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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 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
NASA NTRS2002

Fundamental Studies on Two-Phase Gas-Liquid Flows Through Packed Beds in Microgravity

In the typical operation of a packed-bed reactor, gas and liquid flow simultaneously through a fixed bed of solid particles. Depending on the application, the particles can be of various shapes and sizes and provide for intimate contact and high rates of transport between the phases needed to sustain chemical or biological reactions. The packing may also serve as either a catalyst or as a support for growing biological material. NASA has flown two of these packed-bed systems in a microgravity environment with limited or no success. The goal of this research is to develop models (with scale-up capability) needed for the design of the physicochemical equipment to carry out these unit operations in microgravity. New insight will also lead to improvements in normal gravity operations. Our initial experiment was flown using an existing KC-135 two-phase flow rig with a modified test section. The test section is a clear polycarbonate rectangular column with a depth of 2.54 cm, a width of 5.08 cm, and 60 cm long. The column was randomly packed with spherical glass beads by slowly dropping the beads into the bed. Even though care was taken in handling the column after it was filled with packing, the alternating high and low gravity cycles with each parabola created a slightly tighter packed bed than is typically reported for this type. By the usual method of comparing the weight difference of a completely dry column versus a column filled with water, the void fraction was found to be .345 for both sizes of beads used. Five flush mounted differential pressure transducers are spaced at even intervals with the first location 4 cm from the inlet port and the subsequent pressure transducers spaced at 13 cm intervals along the column. Differential pressure data was acquired at 1000 Hz to adequately observe pulse formation and characteristics. Visual images of the flow were recorded using a high-speed SVHS system at 500 frames per second. Over 250 different test conditions were evaluated along with a companion set of tests in normal gravity. The flow rates, fluid properties and packing properties were selected to provide a range of several orders-of-magnitude for the important dimensionless parameters. Additional information is included in the original extended abstract.

Balakotaiah, Vemuri↗
DOE OSTI2025

Mechanism of the Non‐Kasha Fluorescence in Pyrene

The high-energy shoulder in the gas-phase fluorescence emission spectrum of pyrene is a well-known example of non-Kasha emission. Here, we comparatively assess two approaches, vibronic perturbation theory and nonadiabatic dynamics, in their ability to predict and explain the gas-phase fluorescence spectrum of pyrene. While both methods qualitatively capture the non-Kasha emission, they differ in their computational requirements, accuracy, and physical interpretation. Vibronic perturbation theory and nonadiabatic dynamics are complementary and can be combined in a two-step approach to non-Kasha fluorescence.

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

Resonance-stabilized radical clustering bridges the gap between gaseous precursors and soot in the inception stage

Carbonaceous particles are widespread in combustion, atmospheric, extraterrestrial, and nanomaterials environments. Resonance-stabilized radicals (RSRs) are commonly identified in fuel combustion and pyrolysis processes and play an essential role in carbonaceous particle formation. Despite their importance, comprehensive experimental and mechanistic understanding of particle inception through RSR reactions is lacking. This work investigated particle size distribution, chemical composition, and thermal behavior of soot particles generated by the flow reactor pyrolysis reactions of typical RSRs, in particular, 1-indenyl, 1-methylnaphthyl, and 2-methylnaphthyl radicals, and by the pyrolysis of hydrocarbons with a variety of structures. Particle size distributions show soot particles with mobility diameters in an incipient-particle range of 1.3 to 1.6 nm. Laser desorption/ionization mass spectrometry results suggest that soot products consist of much larger covalently bound clusters (CBCs) than those observed in the gas phase. Under our experimental conditions, the CBCs exhibit a phase transition for particles with calculated molecular diameters of around 1.5 nm. Evaporation experiments and thermogravimetric analysis of the soot products reveal distinct thermal characteristics for small and large CBCs. These results implicate CBCs as bridges between gas-phase species and soot particles. The present work provides a soot-inception mechanism called RSR clustering (RSRC) that is characterized by the reactive clustering of RSRs. The RSRC mechanism contrasts with conventional soot formation models that attribute soot inception primarily to the aggregation of large-size polycyclic aromatic hydrocarbons.

carbonaceous particle↗
DOE OSTI2026

Removal of trace gases can both increase and decrease cloud droplet formation

Aerosols consist of liquid or solid particles dispersed in a gas. Aerosol measurements generally rely on drying the particles before quantifying their physicochemical properties. This drying can potentially remove semivolatile compounds from the particles. Here, we show size-resolved cloud condensation nuclei (CCN) measurements quantifying the hygroscopicity parameter in the presence and absence of a denuder. The denuder efficiently removed alkanes and weakly functionalized acids, aldehydes, and alcohols with fewer than 10 carbon atoms from the gas phase. Denuding organic compounds perturbed the CCN-derived hygroscopicity parameter by up to 50%. Denuding either rendered the particles more or less CCN active, and the direction of the effect depended on sample relative humidity and trace gas concentration. The effect was weakest in early spring and strongest in late spring and summer. The measurements demonstrate an unexpectedly strong coupling between the particle and gas phase, influencing CCN activity through either volatilization or surface adsorption, or both.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1976

The structure of cometary ionospheres. I - H2O dominated comets

A hydrodynamic description of the density distributions of the ionic products of H2O and CO in the atmosphere of an H2O-dominated comet having 10% CO is given. Two models are discussed. In the first, the effecs of photodissociation, photoionization, and gas-phase reactions are considered. In the second, the effect of an internal ionization source is also included. It is found that while the observed morphology of the H2O(+) coma of Comet Kohoutek (1973f) cannot be explained by gas-phase reactions alone, it is consistent with the presence of a strong internal source of ionization, presumably an electric current flowing through the inner coma. In the latter case the number densities of H2O(+) and CO(+) remain more or less constant within the scale lengths against collisional dissociation by the electron flux of their neutrals. While the abundance ratio of CO(+) to H2O(+) remains considerably less than unity when the internal ionization source is neglected, it is significantly larger than unity when the internal ionization source is included. Consequently, even the so-called 'CO-rich' comets may in reality be H2O-dominated, provided a strong internal source of ionization is operative.

Ip, W.-H.↗
NASA NTRS1979

Performance characteristics of a slagging gasifier for MHD combustor systems

The performance of a two stage, coal combustor concept for magnetohydrodynamic (MHD) systems was investigated analytically. The two stage MHD combustor is comprised of an entrained flow, slagging gasifier as the first stage, and a gas phase reactor as the second stage. The first stage was modeled by assuming instantaneous coal devolatilization, and volatiles combustion and char gasification by CO2 and H2O in plug flow. The second stage combustor was modeled assuming adiabatic instantaneous gas phase reactions. Of primary interest was the dependence of char gasification efficiency on first stage particle residence time. The influence of first stage stoichiometry, heat loss, coal moisture, coal size distribution, and degree of coal devolatilization on gasifier performance and second stage exhaust temperature was determined. Performance predictions indicate that particle residence times on the order of 500 msec would be required to achieve gasification efficiencies in the range of 90 to 95 percent. The use of a finer coal size distribution significantly reduces the required gasifier residence time for acceptable levels of fuel use efficiency. Residence time requirements are also decreased by increased levels of coal devolatilization. Combustor design efforts should maximize devolatilization by minimizing mixing times associated with coal injection.

Smith, K. O.↗
NASA NTRS1981

Excited ozone is a possible source of atmospheric N2O

Consideration is given to the possibility that internally excited ozone formed in the three-body recombination reaction between oxygen atoms and molecules may be a potential source of atmospheric N2O through a gas-phase reaction with nitrogen molecules. Determinations of the wavelength dependence of the quantum yield for N2O formation from the photolysis of dilute solutions of O3 in liquid N2 and of the O(1D) quantum yield in the gas-phase photolysis of O3 are interpreted as suggesting the possibility of the excited ozone reaction, and a new expression for N2O quantum yield is derived. An expression for the production rate of N2O through the proposed reaction is then obtained and used to calculate atmospheric concentrations and fluxes of N2O. The theoretical profile obtained is found to agree better with experimental data than that obtained without the excited ozone reaction taken into account and to demonstrate a wide variability in N2O mixing ratios. In addition, the existence of the new N2O source is noted to imply a significantly smaller flux of N2O from surface microbiological activities, and provide a possible physical basis for latitudinal and temporal N2O variations and an additional stability for the ozone layer.

Prasad, S. S.↗
NASA NTRS1996

Polar Vortex Conditions During The 1995-96 Arctic Winter: MLS ClO and HNO3

Microwave Limb Sounder (MLS) measurements of lower stratospheric ClO and HNO3 during the 1995-96 Arctic winter are presented. The 1995-96 Arctic winter was both colder and more persistently cold than usual, leading to an enhancement in lower stratospheric ClO of greater magnitude, vertical extent, and duration than previously observed in the Arctic. Vortex concentrations of HNO3 in mid-December were large due to diabatic descent. Trajectory calculations indicate that localized severe depletions of gas-phase HNO3 in mid-February and early March did not arise from entrainment of midlatitude air into the vortex and were therefore probably related to polar stratospheric cloud (PSC) formation. A strong correlation between temperature and gas-phase HNO3 was evident, consistent with recurring PSC condensation and evaporation cycles.

Santee, M. L.↗
NASA NTRS2001

Particle Generation and Evolution in Silane/Acetylene Flames in Microgravity

The objective of this new experimental program is to advance the understanding of the formation of particles from gas phase combustion processes. The work will utilize the unique SiH4/C2H2 combustion system which generates particulate products ranging from high purity, white SiC to carbonaceous soot depending on equivalence ratio. A key goal of this work is to identify gas phase or particle formation processes that provide the enthalpy release necessary to drive the combustion wave, and to locate the parts of the particle formation process that determine SiC stoichiometry and crystallinity. In a real sense, these SiH4/C2H2 flames act like "highly sooty" hydrocarbon flames, but with simpler chemistry. This simplification is expected to allow them to be used as surrogates to advance understanding of soot formation in such rich hydrocarbon flames. It is also expected that this improved understanding of SiC particle generation and evolution in these self-sustaining flames will advance the commercial potential of the flame process for the generation of high purity SiC powders.

Keil, D. G.↗
NASA NTRS2003

Particle Generation And Evolution In Silane (SiH4)/Acetylene (C2H2) Flames In Microgravity

The objective of this experimental program is to advance the understanding of the coupling of particle formation with gas phase combustion processes. The work utilizes the unique SiH4/C2H2 combustion system which generates particulate products ranging from high purity, white SiC to carbonaceous soot depending on equivalence ratio (Ref. 1). A goal of this work is to identify gas phase or particle formation processes that provide the enthalpy release needed to drive the combustion wave, and to locate the steps of the particle formation process that determine SiC stoichiometry and crystallinity. In a real sense, these SiH4/C2H2 flames act like highly sooty hydrocarbon flames, but with simpler chemistry. This simplification is expected to allow them to be used as surrogates to advance understanding of soot formation in such rich hydrocarbon flames. It is also expected that this improved understanding of SiC particle generation and evolution in these self-sustaining flames will advance the commercial potential of the flame process for the generation of high purity SiC powders.

Keil, D. G.↗
NASA NTRS2011

Application of Laser Mass Spectrometry to Art and Archaeology

REMPI laser mass spectrometry is a combination of resonance enhanced multiphoton ionization spectroscopy and time of flight mass spectrometry, This technique enables the collection of mass specific optical spectra as well as of optically selected mass spectra. Analytes are jet-cooled by entrainment in a molecular beam, and this low temperature gas phase analysis has the benefit of excellent vibronic resolution. Utilizing this method, mass spectrometric analysis of historically relevant samples can be simplified and improved; Optical selection of targets eliminates the need for chromatography while knowledge of a target's gas phase spectroscopy allows for facile differentiation of molecules that are in the aqueous phase considered spectroscopically indistinguishable. These two factors allow smaller sample sizes than commercial MS instruments, which in turn will require less damage to objects of antiquity. We have explored methods to optimize REMPI laser mass spectrometry as an analytical tool to archaeology using theobromine and caffeine as molecular markers in Mesoamerican pottery, and are expanding this approach to the field of art to examine laccaic acid in shellacs.

Gulian, Lase Lisa E.↗
NASA NTRS1986

Interstellar grain mantles

Interstellar molecular grain mantles are an important component of the interstellar dust inside dense molecular clouds as evidenced by the detection of absorption bands at 2.97, 3.08, 4.61, 6.0 and 6.8 microns. Mantles may also be the precursors of more complex grain mantles in the diffuse interstellar medium. The molecular composition of these icy grain mantles were calculated employing gas phase as well as grain surface reactions. The calculated mixtures consist mainly of the molecules H2O, H2CO, N2, CO, O2, H2O2, NH2, and their deuterated counterparts in varying ratios. The exact compositions depend strongly on the physical conditions in the gas phase. The absorption spectra of H2O with other molecules was studied in the laboratory. Optical constants were determined for a few selected mixtures. Extinction and polarization cross sections across the 3 micron ice band were calculated. A comparison with the observations towards BN shows that the low frequency wing observed on this feature is due to absorption by a mixture of H2O and other molecules rather than scattering by large, pure H2O ice grains.

Bregman, J.↗
DOE OSTI2025

Exploring the Coexistence of Spin States in [Fe(tpy-Ph) 2 ] 2+ Complexes on Au(111) Using DFT Calculations

In this work, we systematically study the electronic structure and stability of spin states of the [Fe-(tpy-ph) 2 ] 2+ molecule in both the gas phase and on a Au(111) substrate using density functional theory + U (DFT+ U ) calculations. We find that the stability of the Fe 2+ ion’s spin states predicted by the computations is significantly influenced by the Hubbard U parameter. In the gas phase, the low-spin (LS, S = 0) state is found to be energetically favorable for U (Fe) ≤ 3 eV, whereas the high-spin (HS, S = 2) state is stabilized for U (Fe) > 3 eV. Interaction with the Au(111) substrate is found to elevate the critical U for the spin-state transition to 3.5 eV. Additionally, we perform L-edge X-ray absorption spectroscopy (XAS) calculations for both HS and LS states. The calculated XAS suggests that the HS state more closely aligns with the experimental observations, indicating the potential coexistence of the HS state as the initial state during the X-ray excitation process. These findings enrich our understanding of spin-state dynamics in [Fe(tpy-Ph) 2 ] 2+ .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1982

Model calculations of the molecular composition of interstellar grain mantles

A chemical reaction scheme comprising gas phase as well as grain surface reactions is used for the numerical calculation of the chemical composition of mantles accreting on interstellar grains. The composition of the growing grain mantle is determined on the basis of the relative accretion rates of the gas phase molecules and diffusion-controlled surface reactions. Results show that grain mantles generally consist of the molecules H2O, H2CO, N2, O2, CO, CO2, H2O2, and NH3. A detailed examination of the formation of H2 on grain surfaces leads to the conclusion that it proceeds through hydrogen abstraction from such molecules as H2CO, H2S, N2H2, and N2H4. The IR characteristics of the calculated grain mantles are discussed with emphasis on the observed ice band at the 3250/cm wavelength.

Tielens, A. G. G. M.↗
NASA NTRS1987

Antarctic stratospheric chemistry of chlorine nitrate, hydrogen chloride, and ice - Release of active chlorine

The reaction rate between atmospheric hydrogen chloride (HCl) and chlorine nitrate (ClONO2) is greatly enhanced in the presence of ice particles; HCl dissolves readily into ice, and the collisional reaction probability for ClONO2 on the surface of ice with HCl in the mole fraction range from about 0.003 to 0.010 is in the range from about 0.05 to 0.1 for temperatures near 200 K. Chlorine is released into the gas phase on a time scale of at most a few milliseconds, whereas nitric acid (HNO3), the other product, remains in the condensed phase. This reaction could play an important role in explaining the observed depletion of ozone over Antarctica; it releases photolytically active chlorine from its most abundant reservoir species, and it promotes the formation of HNO3 and thus removes nitrogen dioxide from the gas phase. Hence it establishes the necessary conditions for the efficient catalytic destruction of ozone by halogenated free radicals.

Molina, Mario J.↗
NASA NTRS1992

A source model for the L134N molecular cloud

The dark molecular cloud L134N is observed at millimeter wavelengths in the CS (J = 3-2), OCS (J = 7-6), and HDO (1 sub 11-1 sub 10) transitions. The CS (J = 3-2) transition was observed at four positions within the cloud, while the other two transitions were observed at one position each. Fractional abundances in the LTE approximation are calculated for each emission line detected. L134N appears to have a high-density core characterized by NH3, C3H2, and H(C-13)O(+) emission maps. A lower density envelope characterized by C(0-18), CS (J = 2-1), and SO emission surrounds the core. There appears to be a gas-phase oxygen abundance gradient in L134N with atomic oxygen depleted in the high-density core. Observed molecular distributions within L134N can be explained by a model in which chemical and physical processes in icy-dust-grain mantles influence the gas-phase molecular abundances.

Swade, Daryl A.↗
NASA NTRS1978

The vibrational overtone spectrum of liquid methane in the visible and near infrared - Applications to planetary studies

The strengths of 10 bands in the absorption spectrum of liquid methane between 19,400 and 6190 A have been measured. After a small correction for the polarizability of the liquid is applied for the purpose of comparison with similar gas-phase measurements, it is found that there is no temperature dependence of the band strengths between 95 and 295 K. Changes of band shape with temperature cause the 95 K laboratory spectra to resemble Saturn more than room-temperature observations do. Gas-phase absorption clearly dominates the liquid in planetary spectra, so liquid methane cannot be detected in the outer solar system by earth-based observations.

Ramaprasad, K. R.↗
NASA NTRS1984

The composition of interstellar grain mantles

The molecular composition of interstellar grain mantles employing gas phase as well as grain surface reactions is studied. The calculated mixtures consist mainly of the molecules H2O, H2CO, N2, CO, O2, CO2, H2O2, NH3, and their deuterated counterparts in varying ratios. The exact compositions depend strongly on the physical conditions in the gas phase. The calculated mixtures are compared to the observations by using laboratory spectra of grain mantle analogs. The two are in reasonable agreement except for the strength of the 6.8-micrometers band. A possible solution for this discrepancy is discussed. Finally, future observations are suggested which may shed further light on the composition of interstellar grain mantles.

Tielens, Alexander G. G. M.↗