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At least 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Pathways for methane emissions and oxidation that influence the net carbon balance of a subtropical cypress swamp

We evaluated the major pathways for methane emissions from wetlands to the atmosphere at four wetland sites in the Big Cypress National Preserve in southwest Florida. Methane oxidation was estimated based on the d13C-CH4 of surface water, porewater, and bubbles to evaluate mechanisms that limit surface water emissions. Spatially-scaled methane fluxes were then compared to organic carbon burial rates. The pathway with the lowest methane flux rate was diffusion from surface waters (3.50 ± 0.22 mmol m-2 d-1). Microbial activity in the surface water environment and/or shallow oxic sediment layer oxidized 26 ± 3% of the methane delivered from anerobic sediments to the surface waters. The highest rates of diffusion were observed at the site with the lowest extent of oxidation. Ebullition flux rates were 2.2 times greater than diffusion and more variable (7.79 ± 1.37 mmol m-2 d-1). Methane fluxes from non-inundated soils were 1.6 times greater (18.4 ± 5.14 mmol m-2 d-1) than combined surface water fluxes. Methane flux rates from cypress knees (emergent cypress tree root structures) were 3.7 and 2.3 times higher (42.0 ± 6.33 mmol m-2 d-1) than from surface water and soils, respectively. Cypress knee flux rates were highest at the wetland site with the highest porewater methane partial pressure, suggesting that the emergent root structures allow methane produced in anaerobic sediment layers to bypass oxidation in aerobic surface waters or shallow sediments. Scaled across the four wetlands, emissions from surface water diffusion, ebullition, non-inundated soils, and knees contributed to 14 ± 2%, 25 ± 6%, 34 ± 10%, and 26 ± 5% of total methane emissions, respectively. When considering only the three wetlands with cypress knees present, knee emissions contributed to 39 ± 5% of the total scaled methane emissions. Finally, the molar ratio of CH4 emissions to OC burial ranged from 0.03 to 0.14 in the wetland centers indicating that all four wetland sites are net sources of atmospheric warming potential on 20-100 yr timescales, but net sinks over longer time scales (500 yr) with the exception of one wetland site that was a net source even over 500 yr time scales.

Ward, Nicholas D.↗
DOE OSTI2020

Carbon Nanotube Formation on Cr-Doped Ferrite Catalyst during Water Gas Shift Membrane Reaction: Mechanistic Implications and Extended Studies on Dry Gas Conversions

A nanocrystalline chromium-doped ferrite (FeCr) catalyst was shown to coproduce H2 and multiwalled carbon nanotubes (MWCNTs) during water gas shift (WGS) reaction in a H2-permselective zeolite membrane reactor (MR) at reaction pressures of ~20 bar. The FeCr catalyst was further demonstrated in the synthesis of highly crystalline and dimensionally uniform MWCNTs from a dry gas mixture of CO and CH4, which were the apparent sources for MWCNT growth in the WGS MR. In both the WGS MR and dry gas reactions, the operating temperature was 500 °C, which is significantly lower than those commonly used in MWCNT production by chemical vapor deposition (CVD) method from CO, CH4, or any other precursor gases. Extensive ex situ characterizations of the reaction products revealed that the FeCr catalyst remained in partially reduced states of Fe3+/Fe2+ and Cr6+/Cr3+ in WGS membrane reaction while further reduction of Fe2+ to Fe0 occurred in the CO/CH4 dry gas environments. The formation of the metallic Fe nanoparticles or catalyst surface dramatically improved the crystallinity and dimensional uniformity of the MWCNTs from dry gas reaction as compared to that from WGS reaction in the MR. Reaction of the CO/CH4 mixture containing 500 ppmv H2S also resulted in high-quality MWCNTs similar to those from the H2S-free feed gas, demonstrating excellent sulfur tolerance of the FeCr catalyst that is practically meaningful for utilization of biogas and cheap coal-derived syngas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Air temperature and precipitation constraining the modelled wetland methane emissions in a boreal region in northern Europe

Wetland methane responses to temperature and precipitation are studied in a boreal wetland-rich region in northern Europe using ecosystem process models. Six ecosystem models (JSBACH-HIMMELI, LPX-Bern, LPJ-GUESS, JULES, CLM4.5, and CLM5) are compared to multi-model means of ecosystem models and atmospheric inversions from the Global Carbon Project and upscaled eddy covariance flux results for their temperature and precipitation responses and seasonal cycles of the regional fluxes. Two models with contrasting response patterns, LPX-Bern and JSBACH-HIMMELI, are used as priors in atmospheric inversions with Carbon Tracker Europe–CH4 (CTE-CH4) in order to find out how the assimilation of atmospheric concentration data changes the flux estimates and how this alters the interpretation of the flux responses to temperature and precipitation. Inversion moves wetland emissions of both models towards co-limitation by temperature and precipitation. Between 2000 and 2018, periods of high temperature and/or high precipitation often resulted in increased emissions. However, the dry summer of 2018 did not result in increased emissions despite the high temperatures. The process models show strong temperature and strong precipitation responses for the region (51 %–91 % of the variance explained by both). The month with the highest emissions varies from May to September among the models. However, multi-model means, inversions, and upscaled eddy covariance flux observations agree on the month of maximum emissions and are co-limited by temperature and precipitation. The setup of different emission components (peatland emissions, mineral land fluxes) has an important role in building up the response patterns. Considering the significant differences among the models, it is essential to pay more attention to the regional representation of wet and dry mineral soils and periodic flooding which contribute to the seasonality and magnitude of methane fluxes. The realistic representation of temperature dependence of the peat soil fluxes is also important. Furthermore, it is important to use process-based descriptions for both mineral and peat soil fluxes to simulate the flux responses to climate drivers.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

A permafrost implementation in the simple carbon–climate model Hector v.2.3pf

Abstract. Permafrost currently stores more than a fourth of global soil carbon. A warming climate makes this carbon increasingly vulnerable to decomposition and release into the atmosphere in the form of greenhouse gases. The resulting climate feedback can be estimated using land surface models, but the high complexity and computational cost of these models make it challenging to use them for estimating uncertainty, exploring novel scenarios, and coupling with other models. We have added a representation of permafrost to the simple, open-source global carbon–climate model Hector, calibrated to be consistent with both historical data and 21st century Earth system model projections of permafrost thaw. We include permafrost as a separate land carbon pool that becomes available for decomposition into both methane (CH4) and carbon dioxide (CO2) once thawed; the thaw rate is controlled by region-specific air temperature increases from a preindustrial baseline. We found that by 2100 thawed permafrost carbon emissions increased Hector’s atmospheric CO2 concentration by 5 %–7 % and the atmospheric CH4 concentration by 7 %–12 %, depending on the future scenario, resulting in 0.2–0.25 ∘C of additional warming over the 21st century. The fraction of thawed permafrost carbon available for decomposition was the most significant parameter controlling the end-of-century temperature change in the model, explaining around 70 % of the temperature variance, and was distantly followed by the initial stock of permafrost carbon, which contributed to about 10 % of the temperature variance. The addition of permafrost in Hector provides a basis for the exploration of a suite of science questions, as Hector can be cheaply run over a wide range of parameter values to explore uncertainty and can be easily coupled with integrated assessment and other human system models to explore the economic consequences of warming from this feedback.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1972

Evaluation of advanced bladder technology

Research conducted during this period is reported. Studies presented include: (1) diffusion and permeation of CO2, O2, N2, and NO2 through polytetra fluoroethylene; (2) diffusion, permeation and solubility of simple gases (CO2, O2, N2, CH4, C2H6, C3H8, and C2H4) through a copolymer of hexafluoro propylene and tetrafluoro ethylene (FEP); (3) viscous flow and diffusion of gases throug small apertures; (4) diffusion and permeation of O2, N2, CO2, CH4, C2H6, and C3H8 through nitroso rubber; and (5) results of gas transport studies with carborane siloxane, nitroso rubber, silicone membrane, krytox coating on teflon, and FEP coated glass cloth. Publications generated under this program are listed.

Christensen, M. V.↗
NASA NTRS1972

Carbon chemistry of Apollo 14 size-fractionated fines.

Experiments have been conducted on several Apollo 12 and 14 samples that confirm the identification of CH4 and C2H6 in lunar fines and breccias. In particular, data for various size fractions of sample 14240,5 are reported which show that the concentrations of these species are dependent on particle size. Results strongly support proposals that solar wind activity is a source of CH4 in lunar samples.

Holland, P. T.↗
NASA NTRS1973

Observations of 7.9-micron limb brightening on Jupiter.

Gillett et al. (1969) observed that the brightness temperature in the strong 7.7-micron CH4 band was higher than at the neighboring wavelengths (where the absorption was expected to be less) in the Jovian spectrum from 2.8 to 13 microns. This observation was interpreted as being caused by a temperature inversion in the upper atmosphere of Jupiter. This interpretation is checked by measuring the variation of the brightness temperature from the center to the limb of the disk, and is confirmed by the observation of limb brightening, rather than the usual limb darkening, at a certain wavelength within the 7.7-micron CH4 band.

Gillett, F. C.↗
NASA NTRS1974

Titan - Unidentified strong absorptions in the photometric infrared

The morphology of Titan's infrared spectral features reveals a pattern of differences with respect to Saturn's bands. Titan's bands exhibit a progressive washing out with increasing wavelength relative to the corresponding bands in Saturn's spectrum. Unidentified absorption features of apparently gaseous origin appear in the long-wavelength wing of Titan's 1-micron CH4 band complex with considerably greater strength. Greater absorption is also observed in the 1.1 micron region. Not all of the phenomena can be explained by enhanced CH4 absorption, so Titan's spectrum implies the existence of another spectroscopically active gas. Several candidates for this gas are briefly considered.

Trafton, L.↗
NASA NTRS1974

Theoretical nitric oxide production incidental to autoignition and combustion of several fuels homogeneously dispersed in air under some typical hypersonic flight conditions

A reaction package of 100 chemical reactions and attendant reaction rate constants defined for the autoignition and combustion of four carbonaceous fuels, CH4, CH3OH, C2H6, and C2H5OH. Definition of the package was made primarily by means of comparison between trial calculations and experimental data for the autoignition of CH4. Autoignition and combustion of each of these four fuels was calculated under three sets of conditions realistic for hypersonic flight applications, for comparison to hydrogen fuel, particularly with respect to formation of nitric oxide. Results show that, for all of the fuels including hydrogen, if NO production is a significant problem, compromise must be made between approaching equilibrium heat release and approaching equilibrium NO concentration.

Bahn, G. S.↗
NASA NTRS1975

Sensitivity of gas filter correlation instrument to variations in optical balance

A computer program was used to simulate the response of the Gas Filter Correlation Radiometer (GFCR) to changing pollutant levels of CO, SO2, CH4, and NH3 in two model atmospheres. Positive and negative deviations of tau sub alpha of magnitudes 0.01, 0.1, and 1 percent were imposed upon the simulation and the resulting deviations in inferred concentrations were determined. For the CO, CH4, and the higher pressure cell of the NH3 channel, the deviations are less than + or - 12 percent for deviations in tau sub alpha of + or - 0.1 percent, but increase to significantly higher values for larger deviations. For the lower pressure cell of NH3 and for SO2, the deviations in inferred concentration begin to rise sharply between 0.01 and 0.1 percent deviation in tau sub alpha, suggesting that a tighter control on tau sub alpha may be required for these channels.

Orr, H. D., III↗
NASA NTRS1975

Reactions of CH3, CH3O, and CH3O2 radicals with O3

Ozone was photolyzed at 253.7 nm at 25 and -52 degrees in the presence of CH4 and O2 to measure the reactions of O3 with CH3, CH3O, and CH3O2. The O(1D) atoms produced in the primary photochemical act react with CH4 to give CH3 radicals which in turn can react with O2 to give CH3O2 and CH3O radicals. At very high O2 to O3 concentration ratios, the quantum yield of O3 disappearance approached 1.0, indicating that O3 reactions with CH3O2 and CH3O are slow. Upper limits to the rate coefficients at 25 degrees were computed. At lower values of the concentration ratio, chain decomposition of O3 occurred which could be explained by the reaction of O3 with CH3 radicals to produce CH2O, O2, and H atoms all the time. The two routes to these products are considered, and the preferred reaction channel is found.

Simonaitis, R.↗
NASA NTRS1975

Methane absorption in the visible spectra of the outer planets and Titan

New spectra of Jupiter, Saturn, and Titan show weak methane bands in the region below 6000 A which have been known for many years in the spectra of Uranus and Neptune. Adopting the known abundance of methane on Jupiter, we have used a band model to determine CH4 abundances and broadening pressures for the other objects. The results indicate high values of the CH4 to H2 concentration ratio for Uranus and Neptune; for Titan, a surface pressure in excess of 1 atm is implied.

Owen, T.↗
NASA NTRS1976

The measurement of carbon monoxide and methane in the National Capital Air Quality Control Region. I - Measurement systems

The Carbon Monoxide Pollution Experiment (COPE) and the National Capital Air Quality Control Region (NCAQCR) undertook a series of measurements of atmospheric CO and CH4 to determine the accuracy of the airborne COPE Correlation Interfer4meter. The device, a modified Michelson interferometer, measures the atmospheric column density of CO and CH4 at 2.3 microns with tropospheric measurement sensitivities of 70 and 10 PPB, respectively. Data for evaluating the remote measurements included atmospheric column density measurements at a ground truth site using a van-mounted infrared Fourier spectrometer; continuous ground level gas chromatographic measurements; and chromatographic data from atmospheric grab samples collected by aircraft and at ground locations. The instruments and sampling techniques used in the experiment are described in detail.

Lebel, P. J.↗
NASA NTRS1976

The measurement of carbon monoxide and methane in the national capital air quality control region. II - Meteorological conditions and chromatographic and spectrometric results

The meteorological conditions during this program consisted of a stagnant high pressure system which was subsequently replaced by southward moving Canadian air. This change in air masses produced distinct changes in the ambient CO concentrations. Ground level concentrations decreased from an average of 1.3 ppm at the beginning of the experiment to 0.2 ppm at the end. Vertical profiles obtained during the experiment showed decreases in the CO concentrations with altitude. Agreement of gas chromatography data for CO and CH4 by NASA and NRL was within 5% for the concentrations encountered. Results from NASA's Infrared Fourier Spectrometer agreed with the gas chromatographic results both in trends and concentrations of CO and CH4 observed with the passing frontal system.

Lamontagne, R. A.↗
NASA NTRS1976

Methane rich models of Uranus

A series of models of Uranus is computed assuming that Uranus consists of a core of rocky material surrounded by a convecting envelope rich in H2O, NH3, and CH4. It is found that good fits are obtained to the observed parameters when the CH4:H2 ratio is of the order of 0.1. It is suggested that the rotational period of Uranus is roughly 18 h.

Podolak, M.↗
NASA NTRS1976

The aerosol distribution in Uranus' atmosphere - Interpretation of the hydrogen spectrum

New observations of Uranus' combined H2 spectrum have been obtained. An analysis, emphasizing the leverage provided by the S3(0) quadrupole line, leads to strong constraints on Uranus' bulk aerosol distribution with depth. Using an inhomogeneous model atmosphere program which includes Rayleigh scattering for gases and a 1 plus cos theta phase function for cloud layers, it is shown that Uranus' H2 spectrum implies a cloud layer (or dense aerosol) at a depth from 500 to 700 km-amagat H2. It also implies negligible aerosol scattering in the 280 to 450 km-amagat H2 region and a thin haze at 100 to 200 km-amagat H2 depths. The low albedo in very strong CH4 bands indicates that there is negligible aerosol scattering in Uranus' radiative zone. Hydrogen appears to be more abundant than the sum of all other atmospheric gases. The C/H ratio deep in Uranus' atmosphere is strongly enhanced over the solar value. Accurate limb-darkening measurements in and near strong CH4 bands would be effective in specifying Uranus' aerosol distribution in greater detail.

Trafton, L.↗
NASA NTRS1976

An analysis of Saturn's methane 3 nu /3/ band profiles in terms of an inhomogeneous atmosphere

Observed profiles of the R branch of Saturn's CH4 3 nu (3) band are compared with synthetic profiles computed from inhomogeneous models which are consistent with Saturn's H2 quadrupole-line equivalent widths. A C/H ratio approximately three times the solar value and a CH4 abundance of about 100 m am are found. Scattering plays a significant role in the formation of manifold profiles below a depth where the H2 abundance is 20-30 km am.

Macy, W., Jr.↗
NASA NTRS1977

On the sources of ultraviolet absorption in spectra of Titan and the outer planets

In response to observations of the ultraviolet deficiencies shown by all of the outer planets and Titan, models have been proposed to explain the low albedos in terms of absorption by particles in the upper atmospheres of these objects. These particles are generally believed to be photochemically formed from gases in the upper atmospheres, primarily methane and hydrogen. Such processes may also be operative on Titan. Results of some laboratory experiments on proton irradiation of mixtures of gases including CH4, H2, and NH3 have shown that liquid and solid materials are produced that are strong ultraviolet absorbers. However, the material produced from the CH4 + H2 mixture was colorless, indicating that species containing elements other than carbon and hydrogen are necessary for the production of color. Two such elements are nitrogen (as NH3 or N2) and sulfur (as H2S); colored materials have been produced from such mixtures. None of these materials has spectral properties identical to those shown by the planets. Therefore it is necessary that mixtures (and/or cloud layers) of the photochemical materials be present.

Scattergood, T.↗