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NASA NTRS1987

Pretreatment of Platinum/Tin Oxide-Catalyst

Addition of CO to He pretreatment doubles catalytic activity. In sealed, high-energy, pulsed CO2 laser, CO and O2 form as decomposition products of CO2 in laser discharge zone. Products must be recombined, because oxygen concentration of more than few tenths of percent causes rapid deterioration of power, ending in unstable operation. Promising low-temperature catalyst for combining CO and O2 is platinum on tin oxide. New development increases activity of catalyst so less needed for recombination process.

Hess, Robert V.↗

NASA NTRS1987

Characterization of the LTC catalyst: Performance against common air pollutants

One of the important qualities of the Low-Temperature Catalyst (LTC) is the rapid oxidation of carbon monoxide to carbon dioxide under a wide variety of conditions. The catalytic material is a palladium-copper activated complex which reacts with various contaminant molecules through a continuous oxidation/reduction cycle. The alumina substrate enhances LTC activity with its favorable surface chemistry and very high surface area. About 10 percent surface water is necessary to facilitate the oxidation of CO. This reaction shows a log-log dependence on contact time, suggesting a Langmuir-Hinshelwood mechanism. In the tube tests, LTC removed 90 to 100 percent of contaminating carbon monoxide in the temperature region of 20 to 4000 C, and at ambient over a range of 25 to 65 percent relative humidity. In contrast, NO2 is chemisorbed by the LTC/alumina material--the amount strongly dependent on temperature increases but independent of humidity. The LTC catalyst has demonstrated excellent capability to remove an important variety of hazardous pollutant gases which are common factors to poor indoor air quality. The Instapure Air Filtration System incorporates the LTC catalyst in a 50:50 mixture with activated carbon to effectively remove particulate, odors, and hazardous gases at room temperature and humidities. The ability to remove hazardous gases is unique for the category of portable air filtration equipment. The wide variety of pollutant gases that LTC removes suggests that catalytic technology is adaptable to a considerable range of commercial and industrial applications.

Collins, Marcia F.↗

NASA NTRS1990

Characterization of the surfaces of platinum/tin oxide based catalysts by Fourier Transform Infrared Spectroscopy (FTIR)

A Pt/SnO2 catalyst has been developed at NASA Langley that is effective for the oxidation of CO at room temperature (1). A mechanism has been proposed to explain the effectiveness of this catalyst (2), but most of the species involved in this mechanism have not been observed under actual catalytic conditions. A number of these species are potentially detectable by Fourier Transform Infrared Spectroscopy (FTIR), e.g., HOSnO sub x, HO sub y PtO sub z, Pt-CO, and SnHCO3. Therefore a preliminary investigation was conducted to determine what might be learned about this particular catalyst by transmission FTIR. The main advantage of FTIR for this work is that the catalyst can be examined under conditions similar to the actual catalytic conditions. This can be of critical importance since some surface species may exist only when the reaction gases are present. Another advantage of the infrared approach is that since vibrations are probed, subtle chemical details may be obtained. The main disadvantage of this approach is that FTIR is not nearly as sensitive as the Ultra High Vacuum (UHV) surface analytical techniques such as Auger, Electron Spectroscopy for Chemical Analysis (ESCA), Electron Energy Loss Spectroscopy (EELS), etc. Another problem is that the assignment of the observed infrared bands may be difficult.

Keiser, Joseph T.↗

NASA NTRS1993

Asymptotic analysis for the burning of n-heptane droplets using a four-step reduced mechanism

A four-step reduced mechanism is obtained from a minimal chemical-kinetic description, where the effects of the elementary rates are treated as parameters in the expressions for the global rates. This mechanism is used to analyze the extinction characteristics of a single n-heptane droplet burning under quasi-steady, spherically symmetrical conditions. The reaction layer consists of a merged inner zone, on the fuel-rich side of the flame, where fuel and H atoms are consumed thereby producing H2 and CO along with H2O and CO2, and an oxygen-consumption zone, on the fuel-lean side, where H2 and CO are oxidized to produce additional H2O and CO2 along with H radicals. For the inner zone, a parameter mu is identified which describes the ratio of the thickness of a fuel-consumption layer to that of an H-recombination layer. Analytical solutions for the rate of scalar dissipation at extinction are obtained in the limiting cases of mu tending to 0 and mu tending to infinity. From the results of the analysis, extinction diameters for n-heptane droplets are estimated for different pressures and ambient oxygen concentrations.

Card, J. M.↗

NASA NTRS1993

Remote sounding of tropospheric minor constituents

The etalon interferometer, or Fabry-Perot interferometer (FPI), with its high throughput and high spectral resolution was widely used in the remote-sensing measurements of the earth's atmospheric composition, winds, and temperatures. The most recent satellite instruments include the Fabry-Perot interferometer flown on the Dynamics Explorer-2 (DE-2) and the High Resolution Doppler Imager (HRDI) to be flown on the Upper Atmosphere Research Satellite (UARS). These instruments measure the Doppler line profiles of the emission and absorption of certain atmospheric species (such as atomic oxygen) in the visible spectral region. The successful space flight of DE-FPI and the test and delivery of UARS-HRDI demonstrated the extremely high spectral resolution and ruggedness of the etalon system for the remote sensing of earth and planetary atmospheres. Recently, an innovative FPI focal plane detection technique called the Circle-to-Line Interferometer Optical (CLIO) system was invented at the Space Physics Research Laboratory (SPRL). The CLIO simplifies the FPI focal plane detection process by converting the circular rings or fringes into a linear pattern similar to that produced by a conventional spectrometer, while retaining the throughput advantage of the etalon interferometer. CLIO makes the use of linear array detectors more practical and efficient with FPI, the combination of FPI and CLIO represents a very promising new technique for the remote sensing of the lower atmospheres of Earth, Mars, Venus, Neptune, and other planets. The Multiorder Etalon Spectrometer (MOES), as a combination of the rugged etalon and the CLIO, compares very favorably to other spaceborne optical instruments in terms of performance versus complexity. The feasibility of an advanced etalon spectrometer for the remote sensing of tropospheric trace species, particularly carbon monoxide (CO), nitrous oxide (N2O), and methane (CH4) was discussed. The etalon atmospheric spectroscopy techniques are described, instrument design and related technical issues are discussed. The primary objective is to establish the concept of atmospheric spectroscopy with the CLIO and etalon system and its applications for the measurements of tropospheric trace species analyze system requirements and performance, determine the feasibility of components and subsystem implementation with available technology, and develop inversion algorithm for retrieval simulation and data analysis.

Drayson, S. Roland↗

NASA NTRS1994

The radiocarbon hydroxyl technique

The Radiocarbon Technique depends upon measuring the rate of oxidation of CO in an essentially unperturbed sample of air. The airborne technique is slightly different. Hydroxyl concentrations can be calculated directly; peroxyl concentrations can be obtained by NO doping.

Campbell, Malcolm J.↗

NASA NTRS1996

Designing Ni- and Co-Base Superalloys To Resist Oxidation

Analysis of experimental cyclic-oxidation data yields quantitative design criterion. Equation characterizing abilities of superalloys to resist oxidation at high temperatures proves useful for designing new alloy compositions to resist oxidation. Rates tendency to become oxidized in terms of single attack parameter, K(a), as function of composition and temperature: decrease in K(a) signifies increase in resistance to oxidation.

Barrett, Charles A.↗

NASA NTRS2001

An Investigation of Fully Modulated, Turbulent Diffusion Flames in Reduced Gravity

Pulsed combustion appears to have the potential to provide for rapid fuel/air mixing, compact and economical combustors, and reduced exhaust emissions. The objective of this Flight-Definition experiment (PuFF, for Pulsed-Fully Flames) is to increase the fundamental understanding of the fuel/air mixing and combustion behavior of pulsed, turbulent diffusion flames by conducting experiments in microgravity. In this research the fuel jet is fully modulated (i.e., completely shut off between pulses) by an externally controlled valve system. This gives rise to drastic modification of the combustion and flow characteristics of flames, leading to enhanced fuel/air mixing mechanisms not operative for the case of acoustically excited or partially-modulated jets. The fully-modulated injection approach also simplifies the combustion process by avoiding the acoustic forcing generally present in pulsed combustors. Relatively little is known about the behavior of turbulent flames in reduced-gravity conditions, even in the absence of pulsing. Fundamental issues addressed in this experiment include the impact of buoyancy on the fuel/air mixing and combustion characteristics of fully-modulated flames. It is also important for the planned space experiments to establish the effects of confinement and oxidizer co-flow on these flames.

Hermanson, J. C.↗

NASA NTRS2003

Thermal Characteristics and Structure of Fully-Modulated, Turbulent Diffusion Flames in Microgravity

Turbulent jet diffusion flames are studied in microgravity and normal gravity under fully-modulated conditions for a range of injection times and a 50% duty cycle. Diluted ethylene was injected through a 2-mm nozzle at a Reynolds number of 5,000 into an open duct, with a slow oxidizer co-flow. Microgravity tests are conducted in NASA's 2.2 Second Drop Tower. Flames with short injection times and high duty cycle exhibit a marked increase in the ensemble-averaged flame length due to the removal of buoyancy. The cycle-averaged centerline temperature profile reveals higher temperatures in the microgravity flames, especially at the flame tip where the difference is about 200 K. In addition, the cycle-averaged measurements of flame radiation were about 30% to 60% greater in microgravity than in normal gravity.

Hermanson, J. C.↗

NASA NTRS2004

Buoyancy Effects in Strongly-pulsed, Turbulent Diffusion Flames

The objective of this experiment is to better understand the combustion behavior of pulsed, turbulent diffusion flames by conducting experiments in microgravity. The fuel jet is fully-modulated (i.e., completely shut off between pulses) by an externally controlled valve system leading to enhanced fuel/air mixing compared to acoustically excited or partially-modulated jets. Experiments are conducted both in laboratories at UW and WPI and in the GRC 2.2s Drop Tower. A single fuel nozzle with diameter d = 2 mm is centered in a combustor 20 x 20 cm in cross section and 67 cm in height. The gaseous fuel flow (ethylene or a 50/50 ethylene/nitrogen mixture by volume) is fully-modulated by a fast-response solenoid valve with injection times from tau = 4 to tau = 300 ms. The nominal Reynolds number based on the fuel velocity during injection, U(sub jet), is 5,000. A slow oxidizer co-flow properly ventilates the flame and an electrically heated wire loop serves as a continuous ignition source. Diagnostic techniques include video imaging, fine-wire thermocouples and thermopile radiometers, and gas sampling and standard emissions instruments (the last in the laboratory only).

Hermanson, J. C.↗

NASA NTRS2004

Buoyancy Effects in Strongly-Pulsed, Turbulent Diffusion Flames

The objective of this experiment is to better understand the combustion behavior of pulsed, turbulent diffusion flames by conducting experiments in microgravity. The fuel jet is fully-modulated (i.e., completely shut off between pulses) by an externally controlled valve system leading to enhanced fuel/air mixing compared to acoustically excited or partially-modulated jets. Experiments are conducted both in laboratories at UW and WPI and in the GRC 2.2s Drop Tower. A single fuel nozzle with diameter d = 2 mm is centered in a combustor 20 20 cm in cross section and 67 cm in height. The gaseous fuel flow (ethylene or a 50/50 ethylene/nitrogen mixture by volume) is fully-modulated by a fast-response solenoid valve with injection times from tau = 4 to tau = 300 ms. The nominal Reynolds number based on the fuel velocity during injection, U(sub jet), is 5,000. A slow oxidizer co-flow properly ventilates the flame and an electrically heated wire loop serves as a continuous ignition source. Diagnostic techniques include video imaging, fine-wire thermocouples and thermopile radiometers, and gas sampling and standard emissions instruments (the last in the laboratory only).

Hermanson, J. C.↗

NASA NTRS2007

Transport in the Subtropical Lowermost Stratosphere during CRYSTAL-FACE

We use in situ measurements of water vapor (H2O), ozone (O3), carbon dioxide (CO2), carbon monoxide (CO), nitric oxide (NO), and total reactive nitrogen (NO(y)) obtained during the CRYSTAL-FACE campaign in July 2002 to study summertime transport in the subtropical lowermost stratosphere. We use an objective methodology to distinguish the latitudinal origin of the sampled air masses despite the influence of convection, and we calculate backward trajectories to elucidate their recent geographical history. The methodology consists of exploring the statistical behavior of the data by performing multivariate clustering and agglomerative hierarchical clustering calculations, and projecting cluster groups onto principal component space to identify air masses of like composition and hence presumed origin. The statistically derived cluster groups are then examined in physical space using tracer-tracer correlation plots. Interpretation of the principal component analysis suggests that the variability in the data is accounted for primarily by the mean age of air in the stratosphere, followed by the age of the convective influence, and lastly by the extent of convective influence, potentially related to the latitude of convective injection [Dessler and Sherwuud, 2004]. We find that high-latitude stratospheric air is the dominant source region during the beginning of the campaign while tropical air is the dominant source region during the rest of the campaign. Influence of convection from both local and non-local events is frequently observed. The identification of air mass origin is confirmed with backward trajectories, and the behavior of the trajectories is associated with the North American monsoon circulation.

Pittman, Jasna V.↗

NASA NTRS2007

Transport in the Subtropical Lowermost Stratosphere during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment

We use in situ measurements of water vapor (H2O), ozone (O3), carbon dioxide (CO2), carbon monoxide (CO), nitric oxide (NO), and total reactive nitrogen (NOy) obtained during the CRYSTAL-FACE campaign in July 2002 to study summertime transport in the subtropical lowermost stratosphere. We use an objective methodology to distinguish the latitudinal origin of the sampled air masses despite the influence of convection, and we calculate backward trajectories to elucidate their recent geographical history. The methodology consists of exploring the statistical behavior of the data by performing multivariate clustering and agglomerative hierarchical clustering calculations and projecting cluster groups onto principal component space to identify air masses of like composition and hence presumed origin. The statistically derived cluster groups are then examined in physical space using tracer-tracer correlation plots. Interpretation of the principal component analysis suggests that the variability in the data is accounted for primarily by the mean age of air in the stratosphere, followed by the age of the convective influence, and last by the extent of convective influence, potentially related to the latitude of convective injection (Dessler and Sherwood, 2004). We find that high-latitude stratospheric air is the dominant source region during the beginning of the campaign while tropical air is the dominant source region during the rest of the campaign. Influence of convection from both local and nonlocal events is frequently observed. The identification of air mass origin is confirmed with backward trajectories, and the behavior of the trajectories is associated with the North American monsoon circulation.

Pittman, Jasna V.↗

NASA NTRS2012

Photoacoustic Optical Properties at UV, VIS, and near IR Wavelengths for Laboratory Generated and Winter Time Ambient Urban Aerosols

We present the laboratory and ambient photoacoustic (PA) measurement of aerosol light absorption coefficients at ultraviolet wavelength (i.e., 355 nm) and compare with measurements at 405, 532, 870, and 1047 nm. Simultaneous measurements of aerosol light scattering coefficients were achieved by the integrating reciprocal nephelometer within the PA's acoustic resonator. Absorption and scattering measurements were carried out for various laboratory generated aerosols, including salt, incense, and kerosene soot to evaluate the instrument calibration and gain insight on the spectral dependence of aerosol light absorption and scattering. Ambient measurements were obtained in Reno, Nevada, between 18 December 2009 and 18 January 2010. The measurement period included days with and without strong ground level temperature inversions, corresponding to highly polluted (freshly emitted aerosols) and relatively clean (aged aerosols) conditions. Particulate matter (PM) concentrations were measured and analyzed with other tracers of traffic emissions. The temperature inversion episodes caused very high concentration of PM (sub 2.5) and PM( sub 10) (particulate matter with aerodynamic diameters less than 2.5 micrometers and 10 micrometers, respectively) and gaseous pollutants: carbon monoxide (CO), nitric oxide (NO), and nitrogen dioxide (NO2). The diurnal change of absorption and scattering coefficients during the polluted (inversion) days increased approximately by a factor of two for all wavelengths compared to the clean days. The spectral variation in aerosol absorption coefficients indicated a significant amount of absorbing aerosol from traffic emissions and residential wood burning. The analysis of single scattering albedo (SSA), Angstrom exponent of absorption (AEA), and Angstrom exponent of scattering (AES) for clean and polluted days provides evidences that the aerosol aging and coating process is suppressed by strong temperature inversion under cloudy conditions. In general, measured UV absorption coefficients were found to be much larger for biomass burning aerosol than for typical ambient aerosols.

absorptivity↗

NASA NTRS2019

Earth's Early Reduced Atmospheres

Earth’s early atmosphere evolved in response to cosmic impacts, photochemistry generated by the copious extreme ultraviolet radiation emitted by the young Sun, hydrogen escape, mineral redox buffering, the evolution of iron in the mantle, and the character of crustal weathering and subduction. No single chemical composition, surface pressure, or temperature was typical. After the biggest impacts the temperature likely rose above 3000 K and the atmosphere held rock vapor. As the atmosphere cooled its constituents rained out: first the silicates, then the geochemical volatiles (such as salt), and last the water. Depending on the size of the impact, cooling took thousands to millions of years. Between impacts the atmosphere was thick with gases like CO2, H2, and CH4 that do not condense at Earth but provide greenhouse warming that could easily have maintained surface temperatures in excess of 500 K. At some point the early atmosphere must have been conducive to the evolution of organic chemistry and the origin of life. It was therefore --- at times --- dominated by reduced gases like hydrogen and methane. Hydrogen-methane atmospheres are easily formed thermochemically after major impacts if H2O and CO2 were present on Earth in quantities consistent with their inventories on Earth today – the key is high pressure. Hydrogen-methane atmospheres slowly break down over millions of years by hydrogen escape and photochemistry. At first methane decomposes into tars and nitriles that precipitate, but later as the atmosphere grows more oxidized from hydrogen escape the methane oxidizes to CO and CO2, with a small fraction going to HCN. Impacts can also produce NH3 directly from N2 and H2O, which is expected to rain out with the H2O. As impacts grew infrequent the climate cooled in response to the fixing of CO2 as carbonate and carbonate subduction. Eventually the CO2 was mostly removed to the mantle and the surface mostly frozen.

Zahnle, Kevin↗

NASA NTRS2006

Partitioning of Ni, Co and V between Spinel-Structured Oxides and Silicate Melts: Importance of Spinel Composition

Partitioning of Ni, Co and V between Cr-rich spinels and basaltic melt has been studied experimentally between 1150 and 1325 C, and at controlled oxygen fugacity from the Co-CoO buffer to slightly above the hematite magnetite buffer. These new results, together with new Ni, Co and V analyses of experimental run products from Leeman [Leeman, W.P., 1974. Experimental determination of the partitioning of divalent cations between olivine and basaltic liquid, Pt. II. PhD thesis, Univ. Oregon, 231 - 337.], show that experimentally determined spinel melt partition coefficients (D) are dependent upon temperature (T), oxygen fugacity (fO2) and spinel composition. In particular, partition coefficients determined on doped systems are higher than those in natural (undoped) systems, perhaps due to changing activity coefficients over the composition range defined by the experimental data. Using our new results and published runs (n =85), we obtain a multilinear regression equation that predicts experimental D(V) values as a function of T, fO2, concentration of V in melt and spinel composition. This equation allows prediction of D(V) spinel/melt values for natural mafic liquids at relevant crystallization conditions. Similarly, D(Ni) and D(Co) values can be inferred from our experiments at redox conditions approaching the QFM buffer, temperatures of 1150 to 1250 C and spinel composition (early Cr-bearing and later Ti-magnetite) appropriate for basic magma differentiation. When coupled with major element modelling of liquid lines of descent, these values (D(Ni) sp/melt=10 and D(Co) sp/melt=5) closely reproduce the compositional variation observed in komatiite, mid-ocean ridge basalt (MORB), ocean island basalt (OIB) and basalt to rhyolite suites.

Righter, K.↗

NASA NTRS2009

The Active Oxidation of Silicon Carbide

The high temperature oxidation of silicon carbide occurs in two very different modes. Passive oxidation forms a protective oxide film which limits further attack of the SiC: SiC(s) + 3/2 O2(g) = SiO2(s) + CO(g) Active oxidation forms a volatile oxide and may lead to extensive attack of the SiC: SiC(s) + O2(g) = SiO(g) + CO(g) Generally passive oxidation occurs at higher oxidant pressures and active oxidation occurs at lower oxidant pressures and elevated temperatures. Active oxidation is a concern for reentry, where the flight trajectory involves the latter conditions. Thus the transition points and rates of active oxidation are a major concern. Passive/active transitions have been studied by a number of investigators. An examination of the literature indicates many questions remain regarding the effect of impurity, the hysteresis of the transition (i.e. the difference between active-to-passive and passive-toactive), and the effect of total pressure. In this study we systematically investigate each of these effects. Experiments were done in both an alumina furnace tube and a quartz furnace tube. It is known that alumina tubes release impurities such as sodium and increase the kinetics in the passive region [1]. We have observed that the active-to-passive transition occurs at a lower oxygen pressure when the experiment is conducted in alumina tubes and the resultant passive silica scale contains sodium. Thus the tests in this study are conducted in quartz tubes. The hysteresis of the transition has been discussed in the detail in the original theoretical treatise of this problem for pure silicon by Wagner [2], yet there is little mention of it in subsequent literature. Essentially Wagner points out that the active-to-passive transition is governed by the criterion for a stable Si/SiO2 equilibria and the passive-to-active transition is governed by the decomposition of the SiO2 film. A series of experiments were conducted for active-to-passive and passive-to-active transitions by increasing and decreasing oxygen pressure, respectively. For pure silicon a dramatic difference was found; whereas for SiC the difference was not as great. This may be due to the oxidation of the carbon in SiC which may break down the scale [3]. The third area is the effect of total pressure. In the literature, low oxygen potentials are achieved via either low total pressure or low oxygen pressure in an O2/Ar mixture. Both types of experiments are done in this study and the differences are discussed with regard to the presence or absence of a boundary layer.

Jacobson, Nathan S.↗

NASA NTRS1978

Interactions of simultaneous perturbations of stratospheric photochemistry

The combined effects of two specific ozone perturbation mechanisms are examined. The need to look back to predictions of the near past as well as the future as a means of testing model results is emphasized. The two perturbations examined are that due to chlorofluoromethane (CFM) release and that due to the air pollutants CO and nitrogen oxide. A steady-state model is used to investigate the characteristics of the stratospheric-tropospheric photochemical system for differing levels of CO and nitrogen oxide fluxes at the ground and for simultaneously changing the stratospheric from CFM release. Two basic scenarios chosen to illustrate the competing effects of the two types of perturbation use the time-dependence for chlorine radical buildup calculated for constant continued release of CFM's.

Butler, D. M.↗