel is used. The channel is solvated in a 1 M KCI solution, and an external electric field is applied. The pore specific diffusion coefficients for both ionic species are reduced 5-7 times in comparison to bulk values. Significant statistical variations (17-45%) of the pore-ions diffusivities are observed. Within the statistics, the ionic diffusivities remain invariable for a range of external applied voltages between 30 and 240mV. In the 2D-PNP calculations, the pore stem is approximated by a smooth cylinder of radius approx. 9A with two constriction blocks where the radius is reduced to approx. 6A. The electrostatic potential includes the contribution from the atomistic charges. The MD-PNP model shows that the atomic charges are responsible for the rectifying behaviour and for the slight anion selectivity of the a-hemolysin pore. Independent of the hierarchy between the anion and cation diffusivities, the anionic contribution to the total ionic current will dominate. The predictions of the MD-PNP model are in good agreement with experimental data and give confidence in the present approach of bridging time scales by combining a microscopic and macroscopic model.

Cozmuta, Ioana↗

NASA NTRS1992

The faint galaxy contribution to the diffuse extragalactic background light

Models of the faint galaxy contribution to the diffuse extragalactic background light are presented, which are consistent with current data on faint galaxy number counts and redshifts. The autocorrelation function of surface brightness fluctuations in the extragalactic diffuse light is predicted, and the way in which these predictions depend on the cosmological model and assumptions of biasing is determined. It is confirmed that the recent deep infrared number counts are most compatible with a high density universe (Omega-0 is approximately equal to 1) and that the steep blue counts then require an extra population of rapidly evolving blue galaxies. The faintest presently detectable galaxies produce an interesting contribution to the extragalactic diffuse light, and still fainter galaxies may also produce a significant contribution. These faint galaxies still only produce a small fraction of the total optical diffuse background light, but on scales of a few arcminutes to a few degrees, they produce a substantial fraction of the fluctuations in the diffuse light.

Cole, Shaun↗

DOE OSTI2022

Electrodeposited Sn–Cu@Sn dendrites for selective electrochemical CO 2 reduction to formic acid

Large-scale CO 2 electrolysis can be applied to store renewable energy in chemicals. Recent developments in gas diffusion electrodes now enable a commercially relevant current density. However, the low selectivity of the CO 2 reduction reaction (CO 2 RR) still hinders practical applications. The selectivity of the CO 2 RR highly depends on the electrocatalyst. Sn catalysts are considered promising cathode materials for the production of formic acid. The selectivity of Sn catalysts can be regulated by controlling their morphology or alloying them with secondary metals. In this work, we enhanced the selectivity of CO 2 reduction to formic acid by synthesizing Sn–Cu@Sn dendrites that have a core@shell architecture. The Sn–Cu@Sn dendrites were prepared by a scalable electro-deposition method. The electronic structure was modified to suppress a reaction pathway for CO production on the Sn surface. Notably, the Sn shell inhibited the cathodic corrosion of Cu during the CO 2 RR. On a gas diffusion electrode, the Sn–Cu@Sn dendrites exhibited 84.2% faraday efficiency to formic acid for 120 h with high stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1991

A comparative study of p(+)n and n(+)p InP solar cells made by a closed ampoule diffusion

The purpose was to demonstrate the possibility of fabricating thermally diffused p(+)n InP solar cells having high open-circuit voltage without sacrificing the short circuit current. The p(+)n junctions were formed by closed-ampoule diffusion of Cd through a 3 to 5 nm thick anodic or chemical phosphorus-rich oxide cap layer grown on n-InP:S Czochralski LEC grown substrates. For solar cells made by thermal diffusion the p(+)n configuration is expected to have a higher efficiency than the n(+)p configuration. It is predicted that the AM0, BOL efficiencies approaching 19 percent should be readily achieved providing that good ohmic front contacts could be realized on the p(+) emitters of thickness lower than 1 micron.

Faur, M.↗

NASA NTRS1976

An investigation of impurity redistribution in diffused layer on /n+/-p silicon solar cells parameters

Recent calculations by Wang et al. (1974) have shown that the short-circuit current for silicon solar cells is sensitive to the impurity distribution in the diffused and base region. In the present work, these theoretical results were verified by experimentally investigating the impurity profile and sheet resistance of the diffused layers of (n+)-p silicon solar cells fabricated by normal diffusion processes and at subsequently various drive-in times. Impurity profiles of the n+ diffused layer, measured by differential Hall and resistivity technique, resemble the erfc distribution. The junction depth is larger as drive-in time increases. Measured short-circuit current is in agreement with calculated ones. Open-circuit voltage is independent of drive-in times, and its calculated values are consistent with capacitance-voltage measurements.

Wang, E. Y.↗