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NASA NTRS1984

Abiotic synthesis of purines and other heterocyclic compounds by the action of electrical discharges

The synthesis of purines and pyrimidines using Oparin-Urey-type primitive earth atmospheres has been demonstrated by reacting methane, ethane, and ammonia in electrical discharges. Adenine, guaine, 4-aminoimidazole-5-carboxamide (AICA), and isocytosine have been identified by UV spectrometry and paper chromatography as the products of the reaction. The total yields of the identified heterocyclic compounds are 0.0023 percent. It is concluded that adenine synthesis occurs at a much lower concentration of hydrogen cyanide than has been shown by earlier studies. Pathways for the synthesis of purines from hydrogen cyanide are discussed, and a comparison of the heterocyclic compounds that have been identified in meteorites and in prebiotic reactions is presented.

Yuasa, S.↗

NASA NTRS1986

Spontaneous ignition delay characteristics of hydrocarbon fuel-air mixtures

The influence of pressure on the autoignition characteristics of homogeneous mixtures of hydrocarbon fuels in air is examined. Autoignition delay times are measured for propane, ethylene, methane, and acetylene in a continuous flow apparatus featuring a multi-point fuel injector. Results are presented for mixture temperatures from 670K to 1020K, pressures from 1 to 10 atmospheres, equivalence ratios from 0.2 to 0.7, and velocities from 5 to 30 m/s. Delay time is related to pressure, temperature, and fuel concentration by global reaction theory. The results show variations in global activation energy from 25 to 38 kcal/kg-mol, pressure exponents from 0.66 to 1.21, and fuel concentration exponents from 0.19 to 0.75 for the fuels studied. These results are generally in good agreement with previous studies carried out under similar conditions.

Lefebvre, A. H.↗

NASA NTRS1977

Prediction of hydrodynamics and chemistry of confined turbulent methane-air flames with attention to formation of oxides of nitrogen

A formulation of the governing partial differential equations for fluid flow and reacting chemical species in a tubular combustor is presented. A numerical procedure for the solution of the governing differential equations is described, and models for chemical equilibrium and chemical kinetics calculations are presented. The chemical equilibrium model is used to characterize the hydrocarbon reactions. The chemical kinetics model is used to predict the concentrations of the oxides of nitrogen. The combustor consists of a cylindrical duct of varying cross sections with concentric streams of gaseous fuel and air entering the duct at one end. Four sample cases with specified inlet and boundary conditions are considered, and the results are discussed

Elghobashi, S.↗

NASA NTRS1992

Micrometeorological measurements of CH4 and CO2 exchange between the atmosphere and subarctic tundra

Eddy correlation flux measurements and concentration profiles of total hydrocarbons (THC) and CO2 were combined to provide a comprehensive record of atmosphere-biosphere exchange for these gases over a 30-day period in July-August 1988 in the Yukon-Kuskokwin River Delta of Alaska. Over 90 percent of net ecosystem exchanges of THC were due to methane. Lakes and wet meadow tundra provided the major sources of methane. The average fluxes from lake, dry tundra, and wet tundra were 11 +/- 3, 29 +/- 3, and 57 +/- 6 mg CH4/sq m/d, respectively. The mean remission rate for the site was 25 mg/sq m/d. Maximum uptake of CO2 by the tundra was 1.4 gC/sq m/d between 1000 and 1500 hrs, and nocturnal respiration averaged 0.73 gC/sq m/d. Net uptake of CO2 was 0.30 gC/sq m/d for the 30 days of measurement; methane flux accounted for 6 percent of CO2 net uptake.

Fan, S. M.↗

NASA NTRS2003

STS-113/11A: Assessment of Air Quality in the International Space Station (ISS) and Space Shuttle Based on Samples Returned in December 2002 and in May 2003 aboard Soyuz 5

The toxicological assessments of grab sample canisters (GSCs) returned aboard STS-l13 and Soyuz 5 are reported. Analytical methods have not changed from earlier reports. Surrogate standard recoveries from the GSCs were 79-120% except as noted in the table. One sample was returned with the valve opened. The two general criteria used to assess air quality are the total-non-methane-volatile organic hydrocarbons (NMVOCs) and the total T-value (minus the CO2 and formaldehyde contributions). Control of atmospheric alcohols is important to the water recovery system engineers, hence total alcohols (including acetone) are also shown for each sample. Octafluoropropane (OFP) has leaked from heat-exchange units in large quantities, so its concentration is tracked separately. Because formaldehyde is quantified from sorbent badges, its concentration is also listed separately. The table shows that the air quality in general was acceptable for crew respiration through the middle of December 2002. No conclusions can be made about the air quality after that date due to NASA's inability to return air samples from the ISS . Alcohols are not being controlled to the recently lowered guideline of 5 mg/m3, which was recommended to protect the water recovery systems. The airlock sample was taken during the regeneration of Met ox canisters in the adjacent Node. The trace pollutants were not increased above background; however, inspection of table 1 in the appendix shows a CO2 concentration of 17,000 mg/cu m, which is a relatively high concentration, but still below the 24-hour SMAC of23,000 mg/cu m. The control of OFP continues to be adequate at least through December 2002. Formaldehyde concentrations suggest that the high levels that were being found in the Lab atmosphere have subsided. This is probably attributable to the restoration of IMV in early February 2003 . Before the obstructing material was removed from ducts the Lab formaldehyde concentrations approached 0.06 mg/cu m, whereas after the repair the levels were near 0.04 mg/m3 . This does not mean that local sources in the Lab have been reduced, only that the excess of formaldehyde produced in the Lab is distributed into the whole volume of the ISS.

James, John T.↗

NASA NTRS2015

Active and Widespread Halogen Chemistry in the Tropical and Subtropical Free Troposphere

Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10degN to 40degS), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (approx.3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.

Wang, Siyuan↗

NASA NTRS1982

Molecular-beam sampling study of extinguishment of methane-air flames by dry chemicals

The use of Al2O3, NaHCO3, KHCO3, NH4H2PO4 and KCl powders for the inhibition of a methane/oxygen diffusion flame is studied through measurement of composition and temperature profiles, using a molecular beam mass spectrometer sampling system. In order to obtain significant inhibition without extinguishing the flame, a powder feeding rate of 2 mg/liter of gas was used for KCl and Al2O3, and of 3 mg/liter of gas for the remaining powders. CH4, O2, N2, H2O and CO2 concentrations were measured by the mass spectrometer, while temperature was measured by the time-of-flight technique. For the powder feeding rates used, Al2O3 was the least and KCl and NH2H4PO2 the most effective in reducing temperature; in reaction-inhibition effectiveness, Al2O3 was again lowest while KCl was superior to all others. Because the KCl concentration was only 2/3 that of NH4H2PO4, it is recommended as the most effective temperature reducer and reaction inhibitor.

Knuth, E. L.↗

NASA NTRS1983

Photolysis of methane and the ionosphere of Uranus

Photochemical calculations for Uranus predict an extensive region of condensation of acetylene, ethane and methane in the vicinity of the temperature inversion layer. This could explain why ethane was not detected on Uranus, unlike Neptune which has a much warmer inversion layer. Subsequent snow-out of the condensibles is expected to result in reduced visibility in the troposphere. Ionospheric calculations for the equatorial region to be probed by Voyager, indicate peak electron concentrations on the order of 5,000 per cu cm, if dynamical effects are important. Upper limit to the electron peak is 30,000 per cu cm. Exospheric temperatures as high as 200-250K are conceivable.

Atreya, S. K.↗

NASA NTRSDate not supplied

Analysis of Volatile Compounds from CO2 Removal Systems

One of the primary concerns when designing CO2 scrubber systems that will be integrated with a Sabatier reactor to produce water and methane is the amount of water released from the scrubber. Because the gas stream entering a Sabatier reactor must be compressed, water entering the reactor can condense and compromise the integrity of the system, thus rendering its valuable conversion capability useless. When the Johnson Space Center Environmental Chemistry Laboratory was tasked to develop an assay to quantify the water concentration in air samples from CO2 scrubbers, additional testing was also performed to see if any other compounds were being concentrated on the scrubbers. It was thought that the efficiency of the scrubber systems could be quantified by comparing the differences in samples from the ambient air on the International Space Station (ISS) to the exit gas of the scrubber. As this analysis was carried out, it became evident that the concentrations of certain volatile compounds were higher in the samples from the scrubbers than they were in nominal environmental samples. This meant these compounds were being retained and concentrated on the scrubber beds. Based on this finding, concerns were raised about their potential for these compounds to poison the Sabatier reactor. Further investigation was required to identify these compounds due to their high concentrations and unique matrix of the CO2 scrubber exhaust. This paper describes these events as well as the process that was developed to identify the volatile compounds that increased. An examination of how much the certain compounds can be concentrated by the scrubber systems is also included.

Volatiles↗

NASA NTRSDate not supplied

Analysis of Volatile Compounds From CO2 Removal Systems

Volatiles↗

NASA NTRS2001

H2 cycling and microbial bioenergetics in anoxic sediments

The simple biochemistry of H2 is central to a large number of microbial processes, affecting the interaction of organisms with each other and with the environment. In anoxic sediments, the great majority of microbial redox processes involve H2 as a reactant, product, or potential by-product, and the thermodynamics of these processes are thus highly sensitive to fluctuations in environmental H2 concentrations. In turn, H2 concentrations are controlled by the activity of H2-consuming microorganisms, which efficiently utilize this substrate down to levels which correspond to their bioenergetic limitations. Consequently, any environmental change which impacts the thermodynamics of H2-consuming organisms is mirrored by a corresponding change in H2 concentrations. This phenomenon is illustrated in anoxic sediments from Cape Lookout Bight, NC, USA: H2 concentrations are controlled by a suite of environmental parameters (e.g., temperature, sulfate concentrations) in a fashion which can be quantitatively described by a simple thermodynamic model. These findings allow us to calculate the apparent minimum quantity of biologically useful energy in situ. We find that sulfate reducing bacteria are not active at energy yields below -18 kJ per mole sulfate, while methanogenic archaea exhibit a minimum close to -10 kJ per mole methane.

Hoehler, Tori M.↗

NASA NTRS1985

Multiplex gas chromatography for use in space craft

Gas chromatography is a powerful technique for the analysis of gaseous mixtures. Some limitations in this technique still exist which can be alleviated with multiplex gas chromatography (MGC). In MGC, rapid multiple sample injections are made into the column without having to wait for one determination to be finished before taking a new sample. The resulting data must then be reduced using computational methods such as cross correlation. In order to efficiently perform multiplexgas chromatography, experiments in the laboratory and on board future space craft, skills, equipment, and computer software were developed. Three new techniques for modulating, i.e., changing, sample concentrations were demonstrated by using desorption, decomposition, and catalytic modulators. In all of them, the need for a separate gas stream as the carrier was avoided by placing the modulator at the head of the column to directly modulate a sample stream. Finally, the analysis of an environmental sample by multiplex chromatography was accomplished by employing silver oxide to catalytically modulate methane in ambient air.

Valentin, J. R.↗

NASA NTRS1982

Measurements of the global distribution of carbon monoxide in the troposphere

Carbon monoxide and methane grab samples were obtained simultaneously with ozone, aerosol, nitric oxide and DACOM CO measurements. Eighty grab samples were collected at various altitudes up to 19,000 ft. along a north-south flight path from Wallops Flight Center, VA to 11 N. CO and CH were analyzed by flame ionization gas chromatography with cryogenic preconcentration. The relationship between CO and O3 concentrated is examined. A comparative analysis between trends in aerosol and CO concentration is performed.

Hinton, R. R.↗

NASA NTRS1988

Chlorine-hydrocarbon photochemistry in the marine troposphere and lower stratosphere

The role of chlorine atoms in the oxidation of methane and nonmethane hydrocarbons (NMHCs) in the marine troposphere and lower stratosphere was investigated using a one-dimensional photochemical model that incorporated the chemistry of CH4, NMHCs, NO(x), O(x), and HO(x), as well as organic and inorganic halogens in the troposphere and lower stratosphere. The model predicted that chlorine atoms are present in the marine troposphere at the concentrations of about 1000/cu cm, mostly as a product of the reaction between OH and HCl released from sea spray. The results indicate that Cl atoms cause 20 to 40 percent of NMHC oxidation in the troposphere and 40 to 90 percent in the lower stratosphere. At 15 km, the NMHC-Cl reactions account for nearly 80 percent of the PAN produced. Where available, experimental data confirmed the model predictions.

Singh, H. B.↗

NASA NTRS1991

Counterflow diffusion flames of hydrogen, and hydrogen plus methane, ethylene, propane, and silane vs. air - Strain rates at extinction

Five coaxial tubular opposed jet burners (OJBs) with tube diameter D(T) of 1.8-10 mm and 5 mm conical nozzles were used to form dish-shaped counterflow diffusion flames centered by opposing laminar jets of nitrogen and hydrocarbon-diluted H2 versus air in an argon-purged chamber at 1 atm. Area-averaged air jet velocities at blowoff of the central flame, U(air), characterized extinction of the airside flame as functions of input H2 concentration on the fuelside. A master plot of extensive U(air) data at blowoff versus D(T) shows that U(air) varies linearly with D(T). This and other data sets are used to find that nozzle OJB results for U(air)/diameter average 4.24 + or - 0.28 times larger than tubular OJB results for the same fuel compositions. Critical radial velocity gradients consistent with one-dimensional stagnation point boundary theory and with plug flow inputs are estimated. The results compare favorably with published numerical results based only on potential flow.

Pellett, G. L.↗

NASA NTRS2019

Can Organic Haze and O2 Plumes Explain Patterns of Sulfur Mass-Independent Fractionation During the Archean?

The existence of mass-independently fractionated sulfur in Archean rocks is almost universally accepted as evidence for low atmospheric O2 and O3 concentrations at that time. But the detailed patterns of the values and of the ratios / and / remain to be explained, and the mechanism for producing the mass-independent fractionation remains controversial. Here, we explore the hypothesis that the relatively low values seen during the Mid-Archean, 2.7-3.5 Ga, were caused by the presence of organic haze produced from photolysis of methane. This haze helped shield SO2 from photolysis, while at the same time providing surfaces on which unfractionated short-chain sulfur species could condense. The evolution of oxygenic photosynthesis, and the concomitant disappearance of organic haze towards the end of the Archean allowed more negatively fractionated S4 and S8 to form, thereby generating large positive fractionations in other sulfur species, including sulfate and H2S. Reduction of this sulfate to H2S by bacteria, followed by incorporation of H2S into pyrite, produced the large positive values observed in the Neoarchean rock record, 2.5-2.7 Ga.

Great Oxidation Event↗

NASA NTRS1983

A radiative transfer model for surface radiation budget studies

A high resolution spectral radiative transfer model of the troposphere for computing downwelling radiance and flux density at the surface in the 5-200 micron region has been developed. The model is fast and accurate and takes into consideration all major and minor constituents active in this region, namely, water vapor, carbon dioxide, ozone, nitrous oxide, and methane. It uses the quasi-random band model of absorption for computing atmospheric transmittances due to various bands. Continuum absorption by water vapor in the 8-14 micron region has also been taken into account. The model has been used to examine the sensitivity of downwelling flux to variations of surface water vapor pressure (or surface relative humidity), water vapor scale-height and concentrations of other gaseous constituents of the atmosphere. In addition, sensitivity to changes in a number of cloud parameters, namely, fractional cloud cover, cloud height, and high-cloud emissivity, has also been examined. Results obtained with the present model compare well with those from the empirical and semi-empirical correlations. The present work demonstrates, for the first time, the feasibility of using a high-resolution narrow-band model for computing this flux for a meteorological application.

Gupta, S. K.↗

NASA NTRS2002

Assessment of Air Quality in the International Space Station (ISS) and Space Shuttle Based on Samples Returned Aboard STS-110 (ISS-8A) in April 2002

The toxicological assessment of grab sample canisters (GSCs) returned aboard STS-110 is reported. Analytical methods have not changed from earlier reports, and surrogate standard recoveries from the GSCs were 77-121%, with one exception. Pressure tracking indicated no leaks in the canisters. Recoveries from lab and trip controls for formaldehyde analyses ranged from 87 to 96%. The two general criteria used to assess air quality are the total-non-methane-volatile organic hydrocarbons (NMVOCs) and the total T-value (minus the CO2 and formaldehyde contributions). Because of the inertness of Freon 218 (octafluoropropane, OFP), its contribution to the NMVOC is subtracted and tabulated separately. Control of atmospheric alcohols is important to the water recovery system engineers, hence total alcohols are also shown for each sample. Because formaldehyde is quantified from sorbent badges, its concentration is listed separately. These five indices of air quality are summarized.

James, John T.↗