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NASA NTRS1989

Formation of polycyclic aromatic hydrocarbons in circumstellar envelopes

Production of polycyclic aromatic hydrocarbons in carbon-rich circumstellar envelopes was investigated using a kinetic approach. A detailed chemical reaction mechanism of gas-phase PAH formation and growth, containing approximately 100 reactions of 40 species, was numerically solved under the physical conditions expected in cool stellar winds. The chemistry is based on studies of soot production in hydrocarbon pyrolysis and combustion. Several first-ring and second-ring cyclization processes were considered. A linear lumping algorithm was used to describe PAH growth beyond the second aromatic ring. PAH production using this mechanism was examined with respect to a grid of idealized constant velocity stellar winds as well as several published astrophysical models. The basic result is that the onset of PAH production in the interstellar envelopes is predicted to occur within the temperature interval of 1100 to 900 K. The absolute amounts of the PAHs formed, however, are very sensitive to a number of parameters, both chemical and astrophysical, whose values are not accurately known. Astrophysically meaningful quantities of PAHs require particularly dense and slow stellar winds and high initial acetylene abundance. It is suggested that most of the PAHs may be produced in a relatively small fraction of carbon-rich red giants.

Frenklach, Michael↗

NASA NTRS1984

Possible production by lightning of aerosols and trace gases in Titan's atmosphere

Although lightning has not yet been observed in Titan's atmosphere, the presence of condensable vapors and the deposition of a significant amount of solar energy at the surface suggest the possibility of lightning activity. Based on an understanding of the relationship of lightning activity to the amount of convective energy available on Titan, a lightning energy dissipation rate of 4 x 10 to the -6th W/sq m can be expected. This value is much lower than that for earth or Jupiter, and is a result of both the reduced solar flux at Titan and the absorption of sunlight by the aerosols that lie above the convective layer. For this dissipation rate, the amount of HCN and C2N2 produced by lightning should be greater than that by solar UV, but could be less than that produced by electron precipitation and galactic cosmic rays. Equilibrium calculations indicate that large mole fractions of elemental solid phase carbon will also be produced. Using a simplified model of aerosol formation, coagulation, and settling, it is estimated that a lightning-produced aerosol could have a typical optical depth of 0.01, with values as high as 0.1. The accumulation of soot over geological time might reach a meter or more in depth.

Borucki, W. J.↗

NASA NTRS2001

A Nanometer Aerosol Size Analyzer (nASA) for Rapid Measurement of High-Concentration Size Distributions

We have developed a fast-response Nanometer Aerosol Size Analyzer (nASA) that is capable of scanning 30 size channels between 3 and 100 nm in a total time of 3 seconds. The analyzer includes a bipolar charger (P0210), an extended-length Nanometer Differential Mobility Analyzer (Nano-DMA), and an electrometer (TSI 3068). This combination of components provides particle size spectra at a scan rate of 0.1 second per channel free of uncertainties caused by response-time-induced smearing. The nASA thus offers a fast response for aerosol size distribution measurements in high-concentration conditions and also eliminates the need for applying a de-smearing algorithm to resulting data. In addition, because of its thermodynamically stable means of particle detection, the nASA is useful for applications requiring measurements over a broad range of sample pressures and temperatures. Indeed, experimental transfer functions determined for the extended-length Nano-DMA using the Tandem Differential Mobility Analyzer (TDMA) technique indicate the nASA provides good size resolution at pressures as low as 200 Torr. Also, as was demonstrated in tests to characterize the soot emissions from the J85-GE engine of a T38 aircraft, the broad dynamic concentration range of the nASA makes it particularly suitable for studies of combustion or particle formation processes. Further details of the nASA performance as well as results from calibrations, laboratory tests and field applications are presented.

Han, Hee-Siew↗

NASA NTRS1981

Symposium /International/ on Combustion, 18th, University of Waterloo, Waterloo, Ontario, Canada, August 17-22, 1980, Proceedings

Problems related to combustion generated pollution are explored, taking into account the mechanism of NO formation from nitrogen compounds in hydrogen flames studied by laser fluorescence, the structure and similarity of nitric oxide production in turbulent diffusion flames, the effect of steam addition on NO formation, and the formation of NO2 by laminar flames. Other topics considered are concerned with propellant combustion, fluidized bed combustion, the combustion of droplets and sprays, premixed flame studies, fire studies, and flame stabilization. Attention is also given to coal flammability, chemical kinetics, turbulent combustion, soot, coal combustion, the modeling of combustion processes, combustion diagnostics, detonations and explosions, ignition, internal combustion engines, combustion studies, and furnaces.

Source record↗

NASA NTRS1997

Subsonic Aircraft Contrail and Cloud Effects Special Study (SUCCESS)

During recent years interest in the impact of commercial aircraft on the climate has increased. Aircraft might impact climate in a number of ways. Contrails are clearly a direct radiative forcing mechanism. Exhaust emissions, principally soot and sulfate, might indirectly force the climate by modifying the radiative properties of cirrus clouds. The SUCCESS program was carried out to investigate these issues. It also has several other goals including: better understanding the emissions from aircraft, better understanding the formation of cirrus clouds: better understanding the radiative properties of contrails and clouds and their remote sensing; better understanding the heterogeneous chemistry in the upper atmosphere; and developing new instruments of importance to atmospheric chemistry and cloud physics. SUCCESS took place during April and May of 1997. The NASA DC-8, ER-2, T-39, and 757 aircraft were used as in situ sampling, remote sensing, near field sampling, and emission sources respectively. Most of the operations occurred near the DOE's Atmospheric Radiation Measurement Site in Northern Oklahoma. The DOE operated several other aircraft so that on some days as many as six research aircraft flew together. Numerous new instruments functioned during the mission. This talk will present an overview of SUCCESS from the operational point of view, and provide some of the overall scientific highlights.

Toon, O.B.↗

NASA NTRS1997

Subsonic Aircraft Contrail and Cloud Effects Special Study (SUCCESS)

During recent years interest in the impact of commercial aircraft on the climate has increased. Aircraft might impact climate in a number of ways. Contrails are clearly a direct radiative forcing mechanism. Exhaust emissions, principally soot and sulfate, might indirectly radiative force the climate by modifying the properties of cirrus clouds. The SUCCESS program was carried out to investigate these issues. It also had several other goals including: better understanding the emissions from aircraft, better understanding the formation of cirrus clouds: better understanding the radiative properties of contrail and clouds and their remote sensing; better understanding the heterogeneous chemistry in the upper atmosphere; and developing new instruments of importance to atmospheric chemistry and cloud physics. SUCCESS took place during April and May of 1996. The NASA DC-8, ER-2, T-39, and 757 aircraft were used as in situ sampling, remote sensing, near field sampling, and emission sources respectively. Most of the operations occurred near the DOE's Atmospheric Radiation Measurement Site in Northern Oklahoma. The DOE operated several other aircraft so that on some days as many as six research aircraft operated together. Numerous new instruments operated during the mission. This talk will present an overview of SUCCESS from the operational point of view, and provide some of the overall scientific highlights.

Toon, O. B.↗

NASA NTRS1988

Aerosol formation and distribution in the Arctic during AGASP-II, March-April 1986

The Arctic Gas and Aerosol Sampling Program has undertaken the determination of the distribution, transport, chemistry, aerosol physics, and radiative effects of the 'Arctic haze' air-pollution phenomenon. Attention has been given the April 2-3, 1986 haze zone, with large condensation nuclei, SO2, and soot-carbon concentrations, which appeared near the Barrow Baseline Station. The composite trajectory of the haze zone has been determined, as has its probable source region. After travelling 10,000 km, the haze still had SO2, aerosol black carbon, and condensation nuclei concentrations in excess of those measured off the East Coast of the U.S. in January of the same year.

Schnell, Russell C.↗

NASA NTRS1999

Kinetics and Structure of Superagglomerates Produced by Silane and Acetylene

The evolution of smoke in a laminar diffusion flame involves several steps. The first step is particle inception/nucleation in the high-temperature fuel-rich region of the flame followed by surface growth and coagulation/coalescence of the small particles. As the primary spheres grow in size and lose hydrogen, the colliding particles no longer coalesce but retain their identity as a cluster of primary spheres, termed an agglomerate. Finally, in the upper portion of the flame, the particles enter an oxidizing environment which may lead to partial or complete burnout of the agglomerates. Currently there is no quantitative model for describing the growth of smoke agglomerates up to superagglomerates with an overall dimension of 10 microns and greater. Such particles are produced during the burning of acetylene and fuels containing benzene rings such as toluene and polystyrene. In the case of polystyrene, smoke agglomerates in excess of 1 mm have been observed "raining" out from large fires. Evidence of the formation of superagglomerates in a laminar acetylene/air diffusion flame has been recently reported. Acetylene was chosen as the fuel since the particulate loading in acetylene/air diffusion flames is very high. Photographs were obtained by Sorensen using a microsecond xenon lamp of the "stream" of soot just above the flame. For low flow rates of acetylene, only submicrometer soot clusters are produced and they give rise to the homogeneous appearance of the soot stream. When the flow rate is increased to 1.7 cu cm/s, soot clusters up to 10 microns are formed and they are responsible for the graininess and at a flow rate of 3.4 cu cm/s, a web of interconnected clusters as large as the width of the flame is seen. This interconnecting web of superagglomerates is described as a gel state by Sorensen et al (1998). This is the first observation of a gel for a gas phase system. It was observed that this gel state immediately breaks up into agglomerates due to buoyancy induced turbulence and gravitational sedimentation.

Mulholland, G. W.↗

NASA NTRS1997

Remote Sensing of Aircraft Contrails Using a Field Portable Digital Array Scanned Interferometer

With a Digital Array Scanned Interferometer (DASI), we have obtained proof-of-concept observations with which we demonstrate DASI capabilities for the determination of contrail properties. These include the measurement of the cloud and soot microphysical parameters, as well, the abundances of specific pollutant species such as SO(sub x) or NO(sub x). From high quality hyperspectral data and using radiative transfer methods and atmospheric chemistry analysis in the data reduction and interpretation, powerful inferences concerning cloud formation, evolution and dissipation can be made. Under this sub-topic, we will integrate DASI with computer controlled scanning of the field-of-view to direct the sensor towards contrails and exhaust plumes for tracking the emitting vehicles. The optimum DASI wavelength sensitivity range for sensing contrails is 0.35 - 2.5 micron. DASI deploys on the ground or from aircraft to observe contrails in the vicinity. This enables rapid, accurate measurement of the temporal, spatial, and chemical evolution of contrails (or other plumes or exhaust sources) with a low cost, efficient sensor.

Smith, William Hayden↗

NASA NTRS1985

Fuel-rich catalytic combustion: A soot-free technique for in situ hydrogen-like enrichment

An experimental program on the catalytic oxidation of iso-octane demonstrated the feasibility of the two-stage combustion system for reducing particulate emissions. With a fuel-rich (phi = 4.8 to 7.8) catalytic combustion preburner as the first stage the combustion process was soot free at reactor outlet temperatures of 1200 K or less. Although soot was not measured directly, its absence was indicated. Reaction products collected at two positions downstream of the catalyst bed were analyzed on a gas chromatograph. Comparison of these products indicated that pyrolysis of the larger molecules continued along the drift tube and that benzene formation was a gas-phase reaction. The effective hydrogen-carbon ratio calculated from the reaction products increased by 20 to 68 percent over the range of equivalence ratios tested. The catalytic partial oxidation process also yielded a large number of smaller-containing molecules. The fraction of fuel carbon in compounds having two or fewer carbon atoms ranged from 30 percent at 1100 K to 80 percent at 1200 K.

Brabbs, T. A.↗

NASA NTRS1989

PAH formation in carbon-rich circumstellar envelopes

While there is growing observational evidence that some fraction of interstellar carbon is in polycyclic aromatic hydrocarbons (PAH's), the mechanisms by which these molecules might be formed have not been extensively studied. A detailed investigation of PAH production in the outflowing molecular envelopes of carbon-rich red giant star is presented. The gasphase kinetics of a chemical reaction mechanism developed to study soot production in hydrocarbon flames is modified to apply in circumstellar environments. It was found that astrophysically significant quantities of PAH's can be formed in carbon star envelopes provided the gas is sufficiently dense and resides for a long time in the temperature range of 900 to 1100 k. The precise yield of PAH's is very sensitive to astronomical parameters of the envelope (e.g., mass loss rate, outflow velocity, and acetylene abundance) and certain poorly determined chemical reaction rates.

Feigelson, Eric D.↗

NASA NTRS1991

International Workshop on Stratospheric Aerosols: Measurements, Properties, and Effects

Following a mandate by the International Aerosol Climatology Program under the auspices of International Association of Meteorology and Atmospheric Physics International Radiation Commission, 45 scientists from five nations convened to discuss relevant issues associated with the measurement, properties, and effects of stratospheric aerosols. A summary is presented of the discussions on formation and evolution, transport and fate, effects on climate, role in heterogeneous chemistry, and validation of lidar and satellite remote sensing of stratospheric aerosols. Measurements are recommended of the natural (background) and the volcanically enhanced aerosol (sulfuric acid and silica particles), the exhaust of shuttle, civil aviation and supersonic aircraft operations (alumina, soot, and ice particles), and polar stratospheric clouds (ice, condensed nitric and hydrochloric acids).

Pueschel, Rudolf F.↗

NASA NTRS2000

Introduction to the SONEX (Subsonic Assessment Ozone and Nitrogen Oxides Experiment) and POLINAT-2 (Pollution from Aircraft Emissions in the North Atlantic Flight Corridor) Special Issue

Emissions of atmospheric species from the engines of subsonic aircraft at cruise altitude (roughly, above seven kilometers) are of concern to scientists, the aviation industry and policymakers for two reasons. First, water vapor, soot and sulfur oxides, and related heterogeneous processes, may modify clouds and aerosols enough to perturb radiative forcing in the UT/LS (upper troposphere/lower stratosphere). A discussion of these phenomena appears in Chapter 3 of the IPCC Aviation Assessment (1999). An airborne campaign conducted to evaluate aviation effects on contrail, cirrus and cloud formation, is described in Geophysical Research Letters. The second concern arises from subsonic aircraft emissions of nitrogen oxides (NO + NO2 = NO(sub x)), CO, and hydrocarbons. These species may add to the background mixture of photochemically reactive species that form ozone. In the UT/LS, ozone is a highly effective greenhouse gas. The impacts of subsonic aircraft emissions on tropospheric NO(sub x) and ozone budgets have been studied with models that focus on UT chemistry [e.g. see discussions of individual models in Brasseur et al., 1998; Friedl et al., 1997; IPCC, 1999]. Depending on the model used, projected increases in the global subsonic aircraft fleet from 1992 to 2015 will lead to a 50-100 pptv increase in UT/LS NO. at 12 km (compared to 50-150 pptv background) in northern hemisphere midlatitudes. The corresponding 12-km ozone increase is 7-11 ppbv, or 5-10% (Chapter 4 in IPCC, 1999). Two major sources of uncertainties in model estimates of aviation effects are: (1) the often limited degree to which global models - the scale required to evaluate aircraft emissions - realistically simulate atmospheric transport and other physical processes; (2) limited UT/LS observations of trace gases with which to evaluate model performance. In response to the latter deficiency, a number of airborne campaigns aimed at elucidating the effect of aircraft on atmospheric nitrogen oxides and ozone were performed between 1990 and 1996 (see descriptions in Friedl et al., 1997; Brasseur et al., 1998).

Thompson, Anne M.↗

NASA NTRS2003

Optical and Probe Diagnostics Applied to Reacting Flows

We plan to explore three major threads during the fellowship period. The first interrogates the flame synthesis of carbon nanotubes using aerosol catalysts. Laser light scattering will reveal changes in particle size at various heights above the burner. Analysis of the flame gas by mass spectroscopy will reveal the chemical composition of the mixture. Finally, absorption measurements will map the nanotube concentration within the flow. The second thread explores soot oxidation kinetics. Cavity ring-down absorption measurements of the carbonaceous aerosol can provide a measure of the mass concentration with time and, hence, an oxidation rate. Spectroscopic and direct probe measurements will provide the temperature of the system needed for subsequent modeling. The third thread will explore the details of turbulent flame dynamics. Laser induced incandescence will be applied to measurements of soot volume fraction in a 2-d configuration. Analysis of seed tracer particles by planar laser light MIE scattering will reveal the elemental fuel mixture fraction in the flames. Cavity ring-down spectroscopy, a pulsed transient absorption method, will determine the instantaneous mass loading and its fluctuation. Finally, fluorescence measurements will investigate the formation of PAH's in these flames.

Ticich, Thomas M.↗

NASA NTRS2001

Experimental Assessment of the Emissions Control Potential of a Rich/Quench/Lean Combustor for High Speed Civil Transport Aircraft Engines

In support of Pratt & Whitney efforts to define the Rich burn/Quick mix/Lean burn (RQL) combustor for the High Speed Civil Transport (HSCT) aircraft engine, UTRC conducted a flametube-scale study of the RQL concept. Extensive combustor testing was performed at the Supersonic Cruise (SSC) condition of a HSCT engine cycle, Data obtained from probe traverses near the exit of the mixing section confirmed that the mixing section was the critical component in controlling combustor emissions. Circular-hole configurations, which produced rapidly-, highly-penetrating jets, were most effective in limiting NOx. The spatial profiles of NOx and CO at the mixer exit were not directly interpretable using a simple flow model based on jet penetration, and a greater understanding of the flow and chemical processes in this section are required to optimize it. Neither the rich-combustor equivalence ratio nor its residence time was a direct contributor to the exit NOx. Based on this study, it was also concluded that (1) While NOx formation in both the mixing section and the lean combustor contribute to the overall emission, the NOx formation in the mixing section dominates. The gas composition exiting the rich combustor can be reasonably represented by the equilibrium composition corresponding to the rich combustor operating condition. Negligible NOx exits the rich combustor. (2) At the SSC condition, the oxidation processes occurring in the mixing section consume 99 percent of the CO exiting the rich combustor. Soot formed in the rich combustor is also highly oxidized, with combustor exit SAE Smoke Number <3. (3) Mixing section configurations which demonstrated enhanced emissions control at SSC also performed better at part-power conditions. Data from mixer exit traverses reflected the expected mixing behavior for off-design jet to crossflow momentum-flux ratios. (4) Low power operating conditions require that the RQL combustor operate as a lean-lean combustor to achieve low CO and high efficiency. (5) A RQL combustor can achieve the emissions goal of EINOX = 5 at the Supersonic Cruise operating condition for a HSCT engine.

Rosfjord, T. J.↗

NASA NTRS2001

Experimental Assessment of the Emissions Control Potential of a Rich/Quench/ Lean Combustor for High Speed Civil Transport Aircraft Engines

In support of Pratt & Whitney efforts to define the Rich burn/Quick mix/Lean burn (RQL) combustor for the High Speed Civil Transport (HSCT) aircraft engine, UTRC conducted a flametube-scale study of the RQL concept. Extensive combustor testing was performed at the Supersonic Cruise (SSC) condition of an HSCT engine cycle. Data obtained from probe traverses near the exit of the mixing section confirmed that the mixing section was the critical component in controlling combustor emissions. Circular-hole configurations, which produced rapidly-, highly-penetrating jets, were most effective in limiting NO(x). The spatial profiles of NO(x) and CO at the mixer exit were not directly interpretable using a simple flow model based on jet penetration, and a greater understanding of the flow and chemical processes in this section are required to optimize it. Neither the rich-combustor equivalence ratio nor its residence time was a direct contributor to the exit NO(x). Based on this study, it was also concluded that: (1) While NO(x) formation in both the mixing section and the lean combustor contribute to the overall emission, the NOx formation in the mixing section dominates. The gas composition exiting the rich combustor can be reasonably represented by the equilibrium composition corresponding to the rich combustor operating condition. Negligible NO(x) exits the rich combustor. (2) At the SSC condition, the oxidation processes occurring in the mixing section consume 99 percent of the CO exiting the rich combustor. Soot formed in the rich combustor is also highly oxidized, with combustor exit SAE Smoke Number <3. (3) Mixing section configurations which demonstrated enhanced emissions control at SSC also performed better at part-power conditions. Data from mixer exit traverses reflected the expected mixing behavior for off-design jet to crossflow momentum-flux ratios. (4) Low power operating conditions require that the RQL combustor operate as a lean-lean combustor to achieve low CO and high efficiency. (5) An RQL combustor can achieve the emissions goal of EINO(x) = 5 at the Supersonic Cruise operating condition for an HSCT engine.

Tacina, Robert R.↗

NASA NTRS2016

Spacecraft Fire Safety Research at NASA Glenn Research Center

Appropriate design of fire detection systems requires knowledge of both the expected fire signature and the background aerosol levels. Terrestrial fire detection systems have been developed based on extensive study of terrestrial fires. Unfortunately there is no corresponding data set for spacecraft fires and consequently the fire detectors in current spacecraft were developed based upon terrestrial designs. In low gravity, buoyant flow is negligible which causes particles to concentrate at the smoke source, increasing their residence time, and increasing the transport time to smoke detectors. Microgravity fires have significantly different structure than those in 1-g which can change the formation history of the smoke particles. Finally the materials used in spacecraft are different from typical terrestrial environments where smoke properties have been evaluated. It is critically important to detect a fire in its early phase before a flame is established, given the fixed volume of air on any spacecraft. Consequently, the primary target for spacecraft fire detection is pyrolysis products rather than soot. Experimental investigations have been performed at three different NASA facilities which characterize smoke aerosols from overheating common spacecraft materials. The earliest effort consists of aerosol measurements in low gravity, called the Smoke Aerosol Measurement Experiment (SAME), and subsequent ground-based testing of SAME smoke in 55-gallon drums with an aerosol reference instrument. Another set of experiments were performed at NASAs Johnson Space Center White Sands Test Facility (WSTF), with additional fuels and an alternate smoke production method. Measurements of these smoke products include mass and number concentration, and a thermal precipitator was designed for this investigation to capture particles for microscopic analysis. The final experiments presented are from NASAs Gases and Aerosols from Smoldering Polymers (GASP) Laboratory, with selected results focusing on realistic fuel preparations and heating profiles with regards to early detection of smoke. SAFFIRE is the upcoming large-scale fire experiment which will be executed in a Cygnus vehicle after it undocks from the ISS.

Aerosol↗

NASA NTRS2005

Influence of the Gas Pressure on Single-wall Carbon Nanotubes Formation

Experiments and modeling have been performed to predict the effect of gas pressure on species distribution and nanotube growth rate under specific conditions of synthesis of singlewall carbon nanotubes (SWCNTs) by arc discharge. Numerical results were compared with experiments in order to find a consistent correlation between the nanotube growth and the pressure. We used argon and helium as buffer gases with a total pressure varied between 0.1 and 1 bar. We experimentally observed that both the anode erosion rate and the Brunauer-Emmett-Teller (BET) surface area of the as produced nanotube soot material are very sensitive to the total gas pressure in the reactor

Hinkov, I.↗