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At least 19 records

Contribution of Changing Sources and Sinks to the Growth Rate of Atmospheric Methane Concentrations for the Last Two Decades

In situ measurements of atmospheric methane concentrations begun in the early 1980s show decadal trends, as well as large interannual variations, in growth rate. Recent research indicates that while wetlands can explain several of the large growth anomalies for individual years, the decadal trend may be the combined effect of increasing sinks, due to increases in tropospheric OH, and stabilizing sources. We discuss new 20-year histories of annual, global source strengths for all major methane sources, i.e., natural wetlands, rice cultivation, ruminant animals, landfills, fossil fuels, and biomass burning, and present estimates of the temporal pattern of the sink required to reconcile these sources and atmospheric concentrations over the time period. Analysis of the individual emission sources, together with model-derived estimates of the OH sink strength, indicates that the growth rate of atmospheric methane observed over the last 20 years can only be explained by a combination of changes in source emissions and an increasing tropospheric sink.

Matthews, Elaine↗

Contribution of Changing Sources and Sinks to the Growth Rate of Atmospheric Methane Concentrations for the Last Two Decades

In situ measurements of atmospheric methane concentrations begun in the early 1980s show decadal trends, as well as large interannual variations, in growth rate. Recent research indicates that while wetlands can explain several of the large growth anomalies for individual years, the decadal trend may be the combined effect of increasing sinks, due to increases in tropospheric OH, and stabilizing sources. We discuss new 20-year histories of annual, global source strengths for all major methane sources, i.e., natural wetlands, rice cultivation, ruminant animals, landfills, fossil fuels, and biomass burning. We also present estimates of the temporal pattern of the sink required to reconcile these sources and atmospheric concentrations over this time period. Analysis of the individual emission sources, together with model-derived estimates of the OH sink strength, indicates that the growth rate of atmospheric methane observed over the last 20 years can only be explained by a combination of changes in source emissions and an increasing tropospheric sink. Direct validation of the global sources and the terrestrial sink is not straightforward, in part because some sources/sinks are relatively small and diffuse (e.g., landfills and soil consumption), as well as because the atmospheric record integrates multiple and substantial sources and tropospheric sinks in regions such as the tropics. We discuss ways to develop and test criteria for rejecting and/or accepting a suite of scenarios for the methane budget.

Matthews, Elaine↗

Methane concentrations and source strengths in urban locations

The results of a six year measurement of trace gases in 18 different urban and remote areas throughout the Northern and Southern Hemispheres are reported. It is found that the measurements are consistent with a yearly atmospheric release of 30 to 60 megatons of CH4 in urban environments. Concentrations of CCl3F, CCl2F2, and CH3CCl3 were also found to be higher in the same urban samples than in corresponding samples from remote areas. The 'urban excess' (urban concentration minus remote concentration) was generally 1000 to 2000 times larger on a molar basis for CH4 than for CCl3F. The fraction of world-wide methane release occurring in the urban environment is estimated from the concentration ratios for CH4 vs CCl3F. It is shown that about 8 to 15 percent of atmospheric methane release occurs in urban areas.

Blake, D. R.↗

Methane concentration and isotopic composition measurements with a mid-infrared quantum-cascade laser

A quantum-cascade laser operating at a wavelength of 8.1 micrometers was used for high-sensitivity absorption spectroscopy of methane (CH4). The laser frequency was continuously scanned with current over more than 3 cm-1, and absorption spectra of the CH4 nu 4 P branch were recorded. The measured laser linewidth was 50 MHz. A CH4 concentration of 15.6 parts in 10(6) ( ppm) in 50 Torr of air was measured in a 43-cm path length with +/- 0.5-ppm accuracy when the signal was averaged over 400 scans. The minimum detectable absorption in such direct absorption measurements is estimated to be 1.1 x 10(-4). The content of 13CH4 and CH3D species in a CH4 sample was determined.

Non-NASA Center↗

No detection of methane on Mars from early ExoMars Trace Gas Orbiter observations

The detection of methane on Mars has been interpreted as indicating that geochemical or biotic activities could persist on Mars today. A number of different measurements of methane show evidence of transient, locally elevated methane concentrations and seasonal variations in background methane concentrations. These measurements, however, are difficult to reconcile with our current understanding of the chemistry and physics of the Martian atmosphere, which—given methane’s lifetime of several centuries—predicts an even, well mixed distribution of methane. Here we report highly sensitive measurements of the atmosphere of Mars in an attempt to detect methane, using the ACS and NOMAD instruments onboard the ESA-Roscosmos ExoMars Trace Gas Orbiter from April to August 2018. We did not detect any methane over a range of latitudes in both hemispheres, obtaining an upper limit for methane of about 0.05 parts per billion by volume, which is 10 to 100 times lower than previously reported positive detections. We suggest that reconciliation between the present findings and the background methane concentrations found in the Gale crater would require an unknown process that can rapidly remove or sequester methane from the lower atmosphere before it spreads globally.

Michael Doyle Smith↗

World-wide increase in tropospheric methane, 1978-1983

Techniques used to assess methane concentration in the troposphere are described, and data obtained during the period from 1978 to 1983 are presented in detail. Tropospheric methane concentrations in remote locations averaged a yearly world-wide increase of 0.018 + or - 0.002 parts per million by volume (ppmv). Average world-wide tropospheric concentration of methane in dry air was 1.625 ppmv at the end of 1983 measured against an NBS standard certified as 0.97 ppmv. Contributing to this steady increase in methane concentration are increases in the source strengths from cattle and rice fields, which in turn result from CO, CH4 and HO coupling. Among the physical and chemical effects is an increase in greenhouse warming of about 0.04 C per decade.

Blake, D. R.↗

Laser beam methane detector

Instrument uses infrared absorption to determine methane concentration in liquid natural gas vapor. Two sensors measure intensity of 3.39 mm laser beam after it passes through gas; absorption is proportional to concentration of methane. Instrument is used in modeling spread of LNG clouds and as leak detector on LNG carriers and installations. Unit includes wheels for mobility and is both vertically and horizontally operable.

Hinkley, E. D., Jr.↗

A laser flash photolysis-resonance fluorescence kinetics study of the reaction Cl/2P/ + CH4 yields CH3 + HCl

The technique of laser flash photolysis-resonance fluorescence is employed to study the kinetics of the reaction Cl(2P) + CH4 yields CH3 + HCl over the temperature range 221-375 K. At temperatures less than or equal to 241 K the apparent bimolecular rate constant is found to be dependent upon the identity of the chemically inert gases in the reaction mixture. For Cl2/CH4/He reaction mixtures (total pressure = 50 torr) different bimolecular rate constants are measured at low and high methane concentrations. For Cl2/CH4/CCl/He and Cl2/CH4/Ar reaction mixtures, the bimolecular rate constant is independent of methane concentration, being approximately equal to the rate constant measured at low methane concentrations for Cl2/CH4/He mixtures. These rate constants are in good agreement with previous results obtained using the discharge flow-resonance fluorescence and competitive chlorination techniques. At 298 K the measured bimolecular rate constant is independent of the identity of the chemically inert gases in the reaction mixture and in good agreement with all previous investigations. The low-temperature results obtained in this investigation and all previous investigations can be rationalized in terms of a model which assumes that the Cl(2P 1/2) state reacts with CH4 much faster than the Cl(2P 3/2) state. Extrapolation of this model to higher temperatures, however, is not straightforward.

Ravishankara, A. R.↗

Root-Associated Methane Oxidation and Methanogenesis: Key Determinants of Wetland Methane Emissions

During the award period, we have assessed the extent and controls of methane oxidation in north temperate wetlands. It is evident that wetlands have been a major global source of atmospheric methane in the past, and are so at present. It is also evident that microbial methane oxidation consumes a variable fraction of total wetland methane production, perhaps 10%-90%. Methane oxidation is thus a potentially important control of wetland methane emission. Our efforts have been designed to determine the extent of the process, its controls, and possible relationships to changes that might be expected in wetlands as a consequence of anthropogenic or climate-related disturbances. Current work, has emphasized controls of methane oxidation associated with rooted aquatic plants. As for the sediment-water interface, we have observed that oxygen availability is a primary limiting factor. Our conclusion is based on several different lines of evidence obtained from in vitro and in situ analyses. First, we have measured the kinetics of methane oxidation by intact plant roots harboring methane-oxidizing bacteria, as well as the kinetics of the methanotrophs themselves. Values for the half-saturation constant (apparent K(sub m)) are approximately 5 microns. These values are roughly equivalent to, or much less than porewater methane concentrations, indicating that uptake is likely saturated with respect to methane, and that some other parameter must limit activity. Methane concentrations in the lacunar spaces at the base of plant stems are also comparable to the half-saturation constants (when expressed as equivalent dissolved concentrations), providing further support for limitation of uptake by parameters other than methane.

King, G. M.↗

Determination of methane in ambient air by multiplex gas chromatography

A multiplex gas chromatographic technique for the determination of methane in ambient air over extended periods is reported. A modest gas chromatograph which uses air as the carrier gas was modified by adding a silver oxide sample modulator for multiplex operation. The modulator selectively catalyzes the decomposition of methane in air. The resulting analytical system requires no consumables beyond power. A profile of the methane concentration in this laboratory was obtained for an 8-day period. During this period, methane concentration varied with an approximately daily period from a low of 1.53 + or - 0.60 ppm to a high of 4.63 + or - 0.59 ppm over the entire 8 days. Some of the measured concentrations are higher than those reported elsewhere indicating the presence of some local source or sources for methane. This work has demonstrated the utility of a relatively simple multiplex gas chromatograph for the analysis of environmental samples. The technique should be applicable to other trace components in air through use of other selective modulators.

Valentin, J. R.↗

Atmospheric methane at Cape Meares - Analysis of a high-resolution data base and its environmental implications

Between 1979 and 1992 we took some 120,000 measurements of atmospheric methane at Cape Meares on the Oregon coast. The site is representative of methane concentrations in the northern latitudes (from 30 deg N to 90 deg N). The average concentration during the experiment was 1698 parts per billion by volume (ppbv). Methane concentration increased by 190 ppbv (or 11.9 percent) during the 13-year span of the experiment. The rate of increase was about 20 +/- 4 ppbv/yr in the first 2 yr and 10 +/- 2 ppbv/yr in the last 2 yr of the experiment, suggesting a substantial decline in the trend at northern middle and high latitudes. Prominent seasonal cycles were observed. During the year, the concentration stays more or less constant until May and then starts falling, reaching lowest levels in July and August, then rises rapidly to nearly maximum concentrations in October. Interannual variations with small amplitudes of 2-3 ppbv occur with periods of 1.4 and 6.5 yr.

Khalil, M. A. K.↗

Remote-Raman and Micro-Raman Studies of Solid CO2, CH4, Gas Hydrates and Ice

It is well known that on Mars CO2 is the principal constituent of the thin atmosphere and on a seasonal basis CO2 snow and frost coats the polar caps. Also over 25% of the Martian atmosphere freezes out and sublimes again each year. The Mars Odyssey Emission Imaging system (THEMIS) has discovered water ice exposed near the edge of Mars southern perennials cap. In recent years, it has been suggested that in Martian subsurface CO2 may exist as gas hydrate (8CO2 + 44 H2O) with melting temperature of 10C. Since the crust of Mars has been stable for enough time there is also a possibility that methane formed by magmatic processes and/or as a byproduct of anaerobic deep biosphere activity to have raised toward the planet s surface. This methane would have been captured and stored as methane hydrate, which concentrates methane and water. Determination of abundance and distribution of these ices on the surface and in the near surface are of fundamental importance for understanding Martian atmosphere, and for future exploration of Mars. In this work, we have evaluated feasibility of using remote Raman and micro-Raman spectroscopy as potential nondestructive and non-contact techniques for detecting solid CO2, CH4 gas, and gas hydrates as well as water-ice on planetary surfaces.

Sharma, S. K.↗

Methane transport mechanisms and isotopic fractionation in emergent macrophytes of an Alaskan tundra lake

The stable carbon isotopic composition of methane associated with and emitted by the two dominant emergent macrophytes abundant in the many Alaskan tundra lakes, Carex rostrata and Arctophila fulva, is determined. The carbon isotopic composition of the methane was -58.6 +/- 0.5 (n=2) for Arctophila and -66.6 +/- 2.5 (n=6) for Carex. The methane emitted by these species is depleted in C-13 by 12 per mil for Arctophila and 18 per mil for Carex relative to methane withdrawn from plant stems 1-2 cm below the waterline. The results suggest more rapid transport of (C-12)H4 relative to (C-13)H4 through plants to the atmosphere. Plant stem methane concentrations ranged from 0.2 to 4.0 percent in Arctophila, with an isotopic composition of -46.1 +/- 4.3 percent (n=8). Carex stem methane concentrations ranged from 150 to 1200 ppm, with an isotopic composition of -48.3 +/- 1.4 per mil (n=3).

Chanton, Jeffrey P.↗

Tropospheric methane from an Amazonian floodplain lake

The sources of methane and its flux to the troposphere from the Amazonian floodplain were investigated during the dry season of July and August 1985, using measurements of methane concentration gradients obtained aboard a houseboat laboratory anchored in Lago Calado, a stratified dendritic lake of about 6-sq km area located near the center of the Amazon Basin. Methane concentrations in the mixed layer of the lake were found to vary from 0.0001 to 0.0055 mM, with no consistent temporal trend. The measured methane flux from the surface of the open lake to the atmosphere averaged 27 mg CH4/sq m per day, consistent with the buildup in ambient methane in the nocturnal surface mixed layer of the troposphere. Ebullition contributed 70 percent to the average total flux. The source of methane to the lake and, ultimately, to the troposphere is the benthic sediments.

Crill, Patrick M.↗

Methane oxidation in Saanich Inlet during summer stratification

Saanich Inlet, British Columbia, an fjord on the southeast coast of Vancouver Island, typically stratifies in summer, leading to the formation of an oxic-anoxic interface in the water column and accumulation of methane in the deep water. The results of methane concentration measurements in the water column of the inlet at various times throughout the summer months in 1983 are presented. Methane gradients and calculated diffusive fluxes across the oxic-anoxic interface increased as the summer progressed. Methane distribution and consumption in Saanich Inlet were studied in more detail during August 1986. At this time, a typical summer stratification with an oxic-anoxic interface around 140 m was present. At the interface, steep gradients in nutrient concentrations, bacterial abundance and methane concentration were observed. Methane oxidation was detected in the aerobic surface waters and in the anaerobic deep layer, but highest rates occurred in a narrow layer at the oxic-anoxic interface. Estimated methane oxidation rates were suffcient to consume 100 percent of the methane provided by diffusive flux from the anoxic layer. Methane oxidation is thus a mechanism whereby atmospheric flux from anoxic waters is minimized.

Ward, B. B.↗

Concentration of methane in the troposphere deduced from 1951 infrared solar spectra

The 1-2 percent increase in tropospheric methane determined from gas chromatographic measurements since 1977 has important implications for atmospheric photochemistry and climate. To extend the measurement baseline, solar absorption spectra have been analyzed and mean troposphere CH4 mixing ratios for the years 1951 and 1981, and an average rate of CH4 increase of 1.1 + or - 0.2 percent per year is found for this period.

Rinsland, C. P.↗