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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 1,045 records · Page 58
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

How good are polarizable and flexible models for water: Insights from a many-body perspective

We present a systematic analysis of state-of-the-art polarizable and flexible water models from a many-body perspective, with a specific focus on their ability to represent the Born–Oppenheimer potential energy surface of water from the gas to the liquid phase. Using coupled cluster data in the completed basis set limit as a reference, we examine the accuracy of the polarizable models in reproducing individual many-body contributions to interaction energies and harmonic frequencies of water clusters and compare their performance with that of MB-pol, an explicit many-body model that has been shown to correctly predict the properties of water across the entire phase diagram. Based on these comparisons, we use MB-pol as a reference to analyze the ability of the polarizable models to reproduce the energy landscape of liquid water under ambient conditions. We find that, while correctly reproducing the energetics of minimum-energy structures, the polarizable models examined in this study suffer from inadequate representations of many-body effects for distorted configurations. To investigate the role played by geometry-dependent representations of 1-body charge distributions in reproducing coupled cluster data for both interaction and many-body energies, we introduce a simplified version of MB-pol that adopts fixed atomic charges and demonstrate that the new model retains the same accuracy as the original MB-pol model. Based on the analyses presented in this study, we believe that future developments of both polarizable and explicit many-body models should continue in parallel and would benefit from synergistic efforts aimed at integrating the best aspects of the two theoretical/computational frameworks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

Abstract Interfacially confined microenvironments have recently gained attention in catalysis, as they can be used to modulate reaction chemistry. The emergence of a 2D nanospace at the interface between a 2D material and its support can promote varying kinetic and energetic schemes based on molecular level confinement effects imposed in this reduced volume. We report on the use of a 2D oxide cover, bilayer silica, on catalytically active Pd(111) undergoing the CO oxidation reaction. We “uncover” mechanistic insights about the structure–activity relationship with and without a 2D silica overlayer using in situ IR and X‐ray spectroscopy and mass spectrometry methods. We find that the CO oxidation reaction on Pd(111) benefits from confinement effects imposed on surface adsorbates under 2D silica. This interaction results in a lower and more dispersed coverage of CO adsorbates with restricted CO adsorption geometries, which promote oxygen adsorption and lay the foundation for the formation of a reactive surface oxide that produces higher CO 2 formation rates than Pd alone.

Eads, Calley N.↗
NASA NTRS1986

Hot ions observed by the Giotto ion mass spectrometer inside the Comet Halley contact surface

Just inside the contact surface (approx. 4700 km) the High Energy Range Spectrometer (HERS) sensor of the Giotto ion mass spectrometer detected a sudden, intense burst of ions that lasted until the HERS sensor ceased transmitting data at a distance 3000 km from comet Halley. During this interval ions with M/Q=1, 2, 12, 14, 16, 19, 24 and 28 were observed. The heavier ions appear in two populations (in the S/C frame): a very low energy, almost omnidirectional distribution, and a more energetic (approx. < ram speed) population coming from the ram direction. The low energy ions may belong to the natural Halley environment or be generated at the spacecraft by dust and gas bombardment. The ions may also be related to spacecraft charging processes on Giotto.

Goldstein, R.↗
DOE OSTI2024

Energetic and Spectroscopic Properties of Astrophysically Relevant MgC 4 H Radicals Using High-Level Ab Initio Calculations

Considering the importance of magnesium-bearing hydrocarbon molecules (MgC n H; n = 2, 4, and 6) in the carbon-rich circumstellar envelopes (e.g., IRC+10216), a total of 28 constitutional isomers of MgC 4 H have been theoretically investigated using density functional theory (DFT) and coupled-cluster methods. The zero-point vibrational energy corrected relative energies at the ROCCSD(T)/cc-pCVTZ level of theory reveal that the linear isomer, 1-magnesapent-2,4-diyn-1-yl (1, 2 Σ + ), is the global minimum geometry on the MgC 4 H potential energy surface. The latter has been detected both in the laboratory and in the evolved carbon star, IRC+10216. The calculated spectroscopic data for 1 match well with the experimental observations (error ~ 0.78%) which validates our theoretical methodology. Plausible isomerization processes happening among different isomers are examined using DFT and coupled-cluster methods. CASPT2 calculations have been performed for a few isomers exhibiting multireference characteristics. The second most stable isomer, 1-ethynyl-1λ 3 -magnesacycloprop-2-ene-2,3-diyl (2, 2 A 1 , μ = 2.54 D), is 146 kJ mol –1 higher in energy than 1 and possibly the next promising candidate to be detected in the laboratory or in the interstellar medium in future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Ab Initio Dynamics of Graphene and Graphyne Electrodes in Vacuum and in the Presence of Electrolytes

Graphene and graphyne electrodes are both relevant for electrochemical energy storage applications due to their unique physical, chemical, and electronic properties. Graphyne has been considered even more attractive than graphene due to its larger specific surface area, greater electronic mobility, and intrinsic band gap. The analyses presented in this work reveal relevant features of graphyne in an interaction with an electrolyte that can be useful for practical applications. Although there is already a considerable volume of work on graphyne, the analysis of its properties taking into account the dynamics of its network and the interaction with the condensed medium has not yet been presented. Here, ab initio molecular dynamics simulations were performed to study the energetic, structural, spectroscopic, and electronic properties of graphene and graphyne electrodes in vacuum and in the presence of an electrolyte (EMIM-BF 4 ). A detailed analysis of the electrode–electrolyte interaction is reported for both systems. Structural features are presented in terms of both radial and spatial distribution functions and angular orientation distributions. Power spectral analyses and molecular orbital maps provided important insights into the intermolecular interactions in graphene and graphyne systems, describing the main differences as well as revealing similarities between them.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Understanding the cold plasma synthesis of ammonia with model metal catalysts through plasma diagnostics (Final Report)

The industrial synthesis of ammonia, which amounts to over 200 million tons annually, is the most energy-intensive chemical process. Therefore, there is a critical need and increased interest in exploring less energetic routes to produce ammonia. Not only does ammonia have a direct impact on the food market, but also it has the potential as a fuel and hydrogen carrier. Recently, plasma catalysis has emerged as a promising alternative for synthesizing ammonia at mild (pressure, temperature and power) conditions. The key to this catalytic process is the synergy between the plasma and the catalyst, where the non-equilibrium plasma allows the generation of excited species, which recombine at the catalyst surface to form ammonia. However, our current understanding of this process is in its infancy. In this respect, model metals are ideal candidates for gaining a basic understanding of this reaction. Moreover, a major roadblock to rationally designing novel effective catalysts for plasma-assisted ammonia production is the need for fundamental aspects of this process. Through a comprehensive plan that integrates model metals as catalysts and world-class diagnostics, the proposed work aims to provide fundamental knowledge about the nature of reactive processes occurring during plasma-assisted catalysis and to demonstrate the selective production of ammonia, catalyzed by employing selected metals under non-thermal plasma conditions. Toward this goal, the central thrust of this proposal was to demonstrate that the synergy between plasma and rationally selected model metals will boost ammonia yields during plasma-assisted ammonia synthesis by delaying hydrogen recombination. Specifically, we aimed to (1) understand the formation and role of gas-phase active species such as NH, N 2 , N 2 + and Ha during the plasma-enhanced synthesis of ammonia through OES and FTIRAS using different reaction configurations: a) only plasma (non-packed DBD reactor) and b) packed DBD reactor with metal nanoparticles. This proposal was awarded/recommended with a run time on the PCRF facility FY20.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1972

Discussion of the reliability of electron densities and energies interpreted from data and limits on the proton energy and density

Analysis of radio observations of Jupiter were changed to take into account the antenna resolution. A dipole magnetic field with a surface equatorial value of 7 gauss is assumed. The electron temperature is found to increase for r 2.5 Jupiter radii with decreasing r as 1/r cubed, reaching a peak of about 100 MeV at r = 2.5 Jupiter radii. For r 2.5 Jupiter radii, the electron temperature goes as r to the 6th power because of energy lost to radiation. The consequences of making an upper estimate on the proton flux by assuming the magnetic field is loaded with all the energetic protons it can hold are described. The upper limits of proton energy, density, flux, and energy flux are calculated for 1, 2, 2.5, 3, and 6 Jupiter radii. The proton energy and velocity estimates are considered to be fairly reliable; the upper limit to the number density is probably much higher than actuality.

Beard, D. B.↗
DOE OSTI2021

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

Interfacially confined microenvironments have recently gained attention in catalysis, as they can be used to modulate reaction chemistry. The emergence of a 2D nanospace at the interface between a 2D material and its support can promote varying kinetic and energetic schemes based on molecular level confinement effects imposed in this reduced volume. We report on the use of a 2D oxide cover, bilayer silica, on catalytically active Pd(111) undergoing the CO oxidation reaction. We “uncover” mechanistic insights about the structure-activity relationship with and without a 2D silica overlayer using in situ IR and X-ray spectroscopy and mass spectrometry methods. We find that the CO oxidation reaction on Pd(111) benefits from confinement effects imposed on surface adsorbates under 2D silica. Finally, this interaction results in a lower and more dispersed coverage of CO adsorbates with restricted CO adsorption geometries, which promote oxygen adsorption and lay the foundation for the formation of a reactive surface oxide that produces higher CO 2 formation rates than Pd alone.

36 MATERIALS SCIENCE↗
NASA NTRS1972

Diffusion models for Jupiter's radiation belt

Solutions are given for the diffusion of trapped particles in a planetary magnetic field in which the first and second adiabatic invariants are preserved but the third is not, using as boundary conditions a fixed density at the outer boundary (the magnetopause) and a zero density at an inner boundary (the planetary surface). Losses to an orbiting natural satellite are included and an approximate evaluation is made of the effects of the synchrotron radiation on the energy of relativistic electrons. Choosing parameters appropriate to Jupiter, the electrons required to produce the observed synchrotron radiation are explained. If a speculative mechanism in which the diffusion is driven by ionospheric wind is the true explanation of the electrons producing the synchrotron emission it can be concluded that Jupiter's inner magnetosphere is occupied by an energetic proton flux that would be a serious hazard to spacecraft.

Jacques, S. A.↗
NASA NTRS2007

First X-ray Observations of the Young Pulsar J1357-6429

The first short Chandra and XMM-Newton observations of the young and energetic pulsar J1357-6429 provided strong indications of a tail-like pulsar-wind nebula associated with this object, as well as strong pulsations of its X-ray flux with a pulsed fraction above 40% and a thermal component dominating at lower photon energies (below 2 keV). The elongated nebular is very compact in size. about 1" x 1.5" and might be interpreted as a pulsar jet. The thermal radiation is most plausibly emitted from the entire neutron star surface of an effective temperature about 1 MK covered with a magnetized hydrogen atmosphere At higher energies the pulsar's emission is of a nonthermal (magnetospheric) origin, with a power-law spectrum of a photon index Gamma approx. equals 1.1. This makes the X-ray properties of PSR J1357-6429 very similar to those of the youngest pulsars J1119-6127 and Vela with a detected thermal radiation.

Zavlin, Vyacheslav E.↗
DOE OSTI2020

Resonance-Promoted Formic Acid Oxidation via Dynamic Electrocatalytic Modulation

It is a truth universally acknowledged that faster catalysts enable more efficient transformation of molecules to useful products and enhance the utilization of natural resources. However, the limit of static catalyst performance defined by the Sabatier principle has motivated a dynamic approach to catalyst design, whereby catalysts oscillate between varying energetic states. In this work, the concept of dynamic catalytic resonance was experimentally demonstrated via the electrocatalytic oxidation of formic acid over Pt. Oscillation of the electrodynamic potential between 0 and 0.8 V NHE via a square waveform at varying frequency (10 –3 < f < 10 3 Hz) increased the turnover frequency to ~20 s –1 at 100 Hz, over one order of magnitude (20×) faster than optimal potentiostatic conditions. We attribute the accelerated dynamic catalysis to nonfaradaic formic acid dehydration to surface-bound carbon monoxide at low potentials, followed by surface oxidation and desorption to carbon dioxide at high potentials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1987

Proton and oxygen plasmas at Uranus

Despite the presence of several large, ice moons within the Uranian magnetosphere, the Voyager 2 spacecraft did not detect any heavy ion plasma. This paper estimates the heavy ion density that would be consistent with a heavy neutral torus formed by photosputtering, charged particle sputtering, and micrometeoroid impact vaporization of icy surfaces on the moons, taking into account the large 60 deg angle between the satellite orbit plane and the magnetic equator. The expected heavy ion density is unobservably small. The observed proton plasma of the inner magnetosphere can be maintained by ionization of the atomic hydrogen corona and by the ionospheric proton source driven by photoelectron escape, for a plasma residence time of about 30 days. These two proton sources are comparable near L = 5. The same 30-day residence time for energetic protons implies an upper limit of 0.00001 on the fraction of incident solar wind protons that enter the magnetosphere and penetrate to within L less than 6 while conserving their first adiabatic invariants.

Cheng, Andrew F.↗
NASA NTRS2004

Ion Flux Environments for Exposed Spacecraft Surfaces in Interplanetary Space

Spacecraft surfaces in interplanetary space are exposed to solar wind ions. The bulk of the ions exhibit energies of a few kilovolts and are important only to surface interactions while a fraction of the solar wind extends to greater energies and may penetrate below the material surface. The importance of including solar wind ions in analysis of space environment effects on spacecraft is becoming more important as new spacecraft designs are considered which include systems such as sunshades, solar sail propulsion systems, and other mission critical features based on very thin materials. This paper provides a status report on development of solar wind ion environments to support engineering analysis of materials exposed to the space environment including techniques for reconstructing ion environments from solar wind plasma moments and energetic flux measurements and comparison of statistical flux environments to integrated mission fluence.

Minow, Joseph I.↗
NASA NTRS2010

Complex Role of Secondary Electron Emissions in Dust Grain Charging in Space Environments: Measurements on Apollo 11 and 17 Dust Grains

Dust grains in various astrophysical environments are generally charged electrostatically by photoelectric emissions with radiation from nearby sources, or by electron/ion collisions by sticking or secondary electron emissions. Knowledge of the dust grain charges and equilibrium potentials is important for understanding of a variety of physical and dynamical processes in the interstellar medium (ISM), and heliospheric, interplanetary, planetary, and lunar environments. The high vacuum environment on the lunar surface leads to some unusual physical and dynamical phenomena involving dust grains with high adhesive characteristics, and levitation and transportation over long distances. It has been well recognized that the charging properties of individual micron/submicron size dust grains are expected to be substantially different from the corresponding values for bulk materials and theoretical models. In this paper we present experimental results on charging of individual dust grains selected from Apollo 11 and Apollo 17 dust samples by exposing them to mono-energetic electron beams in the 10- 400 eV energy range. The charging rates of positively and negatively charged particles of approximately 0.2 to 13 microns diameters are discussed in terms of the secondary electron emission (SEE) process, which is found to be a complex charging process at electron energies as low as 10-25 eV, with strong particle size dependence. The measurements indicate substantial differences between dust charging properties of individual small size dust grains and of bulk materials.

Abbas, M. M.↗
DOE OSTI2020

Kinetic versus Thermodynamic Stability of LLZO in Contact with Lithium Metal

Li 7 La 3 Zr 2 O 12 (LLZO) garnet-based oxides are a promising class of solid electrolytes used as the separator in all-solid-state batteries (ASSBs). While LLZO is considered to have a wide electrochemical stability window, its intrinsic stability in contact with lithium metal is not sufficiently well understood, and there is still a debate on the key question of whether LLZO does or does not form passivation layers before and during cycling. Utilizing both in situ and operando X-ray photoelectron spectroscopy techniques, in this work we reveal the presence of a kinetic barrier to the reduction of LLZO by Li metal, with the extent of oxygen-deficient interphase (ODI) formation depending sensitively on the energetics of Li metal arriving at the Li vertical bar LLZO interface. Despite the clear presence of a kinetic barrier to reduction, the electrochemical response of the Li vertical bar LLZO interface is unchanged by the presence of the ODI, indicating that ODI formation during electrochemical cycling does not hinder charge transfer across the Li vertical bar LLZO interface. Overall, these results reveal that the reactivity of LLZO with Li metal depends not only on the material properties of the adjoining phases (i.e., surface purity and active contact) and their resulting thermodynamic stability but also on the energy input at the interface and the resulting reaction kinetics. Furthermore, the presence of a kinetic barrier to reduction highlights the additional complexities governing the reactivity of solid-state interfaces in ASSBs and underscores the importance of operando characterization of interfacial stability to design more robust, high-performance protection strategies for solid electrolytes in contact with reactive electrodes.

25 ENERGY STORAGE↗
NASA NTRS1992

Energetic Particles Investigation (EPI)

The EPI instrument operates during the pre-entry phase of the Galileo Probe. The main objective is the study of the energetic particle population in the inner Jovian magnetosphere and in the upper atmosphere. This will be achieved through omnidirectional measurements of electrons, protons, alpha-particles and heavy ions (Z greater than 2) and recording intensity profiles with a spatial resolution of about 0.02 Jupiter radii. Sectored data will also be obtained for electrons, protons, and alpha-particles to determine directional anisotropies and particle pitch angle distributions. The detector assembly is a two-element telescope using totally depleted circular silicon surface-barrier detectors surrounded by cylindrical tungsten shielding. The lower energy threshold of the particle species investigated during the Probe's pre-entry phase is determined by the material thickness of the Probe's rear heat shield which is required for heat protection of the scientific payload during entry into the Jovian atmosphere. The EPI instrument is combined with the Lightning and Radio Emission Detector and both instruments share one interface of the Probe's power, command, and data unit.

Fischer, H. M.↗
NASA NTRS2004

adwTools Developed: New Bulk Alloy and Surface Analysis Software for the Alloy Design Workbench

A suite of atomistic modeling software, called the Alloy Design Workbench, has been developed by the Computational Materials Group at the NASA Glenn Research Center and the Ohio Aerospace Institute (OAI). The main goal of this software is to guide and augment experimental materials research and development efforts by creating powerful, yet intuitive, software that combines a graphical user interface with an operating code suitable for real-time atomistic simulations of multicomponent alloy systems. Targeted for experimentalists, the interface is straightforward and requires minimum knowledge of the underlying theory, allowing researchers to focus on the scientific aspects of the work. The centerpiece of the Alloy Design Workbench suite is the adwTools module, which concentrates on the atomistic analysis of surfaces and bulk alloys containing an arbitrary number of elements. An additional module, adwParams, handles ab initio input for the parameterization used in adwTools. Future modules planned for the suite include adwSeg, which will provide numerical predictions for segregation profiles to alloy surfaces and interfaces, and adwReport, which will serve as a window into the database, providing public access to the parameterization data and a repository where users can submit their own findings from the rest of the suite. The entire suite is designed to run on desktop-scale computers. The adwTools module incorporates a custom OAI/Glenn-developed Fortran code based on the BFS (Bozzolo- Ferrante-Smith) method for alloys, ref. 1). The heart of the suite, this code is used to calculate the energetics of different compositions and configurations of atoms.

Bozzolo, Guillermo↗
NASA NTRS1986

A high flux pulsed source of energetic atomic oxygen

The design and demonstration of a pulsed high flux source of nearly monoenergetic atomic oxygen are reported. In the present test setup, molecular oxygen under several atmospheres of pressure is introduced into an evacuated supersonic expansion nozzle through a pulsed molecular beam valve. A 10J CO2 TEA laser is focused to intensities greater than 10 to the 9th W/sq cm in the nozzle throat, generating a laser-induced breakdown with a resulting 20,000-K plasma. Plasma expansion is confined by the nozzle geometry to promote rapid electron-ion recombination. Average O-atom beam velocities from 5-13 km/s at fluxes up to 10 to the 18th atoms/pulse are measured, and a similar surface oxygen enrichment in polyethylene samples to that obtained on the STS-8 mission is found.

Krech, Robert H.↗