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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

TGA Study of the Reaction Kinetics of a CuFeMnAlO 4+δ Oxygen Carrier for Methane Chemical Looping Combustion under High Pressure and Atmospheric Pressure Conditions

Reduction and oxidation kinetics of a CuFeMnAlO 4+δ oxygen carrier for methane were studied using an atmospheric thermogravimetric analyzer (TGA) and a pressurized TGA. Important parameters such as temperature (500–900 °C), particle size distribution (150–650 μm), and partial pressures of reactants (methane and oxygen) were evaluated. Results showed that the reduction of the oxygen carrier was not affected by particle size distribution studied in this work, and that above 750 °C, the effect of the temperature on oxygen carrier reduction started to diminish. The reaction time approaches an asymptotic limit as methane partial pressure increases. For oxygen carrier oxidation, it was found that the rate of oxidation increased with increasing oxygen concentration. The effect of the oxygen concentration was more noticeable when the oxygen concentration was below 7.5%. Because of the inherent feature of the oxygen carrier, its chemical looping with oxygen uncoupling property was also assessed. A phase boundary-controlled shrinking sphere model was used to model the test data from the TGAs. Modeling results showed that the oxygen carrier reduction had a reaction order of 1 with an activation energy of ∼46 kJ/mol. Oxygen carrier oxidation demonstrated a reaction order of 1.1 with an activation energy of ∼55 kJ/mol. Additionally, the differences of the experimental results between the atmospheric pressure TGA and the pressurized TGA were discussed in detail and the limitations of the pressurized TGA were highlighted.

Hydrocarbons↗
NASA NTRS1999

Atmospheric pressure chemical ionization of fluorinated phenols in atmospheric pressure chemical ionization mass spectrometry, tandem mass spectrometry, and ion mobility spectrometry

Atmospheric pressure chemical ionization (APCI)-mass spectrometry (MS) for fluorinated phenols (C6H5-xFxOH Where x = 0-5) in nitrogen with Cl- as the reagent ion yielded product ions of M Cl- through ion associations or (M-H)- through proton abstractions. Proton abstraction was controllable by potentials on the orifice and first lens, suggesting that some proton abstraction occurs through collision induced dissociation (CID) in the interface region. This was proven using CID of adduct ions (M Cl-) with Q2 studies where adduct ions were dissociated to Cl- or proton abstracted to (M-H)-. The extent of proton abstraction depended upon ion energy and structure in order of calculated acidities: pentafluorophenol > tetrafluorophenol > trifluorophenol > difluorophenol. Little or no proton abstraction occurred for fluorophenol, phenol, or benzyl alcohol analogs. Ion mobility spectrometry was used to determine if proton abstraction reactions passed through an adduct intermediate with thermalized ions and mobility spectra for all chemicals were obtained from 25 to 200 degrees C. Proton abstraction from M Cl- was not observed at any temperature for phenol, monofluorophenol, or difluorophenol. Mobility spectra for trifluorophenol revealed the kinetic transformations to (M-H)- either from M Cl- or from M2 Cl- directly. Proton abstraction was the predominant reaction for tetra- and penta-fluorophenols. Consequently, the evidence suggests that proton abstraction occurs from an adduct ion where the reaction barrier is reduced with increasing acidity of the O-H bond in C6H5-xFxOH.

NASA Discipline Environmental Health↗
DOE OSTI2015

Diamond synthesis at atmospheric pressure by microwave capillary plasma chemical vapor deposition

Polycrystalline diamond has been synthesized on silicon substrates at atmospheric pressure, using a microwave capillary plasma chemical vapor deposition technique. The CH{sub 4}/Ar plasma was generated inside of quartz capillary tubes using 2.45 GHz microwave excitation without adding H{sub 2} into the deposition gas chemistry. Electronically excited species of CN, C{sub 2}, Ar, N{sub 2}, CH, H{sub β}, and H{sub α} were observed in the emission spectra. Raman measurements of deposited material indicate the formation of well-crystallized diamond, as evidenced by the sharp T{sub 2g} phonon at 1333 cm{sup −1} peak relative to the Raman features of graphitic carbon. Field emission scanning electron microscopy images reveal that, depending on the growth conditions, the carbon microstructures of grown films exhibit “coral” and “cauliflower-like” morphologies or well-facetted diamond crystals with grain sizes ranging from 100 nm to 10 μm.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Advances and challenges in computational fluid dynamics of atmospheric pressure plasmas

Atmospheric pressure plasmas (APPs) are at the core of diverse technological applications in materials processing, chemical synthesis, resource recovery, water treatment, and medicine, among others. APPs span a wide range of power density, from low-power non-thermal to high-power thermal discharges, and typically involve interactions with a stream of working gas, processing material, or gas environment. The article provides an overview of Computational Fluid Dynamics (CFD) approaches, from mathematical models to software strategies, for the analysis of APP flows. Its focus is flows with large variations in ionization degree and significant fluid dynamic-thermal-electromagnetic coupling, as particularly found in mid- to high-power discharges. The advances achieved and challenges faced by CFD of APP flows have been driven by established and emerging applications, and can be broadly characterized in terms of model fidelity and numerical accuracy. Fidelity refers to the degree of underlying phenomena captured by the model, whereas accuracy to the precision of the numerical solution of the model. Two distinct numerical accuracy challenges are addressed: the capture of instability and pattern formation phenomena, and of plasma-gas interaction and turbulence; as well as two representative fidelity challenges: radiative transport under nonequilibrium conditions, and nonequilibrium electron and particle kinetics. The purpose of this article is to offer guidance to researchers, from modelers and code developers to open-source and commercial software users, working on CFD analyses of APP flows within technological contexts.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Particle charge distributions in the effluent of a flow-through atmospheric pressure low temperature plasma

Atmospheric pressure low-temperature plasmas are often utilized to perform particle synthesis, treatment, and removal. It is well-known that dust particles are highly negatively charged in these plasmas; however, little is known about dust particle charging behavior as particles leave the plasma volume and pass through the spatial afterglow region. In this work, monodisperse particles of various sizes and work functions were introduced into an atmospheric pressure radiofrequency capacitively coupled flow-through plasma. Dust particle electrical mobility distributions downstream of the flow-through plasma were measured utilizing a differential mobility analyzer in conjunction with a condensation particle counter at various gas flow velocities. Charge distributions were determined from the measured electrical mobility distributions. Experiments confirm that particles become less negatively charged, and even net-positively charged after leaving the plasma volume, with a distribution that follows a shifted Boltzmann charge distribution. Additionally, particle charge in the effluent of the flow-through plasma is negligibly dependent on work function but highly size and flow velocity dependent. Larger particles were shown to have a higher magnitude of charge under all studied conditions; however, particle polarity was switchable by varying gas flow velocity. The charging dynamics were simulated utilizing a constant number Monte Carlo model that accounts for electron temperature decay and the transition from ambipolar to free diffusion of electrons and ions in the spatial afterglow. Simulation results also suggest that, at the same flow velocity, larger particles obtain a greater magnitude of charge, negative or positive. Furthermore, the decrease in electron mobility and the difference between ion and electron convective loss rates create an ion-rich region in the plasma effluent that promotes ion–particle collisions and drives particle charge removal and even reversal of polarity. Larger particles more favorably collide with energetic species in these environments, which results in higher charge states.

atmospheric pressure low temperature plasma↗
DOE OSTI2020

Interactions between atmospheric pressure plasmas and metallic catalyst particles in packed bed reactors

Atmospheric-pressure plasmas sustained in packed bed reactors (PBRs) are being investigated for chemical conversion of gases and pollution control. Metallic catalysts added to the surfaces of the dielectric beads of PBRs can increase the energy efficiency and selectivity of chemical processes by reducing operating temperature and providing additional reaction pathways. In this paper, results from a computational investigation of plasma surface interactions between micron-scale metallic catalysts and humid-air plasmas in PBRs are discussed. Here we found that high plasma density regions form in the proximity of the metallic catalysts. These higher-density plasma regions were confirmed experimentally using ICCD imaging. The intense plasmas result from geometrical electric field enhancement and redistribution of charges within the conductive particles, leading to further enhancement. The high electric field at the triple points of the catalysts can produce electric field emission of electrons, which provides a pre-ionization source or additional source of electrons. These regions of high electric field and sources of electrons guide discharges towards the catalysts and increases fluxes of excited species, ions, electrons and photons to their surfaces. These fluxes are focused primarily at the triple points between the metal, dielectric and gas. As a result, the catalyst is locally heated, which could lead to further increased rates of thermocatalytic reactions on the surface. Surface roughness of the metal inclusions can lead to additional electric field enhancement, which changes the character of the discharges in the vicinity of the catalysts while reducing breakdown voltage.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Interaction between pulsed discharge and radio frequency discharge burst at atmospheric pressure

The atmospheric pressure glow discharges (APGD) with dual excitations in terms of pulsed voltage and pulse-modulation radio frequency (rf) power are studied experimentally between two parallel plates electrodes. Pulse-modulation applied in rf APGD temporally separates the discharge into repetitive discharge bursts, between which the high voltage pulses are introduced to ignite sub-microsecond pulsed discharge. The discharge characteristics and spatio-temporal evolution are investigated by means of current voltage characteristics and time resolved imaging, which suggests that the introduced pulsed discharge assists the ignition of rf discharge burst and reduces the maintain voltage of rf discharge burst. Furtherly, the time instant of pulsed discharge between rf discharge bursts is manipulated to study the ignition dynamics of rf discharge burst.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2016

Atmospheric-pressure glow plasma synthesis of plasmonic and photoluminescent zinc oxide nanocrystals

In this paper, we present a large-volume (non-micro) atmospheric pressure glow plasma capable of rapid, large-scale zinc oxide nanocrystal synthesis and deposition (up to 400 μg/min), whereas in the majority of the literature, nanoparticles are synthesized using micro-scale or filamentary plasmas. The reactor is an RF dielectric barrier discharge with a non-uniform gap spacing. This design encourages pre-ionization during the plasma breakdown, making the discharge uniform over a large volume. The produced zinc oxide nanocrystals typically have diameters ranging from 4 to 15 nm and exhibit photoluminescence at ≈550 nm and localized surface plasmon resonance at ≈1900 cm{sup −1} due to oxygen vacancies. The particle size can be tuned to a degree by varying the gas temperature and the precursor mixing ratio.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Concomitant ion effects on isotope ratio measurements with liquid sampling – atmospheric pressure glow discharge ion source Orbitrap mass spectrometry

RATIONALE: The field of highly accurate and precise isotope ratio (IR) analysis has been dominated by inductively coupled plasma and thermal ionization mass spectrometers. While these instruments are considered the gold standard for IR analysis, the International Atomic Energy Agency desires a field deployable instrument capable of accurately and precisely measuring U isotope ratios. METHODS: The proposed system interfaces the liquid sampling – atmospheric pressure glow discharge (LS-APGD) ion source with a high resolution Exactive Orbitrap mass spectrometer. With this experimental setup certified U isotope standards and unknown samples were analyzed. The accuracy and precision of the system were then determined. RESULTS: The LS-APGD /Exactive instrument measures a certified reference material of natural U (235U/238U = 0.007258) as 0.007041 with a relative standard deviation of 0.158% meeting the International Target Values for Uncertainty for the destructive analysis of U. Additionally, when three unknowns measured and compared to the results from an ICP multi collector instrument, there is no statistical difference between the two instruments. CONCLUSIONS: The LS-APGD / Orbitrap system, while still in the preliminary stages of development, offers highly accurate and precise IR analysis that suggest a paradigm shift in the world of IR analysis. Furthermore, the portability of the LS-APGD as an elemental ion source combined with the low overhead and small size of the Orbitrap suggest that the instrumentation is capable of being field deployable. With liquid sampling glow discharge-Orbitrap MS, isotope ratio and precision performance improves with rejection of concomitant ion species.

atmospheric pressure sampling↗
DOE OSTI2022

Production and diffusion of H 2 O 2 during the interaction of a direct current pulsed atmospheric pressure plasma jet on a hydrogel

The interaction of cold atmospheric pressure plasma jets with hydrogels has been used as a model system to study the interaction of plasmas with tissues. In this study, we analyze the diffusion of reactive oxygen species (in particular H 2 O 2 ) and quantify the amount of plasma-produced H 2 O 2 species that penetrates into a gelatin hydrogel. We show that the diffusion constant of H 2 O 2 in 10% gelatin hydrogel is similar to its diffusion constant in water and that the production of H 2 O 2 in the hydrogel is significantly less than the production of H 2 O 2 in distilled water for the same plasma operation conditions suggesting that the scavenging of OH radicals at the plasma-gel interface significantly reduces the H 2 O 2 production.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2021

Ion fluxes and memory effects in an Ar–O 2 modulated radiofrequency-driven atmospheric pressure plasma jet

In this work we used molecular beam mass spectrometry to characterize ion fluxes produced by a modulated radiofrequency (RF)-driven atmospheric pressure plasma jet operating in a homogeneous gas environment (Ar + 1% O 2 ). The influence of the RF modulation frequency (100 Hz to 20 kHz) on the ion fluxes was investigated by time-resolved measurements, and the lifetimes of the dominant ions, O 2 + , NO + , O − , O 2 − and O 3 − , were found to be 28 ± 2, 117 ± 8, 7.3 ± 0.4, 17 ± 1 and 23 ± 2 μs, respectively. The absolute ion densities in the near afterglow region were found to be of the order of 1011 cm−3. Significant differences in the dynamics of the positive and negative ions were found; these are explained by the presence of electrons at similar densities in the afterglow produced by electron detachment reactions from negative ions due to the large concentrations of atomic oxygen and singlet delta oxygen. Transitions in ion flux dynamics for different modulation frequencies and at the startup of the plasma were analyzed together with intensified charge coupled device images recording the plasma propagation in order to assess the dynamics of plasma plume propagation and how it is impacted by ‘memory effects’. Quantitative measurements of the ion densities enabling these memory effects are reported. The results in this paper highlight the tremendous impact of memory effects on plasma propagation and the corresponding pre-ionization.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Design and characterization of a solar-enhanced microwave plasma reactor for atmospheric pressure carbon dioxide decomposition

The decomposition of carbon dioxide (CO 2 ) is a main step in carbon re-utilization approaches aimed to fulfill fuels and chemicals demands and mitigate environmental emissions. Plasmachemical CO 2 decomposition processes can be highly efficient; however, their reliance on electrical energy can limit their economic viability and sustainability advantage. In contrast, solar thermochemical CO 2 decomposition approaches can have limited efficiency, but their direct use of the most abundant form of renewable energy affords them the greatest sustainability potential. Solar-Enhanced Microwave Plasma (SEMP) chemical synthesis, based on the direct interaction between microwave plasma and concentrated solar radiation, is investigated as a novel approach to combine the advantages of plasmachemical and solar thermochemical processes. SEMP is motivated by the potential for synergistic effects between solar photons and plasma species, implied by the markedly greater spectral absorption of nonequilibrium CO 2 plasma compared to that of equilibrium CO 2 , to lead to enhanced chemical decomposition. The design, development, and characterization of a SEMP reactor for atmospheric pressure CO 2 decomposition is presented. The reactor is powered by a 1.25 kW magnetron and by up to 525 W of incident radiative power from a high-flux solar simulator. Experimental results reveal that the microwave plasma absorbs up to 20% of concentrated solar radiation at a solar-to-electrical power ratio of 0.5, and that relative absorption decreases with increasing solar input power. Yet, conversion efficiency and plasma energy efficiency increase with increasing solar power, up to 9% and 25% respectively, for a solar-to-electrical power ratio of 0.75. The enhanced process performance appears to be a consequence of the greater power density in the plasma caused by the direct absorption of solar radiation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2018

Design and characterization of an electromagnetic-resonant cavity microwave plasma reactor for atmospheric pressure carbon dioxide decomposition

Plasma processes are ideally suited for the conversion of renewable electricity into gas-phase reactivity, such as for the decomposition of carbon dioxide (CO 2 ). The design, development, and characterization of a microwave plasma reactor for atmospheric pressure undiluted carbon dioxide decomposition are presented. The reactor operates as an electromagnetic-resonant cavity in which the generated plasma forms a bulb attached to a converging-diverging nozzle and stabilized by streams of tangentially-injected processing gas. Electromagnetic wave confinement, residence time, and critical gas vorticity constitute fundamental reactor sizing and operation parameters. Experimental findings demonstrate that flow rate plays a dual role in plasma stabilization and process performance, whereas deposited power has a minor role in CO 2 decomposition.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2017

Effect of water vapor on plasma morphology, OH and H 2 O 2 production in He and Ar atmospheric pressure dielectric barrier discharges

Although atmospheric pressure dielectric barrier discharges (DBDs) have a long history, the effects of water vapor on the discharge morphology and kinetics have not been studied intensively. We report a simultaneous investigation of discharge morphology, OH and H 2 O 2 production in Ar and He DBDs operated at different water vapor concentrations and powers. The combined study allows us to assess the impact of the discharge morphology and power on the concentration dependence of the OH and H 2 O 2 production. The morphology of the discharge is investigated by ICCD images and current–voltage waveforms. These diagnostics are complemented by broadband absorption and a colorimetric method to measure the gas temperature and the OH and H 2 O 2 concentrations. The number of filaments in Ar DBD increases with increasing water concentration and power. The surface discharge part of the micro-discharge also reduces with increasing water concentration most likely due to a change in surface conductivity of the dielectric with changing water concentration. The OH density in the case of Ar is approximately double the OH density in He for similar power and water admixture. In contrast to the root square dependence of the OH density on the water concentration in He similar to diffuse RF discharges, the OH density in Ar increases for small water concentrations followed by a saturation and reduces for higher water concentrations. Furthermore, this dependence of OH density on water concentration is found to correlate with changes in discharge morphology. An analytical balance of the production and destruction mechanism of H 2 O 2 is shown to be able to reproduce the ratio of the measured OH and H 2 O 2 density for realistic values of electron densities.

42 ENGINEERING↗
DOE OSTI2019

Ultra-High Resolution Elemental/Isotopic Mass Spectrometry (m/?m> 1,000,000): Coupling of the Liquid Sampling-Atmospheric Pressure Glow Discharge with an Orbitrap Mass Spectrometer for Applications in Biological Chemistry and Environmental Analysis

Many fundamental questions of astrophysics, biochemistry, and geology rely on the ability to accurately and precisely measure the mass and abundance of isotopes. Taken a step further, the capacity to perform such measurements on intact molecules provides insights into processes in diverse biological systems. Described here is the coupling of a combined atomic and molecular (CAM) ionization source, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma, with a commercially available ThermoScientific Fusion Lumos mass spectrometer. Demonstrated for the first time is the ionization and isotopically-resolved fingerprinting of a long-postulated, but never mass-spectrometrically observed, bi-metallic complex Hg:Se-cysteine. Such a complex has been implicated as having a role in observations of Hg detoxification by selenoproteins/amino acids. Demonstrated as well is the ability to mass spectrometrically-resolve the geochronologically important isobaric 87Sr and 87Rb species (?m ~ 0.3 mDa, mass resolution m/?m ? 1,700,000). The mass difference in this case reflects the beta-decay of the 87Rb to the stable Sr isotope. These two demonstrations highlight what may be a significant change in bioinorganic and atomic mass spectrometry, with impact expected across a broad spectrum of the physical, biological and geological sciences.

Hoegg, Edward D.↗