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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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NASA NTRS1996

Isotopic Evidence for Changes in the Biochemical Carbon Cycle During the Early- and Mid-Proterzoic Eon: Implications for the Biosphere and Atmosphere

The Archean fossil record reveals a biosphere whose biota were remarkably sophisticated. For example, bacteria were capable of photosynthesis, and they withstood the ultraviolet radiation and periodic desiccation which accompanied the intertidal environment. However, we can infer relatively little about evolutionary change between 3 and 1.1 billion years (Ga) ago. What biological events occurred, and how did changes in the environment influence the nature and timing of these events? The carbon biogeochemical cycle played a key role, and isotopic measurements of sedimented carbon can reveal long-term changes in this cycle. Additional information is contained in the original extended abstract.

DesMarais, David J.↗
NASA NTRS1976

Interstellar cloud evolution and the abundance of formaldehyde

The time scale for essentially complete conversion of C(+) to CO in interstellar clouds can be comparable to, or greater than, dynamical time scales for evolution, therefore suggesting steady state time independent abundances to be inappropriate. The solutions for the time-dependent carbon chemistry in dense clouds, with density not less than 500/cu cm, indicate that significant amounts of neutral carbon will be present throughout a cloud's lifetime. These nonequilibrium values of C I can explain the relatively large abundances observed for formaldehyde, isotopes of carbon monoxide, and other trace molecules

Langer, W. D.↗
NASA NTRS1997

A blast of gas in the latest Paleocene: simulating first-order effects of massive dissociation of oceanic methane hydrate

Carbonate and organic matter deposited during the latest Paleocene thermal maximum is characterized by a remarkable -2.5% excursion in delta 13C that occurred over approximately 10(4) yr and returned to near initial values in an exponential pattern over approximately 2 x 10(5) yr. It has been hypothesized that this excursion signifies transfer of 1.4 to 2.8 x 10(18) g of CH4 from oceanic hydrates to the combined ocean-atmosphere inorganic carbon reservoir. A scenario with 1.12 x 10(18) g of CH4 is numerically simulated here within the framework of the present-day global carbon cycle to test the plausibility of the hypothesis. We find that (1) the delta 13C of the deep ocean, shallow ocean, and atmosphere decreases by -2.3% over 10(4) yr and returns to initial values in an exponential pattern over approximately 2 x 10(5) yr; (2) the depth of the lysocline shoals by up to 400 m over 10(4) yr, and this rise is most pronounced in one ocean region; and (3) global surface temperature increases by approximately 2 degrees C over 10(4) yr and returns to initial values over approximately 2 x 10(6) yr. The first effect is quantitatively consistent with the geologic record; the latter two effects are qualitatively consistent with observations. Thus, significant CH4 release from oceanic hydrates is a plausible explanation for observed carbon cycle perturbations during the thermal maximum. This conclusion is of broad interest because the flux of CH4 invoked during the maximum is of similar magnitude to that released to the atmosphere from present-day anthropogenic CH4 sources.

Non-NASA Center↗
NASA NTRS1975

Light element geochemistry of the Apollo 16 site

The abundance and isotopic composition of carbon, sulfur, and nitrogen, the abundance of helium and hydrogen, and the content of metallic iron are reported for lunar surface samples from the Apollo 16 landing site at Cayley-Descartes. The light elements show marked interstation variability at the site. The abundances in soils of C, N, He, and H are apparently controlled mainly by exposure to the solar wind, through implantation or stripping processes. Carbon abundances (but not observed isotopic distributions) are compatible with a model in which equilibrium is established after 10,000-100,000 yr between solar wind input and loss by proton stripping. Sulfur abundances in soils are apparently controlled by abundances in local country rocks, but the lunar S cycle is quite complex. A metallic iron component may have originated by solar wind reduction of lunar Fe(2+).

Kerridge, J. F.↗
NASA NTRS1994

Factors and processes governing the C-14 content of carbonate in desert soils

A model is presented describing the factors and processes which determine the measured C-14 ages of soil calcium carbonate. Pedogenic carbonate forms in isotopic equilium with soil CO2. Carbon dioxide in soils is a mixture of CO2 derived from two biological sources: respiration by living plant roots and respiration of microorganisms decomposing soil humus. The relative proportion of these two CO2 sources can greatly affect the initial C-14 content of pedogenic carbonate: the greater the contribution of humus-derived CO2, the greater the initial C-14 age of the carbonate mineral. For any given mixture of CO2 sources, the steady-state (14)CO2 distribution vs. soil depth can be described by a production/diffusion model. As a soil ages, the C-14 age of soil humus increases, as does the steady-state C-14 age of soil CO2 and the initial C-14 age of any pedogenic carbonate which forms. The mean C-14 age of a complete pedogenic carbonate coating or nodule will underestimate the true age of the soil carbonate. This discrepancy increases the older a soil becomes. Partial removal of outer (and younger) carbonate coatings greatly improves the relationship between measured C-14 age and true age. Although the production/diffusion model qualitatively explains the C-14 age of pedogenic carbonate vs. soil depth in many soils, other factors, such as climate change, may contribute to the observed trends, particularily in soils older than the Holocene.

Amundson, Ronald↗
NASA NTRS1993

Airborne measurements of sulfur dioxide, dimethyl sulfide, carbon disulfide, and carbonyl sulfide by isotope dilution gas chromatography/mass spectrometry

A gas chromatograph/mass spectrometer is described for determining atmospheric sulfur dioxide, carbon disulfide, dimethyl sulfide, and carbonyl sulfide from aircraft and ship platforms. Isotopically labelled variants of each analyte were used as internal standards to achieve high precision. The lower limit of detection for each species for an integration time of 3 min was 1 pptv for sulfur dioxide and dimethyl sulfide and 0.2 pptv for carbon disulfide and carbonyl sulfide. All four species were simultaneously determined with a sample frequency of one sample per 6 min or greater. When only one or two species were determined, a frequency of one sample per 4 min was achieved. Because a calibration is included in each sample, no separate calibration sequence was needed. Instrument warmup was only a few minutes. The instrument was very robust in field deployments, requiring little maintenance.

Bandy, Alan R.↗
NASA NTRS2005

Modeling Chemical and Isotopic Variations in Lab Formed Hydrothermal Carbonates

Chemical and mineralogical data (e.g. [1]) from Mars suggest that the history of liquid water on the planet was more sporadic in nature than long-lived. The non-equilibrium chemical and isotopic compositions of the carbonates preserved in the martian meteorite ALH84001 are direct evidence of ancient secondary minerals that have not undergone significant diagenesis or stabilization processes typical of long-lived aqueous systems on Earth. Thus secondary minerals and sediments on Mars may primarily record the characteristics of the aqueous environment in which they formed without being significantly overprinted by subsequent diagenetic processes during burial.

Niles, P. B.↗
NASA NTRS1992

Silicon isotopic composition in large meteoritic SiC particles and Na-22 origin of Ne-22

Large SiC particles extracted from acid-insoluble residues of carbonaceous chondrites are isotopically anomalous in both silicon and carbon and contain isotopically extreme noble gases. These particles are thought to have originated in mass outflows from red giant stars and to have existed in the interstellar medium at the time the solar system formed from an interstellar cloud. Calculations show that the silicon isotope correlations in those large SiC particles can be generated only in the most massive carbon stars. Consequently, the almost pure Ne-22 in those particles must be interpreted as the condensation of radioactive Na-22 in the particles as they flowed away from the stars. The Na-22 is produced through proton capture by Ne-21 at the base of the surface convection zone. Ne-22 does not exist abundantly in helium shells hot enough to burn magnesium, which is necessary to establish the measured silicon isotopic composition.

Brown, Lawrence E.↗
NASA NTRS1989

The C-13/C-12 kinetic isotope effect for soil oxidation of methane at ambient atmospheric concentrations

During a survey of the Alaskan North Slope to estimate the isotopic composition and fluxes of methane (CH4) from the tundra, two sites were encountered that showed net methane consumption within flux chambers. Methane concentrations decreased from ambient (1.78 ppmv) by up to 50 percent, and the delta C-13 increased by up to 10 percent in the two chamber deployments showing CH4 consumption. CH4 consumption rates were measured to be 1.2 and 0.6 mg CH4/sq m per day; the corresponding carbon kinetic isotope effects (k13/k12) were 0.974 and 0.984, respectively.

King, Stagg L.↗
NASA NTRS1985

The non-mass-dependent oxygen isotope effect in the electrodissociation of carbon dioxide - A step toward understanding NoMaD chemistry

A non-mass dependent (NoMaD) oxygen isotope effect is demonstrated in the dissociation of CO2 similar to that observed in the electrosynthesis of ozone. The molecular oxygen produced carries the signature of two separate isotopic fractionation processes; a mass-dependent fractionation probably due to CO2 + O isotopic exchange, and a secondary NoMaD fractionation (delta O-17 = 0.97 + or - 0.09 delta O-18, with the O2 depleted in O-17 and O-18). It is suggested that the effect is due to either the formation or relaxation of ozone in an excited electronic state. This represents the latest advance in the understanding of chemical NoMaD effects which may be essential to the explanation of non-mass-dependent fractionations observed in meteorites.

Heidenreich, J. E., III↗
NASA NTRS2004

Evolution of the Ureilite Parent Body

Ureilites are ultramafic achondrites composed primarily of olivine and pyroxene with intergranular fine-grained metal, sulfides, and silicates. Ureilites contain significant amounts of carbon (up to about 6.5 wt%) as graphite, lonsdaleite, and/or diamond. It has been shown that carbon-silicate redox (i.e. "smelting") reactions are responsible for the negative FeO-MnO (or positive Fe/Mn-Fe/Mg with constant Mn/Mg) trend seen in the mineral and bulk compositions of ureilites and for the positive correlation between modal percent pigeonite and mg#. Carbon redox reactions are strongly exothermic and pressure dependent; so ureilites with the largest mg# are the most reduced, experienced the highest temperatures, and formed at the lowest pressures, i.e. near the surface of the ureilite parent body. Ureilites with the largest mg# have the smallest the delta(sup 18)O and the largest Delta(sup 17)O. To explain this, Singletary and Grove proposed that heterogeneous accretion took place on the ureilite parent body, which lead to a radial distribution of the oxygen isotopes. To further investigate possible relationships, we performed carbon isotope and electron probe measurements on a suite of 27 ureilites in order to see the type of correlation that exists between mg#, oxygen isotopes, and carbon.

Hudson, P.↗
NASA NTRS1994

Acquisition and processing of data for isotope-ratio-monitoring mass spectrometry

Methods are described for continuous monitoring of signals required for precise analyses of 13C, 18O, and 15N in gas streams containing varying quantities of CO2 and N2. The quantitative resolution (i.e. maximum performance in the absence of random errors) of these methods is adequate for determination of isotope ratios with an uncertainty of one part in 10(5); the precision actually obtained is often better than one part in 10(4). This report describes data-processing operations including definition of beginning and ending points of chromatographic peaks and quantitation of background levels, allowance for effects of chromatographic separation of isotopically substituted species, integration of signals related to specific masses, correction for effects of mass discrimination, recognition of drifts in mass spectrometer performance, and calculation of isotopic delta values. Characteristics of a system allowing off-line revision of parameters used in data reduction are described and an algorithm for identification of background levels in complex chromatograms is outlined. Effects of imperfect chromatographic resolution are demonstrated and discussed and an approach to deconvolution of signals from coeluting substances described.

NASA Discipline Exobiology↗
NASA NTRS1994

Factors controlling precision and accuracy in isotope-ratio-monitoring mass spectrometry

The performance of systems in which picomole quantities of sample are mixed with a carrier gas and passed through an isotope-ratio mass spectrometer system was examined experimentally and theoretically. Two different mass spectrometers were used, both having electron-impact ion sources and Faraday cup collector systems. One had an accelerating potential of 10kV and accepted 0.2 mL of He/min, producing, under those conditions, a maximum efficiency of 1 CO2 molecular ion collected per 700 molecules introduced. Comparable figures for the second instrument were 3 kV, 0.5 mL of He/min, and 14000 molecules/ion. Signal pathways were adjusted so that response times were <200 ms. Sample-related ion currents appeared as peaks with widths of 3-30 s. Isotope ratios were determined by comparison to signals produced by standard gases. In spite of rapid variations in signals, observed levels of performance were within a factor of 2 of shot-noise limits. For the 10-kV instrument, sample requirements for standard deviations of 0.1 and 0.5% were 45 and 1.7 pmol, respectively. Comparable requirements for the 3-kV instrument were 900 and 36 pmol. Drifts in instrumental characteristics were adequately neutralized when standards were observed at 20-min intervals. For the 10-kV instrument, computed isotopic compositions were independent of sample size and signal strength over the ranges examined. Nonlinearities of <0.04%/V were observed for the 3-kV system. Procedures for observation and subtraction of background ion currents were examined experimentally and theoretically. For sample/ background ratios varying from >10 to 0.3, precision is expected and observed to decrease approximately 2-fold and to depend only weakly on the precision with which background ion currents have been measured.

NASA Discipline Exobiology↗
NASA NTRS1990

Isotopic Hg in an Allende carbon-rich residue

A carbon-rich residue from Allende subjected to stepwise heating yielded two isotopically resolvable types of Hg: one with an (Hg-196)/(Hg-202) concentration ratio the same as terrestrial (monitor) Hg; the other enriched in Hg-196 relative to Hg-202 by about 60 percent. Hg with the 202 isotope enriched relative to 196, as is found in bulk Allende, was not observed. Whether the result of mass fractionation or nucleosynthesis, the distinct types of Hg entered different carrier phases and were not thermally mobilized since the accretion of the Allende parent body.

Reed, G. W., Jr.↗
NASA NTRS1994

The ratios of carbon and non-radiogenic helium and argon isotopes in the mantle and crustal rocks

The studies of the relations of carbon and primary isotopes of noble gases were carried out on the natural gases and on the mantle rocks from the mantle M-type sources, which represent the degassed mantle reservoir (MORB's). These works has the aim of estimation of the values of the C/3He ratios in the deep mantle fluids to determine the flux of the mantle CO2 on the basis of known flux of primary mantle 3He. It was found, that in the natural gases the values of the C/3He ratios fall into the range from 1 times E plus 6 to 1 times E plus 15, and in the fluids of MORB's are constant near 2 times E plus 9. We have studied the mantle rocks from the relatively undergassed mantle P minus type sources: continental; Baikal Rift (Siberia), Mongolia, Catalonia (Spain), Pannonia Depression (central Europe) and ocean; Spietzbergen isl., Hawaii isl., Canarian isl. It ws found, that in mantle xenolites and the host alkaline basalts from the continental rifts and ocean islands, the values of the C/3He ratios fall into the range from E plus 11 to E plus 15 (and this result needed to be explained; the higher carbon to helium ratios is relatively undergassed mantle reservoir compared with the degassed one, requires whether hilly compatibility of helium compared with carbon, whether additional flux of 3He to the degassed mantle reservoir). From the other hand it was found that in the mantle rocks from the sources of P minus and M minus types, continental carbonatites, the values of the C/36Ar ratios are constant in the range from E plus 9 to E plus 10, the close values have the MORB's also.

Lokhov, K.↗
NASA NTRS1990

Primary and diagenetic controls of isotopic compositions of iron-formation carbonates

Results are presented on parallel analyses of carbonate and chert microbands in segments from the early Proterozoic Dales Gorge Member of the Brockman Iron Formation (western Australia), including data on isotopic, chemical, and mineralogic variations in microbanded carbonates, cherts, and coexisting minerals in four core segments from Paraburdoo and one from Wittenoom. It is shown that patterns of variation observed in isotopic abundance and mineral composition can be consistently explained in terms of diagenetic replacement of fine-grained primary precipitates by secondary ones, rather than by mineral-dependent fractionations, metamorphism, or the influence of large volumes of water in an open system.

Kaufman, Alan J.↗