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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Closures for multicomponent reacting flows based on dispersion analysis

This work presents algebraic closure models associated with advective transport and nonlinear reactions in a Reynolds-averaged Navier-Stokes context for a system of species subject to binary reactions and transport by advection and diffusion. Expanding upon analysis originally developed for non-reactive transport in the context of Taylor dispersion of scalars, this work extends the modified gradient diffusion model explicated by Peters [N. Peters, Turbulent Combustion, Cambridge Monographs on Mechanics (Cambridge University Press, Cambridge, 2000)] and based on work by Corrsin [S. Corrsin, The reactant concentration spectrum in turbulent mixing with a first-order reaction, J. Fluid Mech. 11, 407 (1961)] beyond single-component transport phenomena and involving nonlinear reactions. The presented model forms, from this weakly nonlinear extension of the original dispersion theory, lead to an analytic expression for the eddy diffusivity matrix that explicitly captures the influence of the reaction kinetics on the closure operators. Furthermore, we demonstrate that the derived model form directly translates between flow topologies through a priori and a posteriori testing of a binary species system subject to homogeneous isotropic turbulence. Using two- and three-dimensional direct numerical simulations involving laminar and turbulent flows, it is shown that this framework improves prediction of mean quantities compared to previous results. Lastly, the presented model form, collapses to the earlier gradient diffusion and its modified version derived by Corrsin in the limits of nonreactive species and linear reactions, respectively.

42 ENGINEERING↗
DOE OSTI2024

Large eddy simulation of a supersonic lifted hydrogen flame: Impacts of Lewis, turbulent Schmidt and Prandtl numbers

Parametric large eddy simulations (LES) of a supersonic lifted hydrogen flame are reported. The emphases are on two aspects: impacts of (1) Lewis number (Lei of the ith species) and (2) turbulent Schmidt and Prandtl numbers (⁠Sc t and Pr t ⁠) on supersonic turbulent flame and flow structures. Five cases are considered: species-specific Le i , Sc t = Sr t = 1.0 (C 0 ); unity Le i , Sc t = Pr t = 1.0 (C 1 ); species-specific Sc t = 0.5, Pr t = 1.0 (C 2 ); species-specific Le i , Sc t = 1.0, Pr t = 0.5 (C 3 ); and species-specific Le i , Sc t = Pr t = 0.5 (C 4 ). Numerical results of instantaneous and/or time-averaged species mole fractions, mixture fraction, heat release rate, flame base location, and mixed modes of premixed and diffusion combustion are compared between cases C 0 and C 1 . Differences in auto-ignition locations and strengths and flame structures and stabilization specify the impacts of Lewis number. They are triggered by different predictions of species mass and thermal diffusions at fuel-coflow and/or coflow-ambient air mixing layers. These differences are rationalized by a scale analysis of mass/thermal diffusion and convection for case C 0 , which suggests the relatively low but non-negligible former against the latter. Cases C 0 and C 2 –C 4 barely see differences in terms of instantaneous and/or time-averaged temperature, velocity, and mixed combustion modes except for further downstream areas where combustion occurs. Both Sc t and Pr t impose less significant influences than Lewis number, as sub-grid scale mass/thermal diffusion is subordinate to its resolved counterpart according to their scale analysis for case C 4 .

42 ENGINEERING↗
DOE OSTI2023

The kinetics of the PuO 2 to Pu 2 O 3 conversion

Here in an oxidizing environment, the oxide formed on plutonium (Pu) metal is composed of a plutonium dioxide (PuO 2 ) top layer and a thin cubic plutonium sesquioxide (Pu 2 O 3 ) middle layer. In a reducing environment, the PuO 2 layer auto-reduces to cubic Pu 2 O 3 . The speed and extent of this conversion depend on the combination of temperature and time. While PuO 2 provides a strong diffusion barrier against unwanted Pu corrosion by gaseous species (like hydrogen), Pu 2 O 3 does not, since its crystal structure has chains of oxygen vacancies. The kinetics of the PuO 2 reduction are, therefore, of fundamental interest and enable researchers to better protect Pu from corrosion. In this report, the oxygen-diffusion-limited kinetics of the dioxide to sesquioxide conversion were obtained by dynamically heating a PuO 2 -covered Pu sample from 294 to 418 K in a high-vacuum vessel equipped with an in situ spectroscopic ellipsometer. The physical/chemical constraints in the conversion process were combined with the ellipsometry method of multi-sample analysis to track the percentage of PuO 2 and to compute the extent of Pu 2 O 3 formation. The resulting diffusion coefficients were compared against and then combined with complementary literature data to produce a comprehensive set of kinetic parameters for reliably modeling oxide conversion over a larger temperature range than spanned by prior studies. The extracted thermal activation energy barrier (43.7 kJ/mol) and pre-exponential factor (5.0 × 10 -10 cm 2 /s) for the oxygen-diffusion-limited process can be used to accurately model the PuO 2 to Pu 2 O 3 transformation in vacuum and/or inert gas applications.

36 MATERIALS SCIENCE↗
NASA NTRS2002

Angular Distributions of Fe/O From Wind: New Insight Into SEP Transport

We examine the angular distributions of He, O, and Fe in large solar energetic particle (SEP) events measured on the Wind spacecraft. We report for the first time, that in a fixed velocity interval, Fe/O is often larger for particles flowing sunward along the magnetic field than for particles flowing outward from the Sun in many SEP events. This occurs because the anisotropy for O exceeds that for Fe, even though both species are streaming outward. There are no examples of events for which the outward Fe/O dominates. The behavior of Fe and O conflicts with the expectations of simple diffusion theory, that angular distributions should be independent of species. It also seems to conflict with the idea that energetic Fe scatters less than O of the same velocity. However, preliminary modeling suggests that the presence of a reflecting magnetic boundary beyond 1 AU, together with the increased scattering of O over Fe due to proton generated Alfven waves, can explain the direction and magnitude of the effect. These observations add a new dimension to the study of SEP transport.

Reames, D. V.↗
DOE OSTI2020

Online ion mobility spectrometry of nanoparticle formation by non-thermal plasma conversion of metal salts in liquid aerosol droplets

The synthesis of nanoparticles by reaction of liquid aerosol droplets containing precursors in a flow-through, atmospheric-pressure, non-thermal plasma offers a continuous, scalable, substrate- and stabilizer-free approach for direct deposition into liquids or onto soft substrates. However, the combination of multiphase and non-equilibrium chemistry makes the process complicated and poorly understood. Here, we present ion mobility spectrometry measurements of liquid water droplets containing silver nitrate passing through an atmospheric-pressure dielectric barrier discharge reactor that allows us to monitor silver nanoparticle formation online for the first time. Mobility diameter distributions were obtained with the plasma on and off, and exhibited a shift, which was related to the degree of conversion of silver nitrate. The silver nanoparticles were also collected and characterized by UV–visible absorbance spectroscopy and transmission electron microscopy to support the online measurements. Importantly, negligible conversion was found when the water was removed by a diffusion dryer, suggesting that the key reducing species are in the liquid phase, such as solvated electrons. Finally, the study demonstrates how ion mobility spectrometry measurements can be applied to provide insight into this approach to nanoparticle synthesis.

42 ENGINEERING↗
DOE OSTI2023

Coherences of Photoinduced Electron Spin Qubit Pair States in Photosystem I

Here, this publication presents the first comprehensive experimental study of electron spin coherences in photosynthetic reaction center proteins, specifically focusing on photosystem I (PSI). The ultrafast electron transfer in PSI generates spin-correlated radical pairs (SCRPs), which are entangled spin pairs formed in well-defined spin states (Bell states). Since their discovery in our group in the 1980s, SCRPs have been extensively used to enhance our understanding of structure–function relationships in photosynthetic proteins. More recently, SCRPs have been utilized as tools for quantum sensing. Electron spin decoherence poses a significant challenge in realizing practical applications of electron spin qubits, particularly the creation of quantum entanglement between multiple electron spins. This work is focused on the systematic characterization of decoherence in SCRPs of PSI. These decoherence times were measured as electron spin echo decay times, termed phase memory times (T M ), at various temperatures. Decoherence was recorded on both transient SCRP states P 700 + A 1 – and thermalized states. Our study reveals that T M exhibits minimal dependence on the biological species, biochemical treatment, and paramagnetic species. The analysis indicates that nuclear spin diffusion and instantaneous diffusion mechanisms alone cannot explain the observed decoherence. As a plausible explanation we discuss the assumption that the low-temperature dynamics of methyl groups in the protein surrounding the unpaired electron spin centers is the main factor governing the loss of the spin coherence in PSI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Highly Efficient Proton Conduction in the Metal–Organic Framework Material MFM-300(Cr)·SO 4 (H 3 O) 2

The development of materials showing rapid proton conduction with a low activation energy and stable performance over a wide temperature range is an important and challenging line of research. Here, we report confinement of sulfuric acid within porous MFM-300(Cr) to give MFM-300(Cr)·SO 4 (H 3 O) 2 , which exhibits a record-low activation energy of 0.04 eV, resulting in stable proton conductivity between 25 and 80 °C of >10 –2 S cm –1 . In situ synchrotron X-ray powder diffraction (SXPD), neutron powder diffraction (NPD), quasielastic neutron scattering (QENS), and molecular dynamics (MD) simulation reveal the pathways of proton transport and the molecular mechanism of proton diffusion within the pores. Confined sulfuric acid species together with adsorbed water molecules play a critical role in promoting the proton transfer through this robust network to afford a material in which proton conductivity is almost temperature-independent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Room temperature buffer gas beam of metastable state titanium atoms

We produce beams of neutral titanium (Ti) atoms in their metastable 3d3(F4)4sa5F5 state by laser ablation into He, N2, and Ar buffer gases. The high temperatures associated with the ablation process populate the a5F5 level without the need for optical pumping. Remarkably, we observe that Ti atoms in the a5F5 state survive thousands of collisions with He and Ar buffer gas atoms without being quenched to lower-energy states. We study the yield of Ti atoms when ablated into buffer gases of varying species and pressure, quantify quenching rates and diffusion cross sections based on simple models, and provide insight into optimal design parameters for an ablation cell. Using a 3.3 cm ablation cell with interchangeable exit apertures, we produce metastable atom beams and quantify their brilliance and velocity distributions as functions of buffer gas pressure.

Schrott, Jackson↗
DOE OSTI2023

Reactive high-spin iron(IV)-oxo sites through dioxygen activation in a metal–organic framework

In nature, nonheme iron enzymes use dioxygen to generate high-spin iron(IV)=O species for a variety of oxygenation reactions. Although synthetic chemists have long sought to mimic this reactivity, the enzyme-like activation of O 2 to form high-spin iron(IV) = O species remains an unrealized goal. Here, we report a metal–organic framework featuring iron(II) sites with a local structure similar to that in α-ketoglutarate-dependent dioxygenases. The framework reacts with O 2 at low temperatures to form high-spin iron(IV) = O species that are characterized using in situ diffuse reflectance infrared Fourier transform, in situ and variable-field Mössbauer, Fe Kβ x-ray emission, and nuclear resonance vibrational spectroscopies. In the presence of O 2 , the framework is competent for catalytic oxygenation of cyclohexane and the stoichiometric conversion of ethane to ethanol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1979

Latitudinal distribution of the sources of carbon monoxide in the troposphere

A vertically and zonally averaged model of the troposphere has been constructed which calculates photochemical interactions and diffusive North-South transport of trace species. The model can be used to calculate the latitudinal distribution of the source function of a species if its concentration distribution is known. This procedure has been applied to carbon monoxide and large sources have been found outside the industrialized belt in the Northern Hemisphere.

Hameed, S.↗
NASA NTRS1981

Transport properties associated with entry into the atmosphere of Titan

In this paper the transport properties in the atmosphere of Titan and at the shock front and the probe surface for non-ablative entry into Titan's atmosphere are calculated, using the kinetic theory of gases. The species N2, H2, CH4, HCN, N, and H contribute to the transport properties under these conditions. The transport properties were calculated by using accurate potential energy curves for each of the thirteen two-body interactions which occur between these species. Results are given for the binary diffusion coefficients, the non-reactive and reactive thermal conductivity, and the viscosity from 1000 K to 8000 K. This information is needed for calculating flowfield properties and surface heating rates. The most important conclusions are that the non-reactive thermal conductivity is much larger behind the shock layer than it is in the ambient atmosphere and that the nonreactive thermal conductivity appears to be nearly constant in the shock layer.

Flori, B.↗
NASA NTRS1984

Use of the Burton-prim-slichter Equation at High Growth Rates

The following must be assumed in order to derive the classic Burton-Prim-Slichter equation for segregation during crystal growth: isobaric, isothermal, isopotential or uncharged species, binary, planar interface, steady state, constant diffusion coefficient in fluid, no diffusion in crystal, no lateral convection within fluid film at interface with complete mixing beyond (stagnant film model), and either density, total concentration or partial molar volumes constant in the fluid phase. In addition, the effective distribution coefficient and the interfacial distribution coefficient must be defined properly. The velocity in the equation is the growth rate times a factor correcting for the difference in volumetric properties between crystal and fluid. The stagnant film thickness is found to be a function of freezing rate, with the precise functionality depending on the type of stirring occurring in the growth fluid.

Wilcox, W. R.↗
NASA NTRS1987

Facilitation of the growth of protein crystals by heterogeneous/epitaxial nucleation

A preliminary exploration has been made of the effect of inorganic crystals on the nucleation of protein crystals. Four representative proteins were crystallized by the vapor diffusion technique in the presence of fifty species of inorganic crystals. A substantial decrease in critical supersaturation was caused by thirty nucleants for canavalin and by seven to fifteen nucleants for the other proteins. Several cases of anomalous morphology were observed, as well as one instance of epitaxy, i.e., lysozyme on apophyllite. It has thus been shown that inorganic crystals can be used as heterogeneous nuclei or epitaxial substrates for facilitating reliable and controlled nucleation in automated protein crystal growth experiments.

Mcpherson, Alexander↗
NASA NTRS1990

A two-component volatile atmosphere for Pluto. I - The bulk hydrodynamic escape regime

The seasonal effects on Pluto's atmosphere of a simplified system of CH4 and N2 saturated over a solid solution are investigated, and the results are compared with previous CH4 models. It is found that bulk escape occurs for CH4 mole fractions less than 0.7 of Pluto's volatile reservoir. Greater CH4 abundance leads to diffusive separation during the escape of both species and an atmospheric mixing ratio of about Xc(0). If Xc(0) is in the range 0.02-0.10, Pluto's atmosphere remains largely intact at aphelion rather than virtually freezing out as it does for Xc(0) greater than 0.3 or less than 0.001, or form an atmosphere with only a single volatile gas. An upper limit for the CH4 mixing ratio is about 0.07 if N2 is the second gas. On the other hand, CH4 is the dominant surface constituent of the volatile deposit if Xc(0) is greater than 0.0001.

Trafton, L.↗
NASA NTRS1991

MOCVD of GaAs in a horizontal reactor - Modeling and growth

A two-dimensional model for metalorganic chemical vapor deposition of GaAs in a horizontal reactor is presented. The model is characterized by the following parameters: reactor geometry and operating pressure, thermal boundary conditions, ratio of reactants, chemical reactions, total inlet gas flow rate, as well as molecular weights, thermal conductivities, heat capacities, viscosities, and binary diffusion coefficients of the gas-phase species. Film thickness profiles predicted by the model are compared with those of GaAs thin films grown in the modeled reactor. Results obtained show a good agreement between the predictions and data over the entire length of the deposition region for the low pressure and high flow rate run. Attention is also given to the reactor design and growth conditions.

Clark, Ivan O.↗
NASA NTRS1993

A model for heterogeneous chemical processes on the surfaces of ice and nitric acid trihydrate particles

The study presents a model that incorporates the physics and physical chemistry of ice surfaces relevant to polar stratospheric clouds. Surface concentrations of H2O, HCl, HOCl, ClONO2, and N2O5 on ice and nitric acid trihydrate (NAT) crystals are computed, and surface reaction rates and reaction probabilities (sticking coefficients) are determined. For gas pressures of about 10 exp -7 torr and temperatures in the range of 180-200 K, HCl completely coats ice and water-rich NAT surfaces, while HOCl, ClOHO2, and N2O5 may cover 0.01-1 percent of these surfaces. The energy parameters are used to calculate surface temperatures such as adsorption and desorption constants, surface coverages, reaction rate coefficients, surface diffusion coefficients, and reaction probabilities for various species and chemical interactions on ice and NAT surfaces. Implications for chemical processing on polar stratospheric clouds are discussed.

Tabazadeh, Azadeh↗
NASA NTRS1997

Characteristics of Non-Premixed Turbulent Flames in Microgravity

The overall objectives of this research are: (1) to obtain and analyze experimental data on flame images, and the spatial and temporal distributions of temperature, radiation, velocity and gas-phase species in microgravity turbulent gas-jet diffusion flames; and (2) to utilize these data to validate and refine the existing predictive capabilities. Work on this project commenced in June 1996. The first investigations on turbulent gas-jet diffusion flames in microgravity were initiated by Bahadori and co-workers in 1991. These studies have shown that significant differences exist in the transition processes in normal-gravity and microgravity flames, and that the turbulent flames in microgravity behave very differently as compared to their buoyancy-dominated normal-gravity counterparts. For example, in the transition regime while the visible flame height, for given fuel and nozzle size, in normal gravity decreases, the height of the microgravity flame increases. In the fully developed turbulent regime, the normal-gravity flame height is independent of injection velocity, whereas the microgravity flame height continues to increase, although at a lower rate than in the laminar and transitional regimes. Other differences between the normal-gravity and microgravity flames arise in the jet shear-layer instability characteristics, extent of the transitional regime and blow-off limit characteristics.

Hegde, Uday↗
DOE OSTI2020

Multi-scale model based design of membrane reactor/separator processes for intensified hydrogen production through the water gas shift reaction

This paper aims to first quantify the impact of various diffusion models (Maxwell-Stefan, Wilke, Dusty-Gas) on the predictions of a multi-scale membrane reactor/separator mathematical model, and to then demonstrate this model's use for the design and process intensification of membrane reactor/separator systems for hydrogen production. This multi-scale model captures velocity, temperature and species' concentration profiles along the catalyst pellet's radial direction, and along the reactor's axial direction, by solving the momentum, energy, and species transport equations, accounting for convection, conduction, reaction, and diffusion mechanisms. In the first part of work, the effect of pellet-scale design parameters (mean pore diameter, volumetric porosity, tortuosity factor, etc.) and various species' flux models on the model predictions is studied. In the second part, the study focuses on the comparison, in terms of their process intensification characteristics, of various hydrogen production processes. These include a conventional high-temperature shift reactor (HTSR)/low-temperature shift reactor (LTSR) sequence, a novel HTSR/membrane separator (MS)/LTSR/MS sequence, and a process that involves low-temperature shift membrane reactors-LTSMR in a series.

08 HYDROGEN↗