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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
NASA NTRS1975

Evaluation and characterization of the methane-carbon dioxide decomposition reaction

A program was conducted to evaluate and characterize the carbon dioxide-methane (CO2-CH4) decomposition reaction, i.e., CO2 + CH4 = 2C + 2H2O. The primary objective was to determine the feasibility of applying this reaction at low temperatures as a technique for recovering the oxygen (O2) remaining in the CO2 which exits mixed with CH4 from a Sabatier CO2 reduction subsystem (as part of an air revitalization system of a manned spacecraft). A test unit was designed, fabricated, and assembled for characterizing the performance of various catalysts for the reaction and ultraviolet activation of the CH4 and CO2. The reactor included in the test unit was designed to have sufficient capacity to evaluate catalyst charges of up to 76 g (0.17 lb). The test stand contained the necessary instrumentation and controls to obtain the data required to characterize the performance of the catalysts and sensitizers tested: flow control and measurement, temperature control and measurement, product and inlet gas analysis, and pressure measurement. A product assurance program was performed implementing the concepts of quality control and safety into the program effort.

Davenport, R. J.↗
NASA NTRS1975

Photosynthesis of organic compounds in the atmosphere of Jupiter

An efficient conversion of CH4 to hydrocarbons and HCN takes place when NH3 is photolysed in the presence of CH4, H2, and He using a 184.9 nm light source. The extent of NH3 decomposition after a 1 hr exposure was determined spectrophotometrically; CH4, N2, and C2 and C3 hydrocarbons were detected and analyzed by mass spectrometry. Photolysis of one molar equivalent of NH3 results in the loss of 0.84 molar equivalent of CH4, which apparently reacts with hot hydrogen atoms produced by photolysis. The 8% of the NH3 which is not converted to N2 probably is converted to organic amines and nitrile derivatives. The results indicate that NH3 photolysis is a highly probable mechanism for the conversion of methane to more complex hydrocarbons in the upper atmosphere of Jupiter, and predict the occurrence of HCN, NH2NH2, and higher hydrocarbons in the Jovian atmosphere above the NH3 clouds.

Ferris, J. P.↗
NASA NTRS1976

Isotope shifts in methane near 6000/cm

Isotope shifts for cleanly resolved vibrational-rotational absorption lines of CH4-12 and CH4-13 were measured by a 5-m focal length Littrow spectrometer in the 6000/cm range. The methane isotopes were held in separate absorption cells: 20 torr of CH4-13 in a 1-m cell, and 5 torr of CH4-12 in a White cell of 4-m optical path length. Measured shifts for the cleanly resolved singlets R(0), R(1), Q(1) and P(1) are summarized in tabular form.

Fox, K.↗
NASA NTRS1977

The structure of the atmosphere of Uranus

Models of the interior of Uranus suggest that the abundances of such substances as CH4 are greatly enhanced with respect to solar abundances of heavy elements. Such enhancement leads to a new type of model atmosphere for Uranus, which agrees with observation if the internal energy flux is small (no more than 10%) compared with the absorbed solar energy. An important feature of the models is the presence of a cloud of CH4 droplets whose top is at a temperature of approximately 90 K and a pressure of about 4 atm. Above the cloud, the atmosphere is stable because of the rapid decrease in the thermal flux with depth. Being saturated, most of the observable gaseous CH4 is near the cloud; the CH4 abundance above the cloud, of the order of 5 km-am, is a very sensitive function of the cloud-top temperature.

Danielson, R. E.↗
NASA NTRS1978

Titan's atmosphere: Comments on haze content, methane abundance, band shapes, and hydrogen upper limit

The existence of scatterers in Titan's atmosphere was demonstrated in a paper published in the Astrophysical Journal three years ago. This conclusion was not affected by recent laboratory investigations showing that certain CH4 bands are independent of pressure because it was shown that the reflecting layer model failed to explain Titan's CH4 absorptions regardless on which portion of the curve of growth Titan's CH4 lines lie. Saturn's atmosphere was utilized along the central meridian for studies of CH4 absorption, and to show that the conclusion is insensitive to the moderate scattering there. The quite pronounced role of scattering in Titan's atmosphere strongly suggests that Titan's surface is obscured.

Trafton, L.↗
NASA NTRS1980

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

Recent modeling of atmospheric chemical processes (Logan et al, 1978; Hameed et al, 1979) suggests that tropospheric ozone and methane might significantly increase in the future as the result of increasing anthropogenic emissions of CO, NO(x), and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test the possible climatic impact of changes in tropospheric chemical composition, a zonal energy-balance climate model has been combined with a vertically averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4, and NO(x). The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NO(x) and CH4, and that future increases in these emissions could augment global warming due to increasing atmospheric CO2.

Hameed, S.↗
NASA NTRS1980

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

Tropospheric ozone and methane might increase in the future as the result of increasing anthropogenic emissions of CO, NOx and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test this possible climatic impact, a zonal energy-balance climate model has been combined with a vertically-averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4 and NOx. The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NOx and CH4, and that future increases in these emissions could enhance global warming due to increasing atmospheric CO2.

Cess, R. D.↗
NASA NTRS1981

Atmospheric methane /CH4/ - Trends and seasonal cycles

On the basis of 22 months of almost continuous automated, GC/FID measurements of atmospheric CH4 and Cape Meares (45 deg N), it is shown that the concentration of CH4 is increasing at about 2% per yr (+ or - 0.5%/yr). The data also revealed stable seasonal cycles with peak concentrations in October and minimum concentrations in July. The magnitude of the seasonal variations during these months is about + or - 20 ppby from the average (+ or - 1.2%). If the current trend continues, the increased CH4 concentration may result in a 0.2 K to 0.4 K average increase in earth's surface temperature over the next 40 years or so (based on calculations of Wang et al. (1976)). The coupling of CH4 to tropospheric and stratospheric chemical processes is discussed.

Rasmussen, R. A.↗
NASA NTRS1982

The spectrum of Titan in the far-infrared and microwave regions

The pressure-induced absorptions of gaseous nitrogen (N2) and methane (CH4) are computed on the basis of the collisional lineshape theory of Birnbaum and Cohen (1976). Laboratory data at 300 and 124 K for N2 and at 296 and 195 K for CH4 are used to determine the collisional time constants and their temperature dependence. The spectrum of Titan from the microwave to the far-infrared region (0.1-600/cm) is then modeled using these opacities and a temperature profile of Titan's atmosphere derived from the Voyager 1 radio occultation experiment. The model atmosphere is composed of N2 and CH4, their relative proportions being determined by the vapor pressure law of CH4. A model with gaseous opacity alone is ruled out by the far-infrared observations. An additional opacity, thought to be associated with a methane cloud, is confirmed. The effective temperature of Titan is estimated at 83.2 plus or minus 1.4 K.

Courtin, R.↗
NASA NTRS1983

The atmosphere of the primitive earth and the prebiotic synthesis of organic compounds

The prebiotic synthesis of organic compounds is investigated using a spark discharge on various simulated prebiotic atmospheres at 25 C. It is found that glycine is almost the only amino acid produced from the model atmospheres containing CO and CO2. These results show that the maximum yield is about the same for the three carbon sources (CO, CO2, and CH4) at high H2/carbon ratios, but that CH4 is superior at low H2/carbon ratios. CH4 is found to yield a much greater variety of amino acids than either CO or CO2. If it is assumed that amino acids more complex than glycine were required for the origin of life, then these findings indicate the need for CH4 in the primitive atmosphere. The yields of cyanide and formaldehyde are shown to parallel the amino acid results, with yields of HCN and H2CO as high as 13 percent based on carbon. Ammonia is also found to be produced from N2 in experiments with no added NH3 in yields as high as 4.9 percent. These results indicate that large amounts of NH3 would have been synthesized on the primitive earth by electric discharges.

Miller, S. L.↗
NASA NTRS1985

The photochemistry of biogenic gases in the early and present atmosphere

The distribution of gases in the prebiologial paleoatmosphere is investigated using photochemical models. A chart of the photochemical and chemical reactions and reaction rates for CH4, NH3, H2S, N2O, and CO atmospheric gases is given. Mixing ratios and surface mixing ratios for CH4, NH3, CO, and N2O are obtained using thermodynamic equilibrium calculations; an increase in CH4 and N2O is observed. The reactions, which explain the photochemistry of the gases studied, are presented. The sources of these gases and their concentration with regards to altitude are examined. Graphs of the vertical distribution of CH4, NH3, H2S, CO, O2, and N2O in prebiological paleoatmosphere are provided. The data reveals the presence of only N2, CO2, and N2O in the early atmosphere; with the evolution of life, sources of atmospheric gases increased and their influence on the photochemistry of the troposphere and stratosphere increased.

Levine, J. S.↗
NASA NTRS1986

Photochemistry of methane and the formation of hydrocyanic acid (HCN) in the earth's early atmosphere

A one-dimensional photochemical model is used to analyze the photochemistries of CH4 and HCN in the primitive terrestrial atmosphere. CH4, N2, and HCN photolysis are examined. The background atmosphere and boundary conditions applied in the analysis are described. The formation of HCN as a by-product of N2 and CH4 photolysis is investigated; the effects of photodissociation and rainfall on HCN is discussed. The low and high CH4 mixing ratios and radical densities are studied.

Zahnle, K. J.↗
NASA NTRS1986

Methane, carbon monoxide and methylchloroform in the Southern Hemisphere

New observational data on CH4, CO and CH3CCl3 in the Southern Hemisphere are reported. The data are analyzed for long term trends and seasonal cycles. CH3CCl3 data are used to scale the OH fields incorporated in a two-dimensional model, which in turn, is used to constrain the magnitude of a global CH4 source function. The possible causes of observed seasonality of CH3CCl3, CH4 and CO are identified, and several other aspects of observed CH4 variability are discussed. Possible future research directions are also given.

Fraser, P. J.↗
NASA NTRS1986

Stable carbon isotope ratios in atmospheric methane and some of its sources

Ratios of C-13/C-12 have been measured in atmospheric methane and in methane collected from sites and biota that represent potentially large sources of atmospheric methane. These include temperate marshes (about -48 percent to about -54 percent), landfills (about -51 percent to about -55 percent), and the first reported values for any species of termite (-72.8 + or - 3.1 percent for Reticulitermes tibialis and -57.3 + or - 1.6 percent for Zootermopsis angusticollis). Numbers in parentheses are delta C-13 values with respect to PDB (Peedee belemnite) carbonate. Most methane sources reported thus far are depleted in C-13 with respect to atmospheric methane (-47.0 + or - 0.3 percent). Individual sources of methane should have C-13/C-12 ratios characteristic of mechanisms of CH4 formation and consumption prior to release to the atmosphere. The mass-weighted average isotopic composition of all sources should equal the mean C-13 of atmospheric methane, corrected for a kinetic isotope effect in the OH attack of CH4. Assuming the kinetic isotope effect to be small (about -3.0 percent correction to -47.0), as in the literature, the new values given here for termite methane do not help to explain the apparent discrepancy between C-13/C-12 ratios of the known CH4 sources and that of atmospheric CH4.

Tyler, Stanley C.↗
NASA NTRS1987

C-13/C-12 ratio in methane from the flooded Amazon forest

The C1-C4 hydrocarbon concentrations and the C-13/C-12 ratio in CH4 detected in air samples collected in the Amazon region (3.5 deg S latitude and 5.9 deg W longitude) are analyzed. It is observed that the CH4 concentrations of each sample are enhanced over the background concentration for remote locations, and the C-13/C-12 ratio in this biogenic methane is depleted in C-13 relative to atmospheric CH4. It is concluded, from the C2-C4 hydrocarbon data, that minor yields of C2-C4 hyrocarbons are released coincident with CH4; however, the minor yields do not contribute to the regionally enhanced concentrations of hydrocarbons found in Amazonia and the global atmosphere release of C2-C4 compounds.

Tyler, Stanley C.↗
NASA NTRS1986

Oxidation and reduction rates for organic carbon in the Amazon mainstream tributary and floodplain, inferred from distributions of dissolved gases

Concentrations of CO2, O2, CH4, and N2O in the Amazon River system reflect an oxidation-reduction sequence in combination with physical mixing between the floodplain and the mainstem. Concentrations of CO2 ranged from 150 microM in the Amazon mainstem to 200 to 300 microM in aerobic waters of the floodplain, and up to 1000 microM in oxygen-depleted environments. Apparent oxygen utilization (AOU) ranged from 80 to 250 microM. Methane was highly supersaturated, with concentrations ranging from 0.06 microM in the mainstem to 100 microM on the floodplain. Concentrations of N2O were slightly supersaturated in the mainstem, but were undersaturated on the floodplain. Fluxes calculated from these concentrations indicated decomposition of 1600 g C sq m y(-1) of organic carbon in Amazon floodplain waters. Analysis of relationships between CH4, O2, and CO2 concentrations indicated that approximately 50 percent of carbon mineralization on the floodplain is anaerobic, with 20 percent lost to the atmoshphere as CH4. The predominance of anaerobic metabolism leads to consumption of N2O on the flood plane. Elevated concentrations of CH4 in the mainstem probably reflect imput from the floodplain, while high levels of CO2 in the mainstem are derived from a combination of varzea drainage and in situ respiration.

Richey, Jeffrey E.↗
NASA NTRS1990

Liquid-Vapor Equilibrium of Multicomponent Cryogenic Systems

Liquid-vapor and solid-vapor equilibria at low to moderate pressures and low temperatures are important in many solar system environments, including the surface and clouds of Titan, the clouds of Uranus and Neptune, and the surfaces of Mars and Triton. The familiar cases of ideal behavior are limiting cases of a general thermodynamic representation for the vapor pressure of each component in a homogeneous multicomponent system. The fundamental connections of laboratory measurements to thermodynamic models are through the Gibbs-Duhem relation and the Gibbs-Helmholtz relation. Using laboratory measurements of the total pressure, temperature, and compositions of the liquid and vapor phases at equilibrium, the values of these parameters can be determined. The resulting model for vapor-liquid equilibrium can then conveniently and accurately be used to calculate pressures, compositions, condensation altitudes, and their dependencies on changing climatic conditions. A specific system being investigated is CH4-C2H6-N2, at conditions relevant to Titan's surface and atmosphere. Discussed are: the modeling of existing data on CH4-N2, with applications to the composition of Titan's condensate clouds; some new measurements on the CH4-C2H6 binary, using a high-precision static/volumetric system, and on the C2H6-N2 binary, using the volumetric system and a sensitive cryogenic flow calorimeter; and describe a new cryogenic phase-equilibrium vessel with which we are beginning a detailed, systematic study of the three constituent binaries and the ternary CH4-C2H6-N2 system at temperatures ranging from 80 to 105 K and pressures from 0.1 to 7 bar.

Thompson, W. Reid↗
NASA NTRS1990

Global mapping of minor atmospheric constituents with AIRS on EOS

The Atmospheric Infrared Sounder (AIRS) is a grating-array spectrometer on EOS. It covers the region from 650 to 3000/cm with spectral resolution of 1200. The prime objective of AIRS is the global retrieval of temperature and water vapor profiles and of surface temperatures. The wide spectral coverage of AIRS permits the measurement of a number of additional atmospheric and surface parameters. Of particular interest is the potential to produce daily global maps of the spatial distribution of the more abundant of the minor gases, e.g. ozone, CO, CH4, and N2O. This potential capability for CH4 and N2O is strongly affected by cloud residual. Using the CH4 band at 1306/cm as example, spatial averaging of AIRS data is required to measure a 10 percent change in the nominal CH4 column abundance. At 1300/cm, this requires cloud clearing at the 0.3 percent level. The mapping capability for ozone and CO in terms of rural/urban abundance patterns is not likely to be impacted with cloud-clearing residuals as high as 5 percent.

Aumann, H. H.↗