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DOE OSTI2021

Beyond the usual suspects: methanogenic communities in eastern North American peatlands are also influenced by nickel and copper concentrations

Peatlands both accumulate carbon and release methane, but their broad range in environmental conditions means that the diversity of microorganisms responsible for carbon cycling is still uncertain. Here, we describe a community analysis of methanogenic archaea responsible for methane production in 17 peatlands from 36 to 53 N latitude across the eastern half of North America, including three metal-contaminated sites. Methanogenic community structure was analysed through Illumina amplicon sequencing of the mcrA gene. Whether metal-contaminated sites were included or not, metal concentrations in peat were a primary driver of methanogenic community composition, particularly nickel, a trace element required in the F 430 cofactor in methyl-coenzyme M reductase that is also toxic at high concentrations. Copper was also a strong predictor, likely due to inhibition at toxic levels and/or to cooccurrence with nickel, since copper enzymes are not known to be present in anaerobic archaea. Here, the methanogenic groups Methanocellales and Methanosarcinales were prevalent in peatlands with low nickel concentrations, while Methanomicrobiales and Methanomassiliicoccales were abundant in peatlands with higher nickel concentrations. Results suggest that peat-associated trace metals are predictors of methanogenic communities in peatlands.

54 ENVIRONMENTAL SCIENCES↗

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 NTRS1973

Spacecraft oxygen recovery system

A system which uses an electrochemical carbon dioxide concentrator to remove carbon dioxide from the cabin atmosphere and a Sabatier reactor to reduce carbon dioxide with hydrogen to form methane and water is described. Oxygen is recovered from water by means of a static-feed water electrolysis system. The hydrogen thus generated is reused in the carbon dioxide concentrator. The methane is a system byproduct. The CO2 removal reactions and the implementation of the CO2 concentration concept are discussed, and test results are examined.

Quattrone, P. D.↗

NASA NTRS2000

Synthetic spectra of simulated terrestrial atmospheres containing possible biomarker gases

NASA's proposed Terrestrial Planet Finder, a space-based interferometer, will eventually allow spectroscopic analyses of the atmospheres of extrasolar planets. Such analyses would provide information about the existence of life on these planets. One strategy in the search for life is to look for evidence of O3 (and hence O2) in a planet's atmosphere; another is to look for gases that might be present in an atmosphere analogous to that of the inhabited early Earth. In order to investigate these possibilities, we have calculated synthetic spectra for several hypothetical terrestrial-type atmospheres. The model atmospheres represent four different scenarios. The first two, representing inhabited terrestrial planets, are an Earth-like atmosphere containing variable amounts of oxygen and an early Earth-type atmosphere containing methane. In addition, two cases representing Mars-like and early Venus-like atmospheres were evaluated, to provide possible "false positive" spectra. The calculated spectra suggest that ozone could be detected by an instrument like Terrestrial Planet Finder if the O2 concentration in the planet's atmosphere is > or = 200 ppm, or 10(-3) times the present atmospheric level. Methane should be observable on an early-Earth type planet if it is present in concentrations of 100 ppm or more. Methane has both biogenic and abiogenic sources, but concentrations exceeding 1000 ppm, or 0.1% by volume, would be difficult to produce from abiogenic sources alone. High methane concentrations in a planet's atmosphere are therefore another potential indicator for extraterrestrial life.

NASA Discipline Exobiology↗

NASA NTRS1993

Deduction of emissions of source gases using an objective inversion algorithm and a chemical transport model

An inversion algorithm, constructed to deduce the emissions of a source gas required to produce a specified surface concentration, is applied to the observed surface concentrations of CFC 11, methylchloroform, and methane, using a two-dimensional chemical transport model. The information utilized for this deduction process is limited to the measured atmospheric concentration of the source gas, including the associated standard deviations of these measurements. In this way the amount of objective information available in these measurements is assessed. The algorithm is shown to be capable of producing a latitudinal emissions distribution as well as the error bounds on the deduced emission distribution. The 'ill posed' nature of this inverse problem is discussed as well as the implications this has on the spatial and temporal resolution at which emissions can be resolved. Finally, a methane emission distribution is deduced which has the expected seasonal variations and consistent with results from other, more subjective, deduction studies.

Brown, Margaret↗

NASA NTRS1983

A general circulation model study of atmospheric carbon monoxide

The carbon monoxide cycle is studied by incorporating the known and hypothetical sources and sinks in a tracer model that uses the winds generated by a general circulation model. Photochemical production and loss terms, which depend on OH radical concentrations, are calculated in an interactive fashion. The computed global distribution and seasonal variations of CO are compared with observations to obtain constraints on the distribution and magnitude of the sources and sinks of CO, and on the tropospheric abundance of OH. The simplest model that accounts for available observations requires a low latitude plant source of about 1.3 x 10 to the 15th g/yr, in addition to sources from incomplete combustion of fossil fuels and oxidation of methane. The globally averaged OH concentration calculated in the model is 750,000/cu cm. Models that calculate globally averaged OH concentrations much lower than this nominal value are not consistent with the observed variability of CO. Such models are also inconsistent with measurements of CO isotopic abundances, which imply the existence of plant sources.

Pinto, J. P.↗

NASA NTRS2022

Source and Chemistry of Hydroxymethanesulfonate (HMS) in Fairbanks, Alaska

Fairbanks, Alaska is a subarctic city with fine-particle (PM 2.5 ) concentrations that exceed air quality regulations in winter due to weak dispersion caused by strong atmospheric inversions, local emissions, and the unique chemistry occurring under the cold and dark conditions. Here we report on observations from the winters of 2020 and 2021, motivated by our pilot study which showed exceptionally high concentrations of fine particle hydroxy methane sulfonate (HMS) or related sulfur (IV) species (e.g., sulfite and bisulfite). We deployed an online Particle-Into-Liquid Sampler-Ion Chromatography (PILS-IC) in conjunction with a suite of instruments to determine HMS precursors (HCHO, SO 2 ) and aerosol composition in general, with the goal to characterize the sources and sinks of HMS in wintertime Fairbanks. PM 2.5 HMS comprised a significant fraction of PM 2.5 sulfur (26-41%) and overall PM 2.5 mass concentration (2.8-6.8%) during pollution episodes, substantially higher than what has been observed in other regions, likely due to the exceptionally low temperatures. HMS peaked in January, with lower concentrations in December and February, resulting from changes in precursors as well as meteorological conditions. Strong correlations with inorganic sulfate and organic mass during pollution events suggest HMS is linked to processes responsible for poor air quality episodes. These findings demonstrate unique aspects of air pollution formation in cold and humid atmospheres.

Fine-particle↗

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 NTRS2005

Thinking Like a Wildcatter: Prospecting for Methane in Arabia Terra, Mars

Methane has been detected in the martian atmosphere at a concentration of approximately 10 ppb. The lifetime of such methane against decomposition by solar radiation is approximately 300 years, strongly suggesting that methane is currently being released to the atmosphere. By analogy to Earth, possible methane sources on Mars include active volcanism, hot springs, frozen methane clathrates, thermally-matured sedimentary organic matter, and extant microbial metabolism. The discovery of any one of these sources would revolutionize our understanding of Mars.

Allen, C. C.↗

DOE OSTI2022

Cryptic Methane-Cycling by Methanogens During Multi-Year Incubation of Estuarine Sediment

As marine sediments are buried, microbial communities transition from sulfate-reduction to methane-production after sulfate is depleted. When this biogenic methane diffuses into the overlying sulfate-rich sediments, it forms a sulfate-methane transition zone (SMTZ) because sulfate reducers deplete hydrogen concentrations and make hydrogenotrophic methanogenesis exergonic in the reverse direction, a process called the anaerobic oxidation of methane (AOM). Microbial participation in these processes is often inferred from geochemistry, genes, and gene expression changes with sediment depth, using sedimentation rates to convert depth to time. Less is known about how natural sediments transition through these geochemical states transition in real-time. We examined 16S rRNA gene amplicon libraries and metatranscriptomes in microcosms of anoxic sediment from the White Oak River estuary, NC, with three destructively sampled replicates with methane added (586-day incubations) and three re-sampled un-amended replicates (895-day incubations). Sulfate dropped to a low value (∼0.3 mM) on similar days for both experiments (312 and 320 days, respectively), followed by a peak in hydrogen, intermittent increases in methane-cycling archaea starting on days 375 and 362 (mostly Methanolinea spp. and Methanosaeta spp., and Methanococcoides sp. ANME-3), and a methane peak 1 month later. However, methane δ 13 C values only show net methanogenesis 6 months after methane-cycling archaea increase and 4 months after the methane peak, when sulfate is consistently below 0.1 mM and hydrogen increases to a stable 0.61 ± 0.13 nM (days 553–586, n = 9). Sulfate-reducing bacteria (mostly Desulfatiglans spp. and Desulfosarcina sp. SEEP-SRB1) increase in relative abundance only during this period of net methane production, suggesting syntrophy with methanogens in the absence of sulfate. The transition from sulfate reduction to methane production in marine sediments occurs through a prolonged period of methane-cycling by methanogens at low sulfate concentrations, and steady growth of sulfate reducers along with methanogens after sulfate is depleted.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS2014

Analyzing Source Apportioned Methane in Northern California During DISCOVER-AQ-CA Using Airborne Measurements and Model Simulations

This study analyzes source apportioned methane (CH4) emissions and atmospheric concentrations in northern California during the Discover-AQ-CA field campaign using airborne measurement data and model simulations. Source apportioned CH4 emissions from the Emissions Database for Global Atmospheric Research (EDGAR) version 4.2 were applied in the 3-D chemical transport model GEOS-Chem and analyzed using airborne measurements taken as part of the Alpha Jet Atmospheric eXperiment over the San Francisco Bay Area (SFBA) and northern San Joaquin Valley (SJV). During the time period of the Discover-AQ-CA field campaign EDGAR inventory CH4 emissions were 5.30 Gg/day (Gg 1.0 109 grams) (equating to 1.9 103 Gg/yr) for all of California. According to EDGAR, the SFBA and northern SJV region contributes 30 of total emissions from California. Source apportionment analysis during this study shows that CH4 concentrations over this area of northern California are largely influenced by global emissions from wetlands and local/global emissions from gas and oil production and distribution, waste treatment processes, and livestock management. Model simulations, using EDGAR emissions, suggest that the model under-estimates CH4 concentrations in northern California (average normalized mean bias (NMB) -5 and linear regression slope 0.25). The largest negative biases in the model were calculated on days when hot spots of local emission sources were measured and atmospheric CH4 concentrations reached values 3.0 parts per million (model NMB -10). Sensitivity emission studies conducted during this research suggest that local emissions of CH4 from livestock management processes are likely the primary source of the negative model bias. These results indicate that a variety, and larger quantity, of measurement data needs to be obtained and additional research is necessary to better quantify source apportioned CH4 emissions in California and further the understanding of the physical processes controlling them.

Methane↗

NASA NTRS1992

Measurements and model calculations of HCl column amounts and related parameters over McMurdo during the austral spring in 1989

Solar spectra obtained from a ground-based Fourier transform infrared instrument at McMurdo (Antarctica) in the spring of 1989 have been analyzed to determine total HCl column amounts. A one-dimensional photochemical model was used to simulate the rate of recovery of HCl in the springtime. Low column amounts (about 1 x 10 exp 15 molecules/sq cm) were observed in early September and may be attributed to the heterogeneous conversion of HCl to active chlorine species during the polar night. The rate of recovery of HCl is consistent with its production by chlorine atoms reacting with methane and is dependent on concentrations of active chlorine species and NO molecules in the altitude region from 12 to 22 km. High HCl column amounts (about 7 x 10 exp 15 molecules/sq cm) were observed following recovery in late October, suggesting that the lower stratosphere in the polar region had descended relative to mid-latitudes and that the degree of dechlorination of the transported air was very small.

Liu, X.↗

NASA NTRS1997

Potential New Sensor for Use With Conventional Gas Carburizing

Diagnostics developed for in-situ monitoring of rocket combustion environments have been adapted for use in heat treating furnaces. Simultaneous, in-situ monitoring of the carbon monoxide, carbon dioxide, methane, water, nitrogen and hydrogen concentrations in the endothermic gas of a heat treating furnace has been demonstrated under a Space Act Agreement between NASA Lewis, the Heat Treating Network, and Akron Steel Treating Company. Equipment installed at the Akron Steel Treating Company showed the feasibility of the method. Clear and well-defined spectra of carbon monoxide, nitrogen and hydrogen were obtained by means of an optical probe mounted on the endothermic gas line of a gas generator inside the plant, with the data reduction hardware located in the basement laboratory. Signals to and from the probe were transmitted via optical fibers.

deGroot, W. A.↗

NASA NTRS2002

Orbital Noise in the Earth System is a Common Cause of Climate and Greenhouse-Gas Fluctuation

The mismatch between fossil isotopic data and climate models known as the cool-tropic paradox implies that either the data are flawed or we understand very little about the climate models of greenhouse warming. Here we question the validity of the climate models on the scientific background of orbital noise in the Earth system. Our study shows that the insolation pulsation induced by orbital noise is the common cause of climate change and atmospheric concentrations of carbon dioxide and methane. In addition, we find that the intensity of the insolation pulses is dependent on the latitude of the Earth. Thus, orbital noise is the key to understanding the troubling paradox in climate models.

Liu, H. S.↗

NASA NTRS2003

Estimating the Tropospheric Ozone Distribution by the Assimilation of Satellite Data

Tropospheric ozone is important to the environment, because it acts as a strong oxidant to control the concentrations of many reduced gases (methane, carbon monoxide, ... ), its radiative forcing plays a significant role in the greenhouse effect, and direct contact with ozone is harmful to human health. Tropospheric ozone, whose main sources are intrusion from the stratosphere and chemical production from source gases associated with urban pollution or biomass burning, varies on a wide range of spatial and temporal scales. Its transport and chemistry can be influenced by weather, seasonal, or multiannual variability. Despite the importance of tropospheric ozone, it contributes only about 10% of the total ozone loading in the atmosphere. Consequently, satellite instruments lose sensitivity below the stratospheric ozone peak, and provide little information about middle and lower tropospheric ozone. This talk will discuss recent modifications made to the satellite ozone data assimilation system at NASA's Data Assimilation Office (DAO) in order to provide better tropospheric ozone columns and profiles. We use a version of the system that assimilates only the data from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument. The quality of the assimilated ozone in the tropical troposphere is evaluated by comparison with independent observations obtained from the Southern Hemispheric Additional Ozonesondes (SHADOZ) network. It is shown that the quality of ozone fields is sensitive to the winds used in the transport model. Increasing the vertical resolution of the model also has a beneficial impact. The assimilated ozone in the lower troposphere was substantially improved by inclusion of tropospheric ozone production, loss, and dry deposition rates from the Harvard GEOS-CHEM model. The mechanisms behind these results will be examined and the implications for our understanding of tropospheric ozone will be discussed.

Hayashi, Hiroo↗

NASA NTRS2012

Miniaturized Laser Heterodyne Radiometer (LHR) for Measurements of Greenhouse Gases in the Atmospheric Column

This passive laser heterodyne radiometer (LHR) instrument simultaneously measures multiple trace gases in the atmospheric column including carbon dioxide (CO2) and methane (CH4), and resolves their concentrations at different altitudes. This instrument has been designed to operate in tandem with the passive aerosol sensor currently used in AERONET (an established network of more than 450 ground aerosol monitoring instruments worldwide). Because aerosols induce a radiative effect that influences terrestrial carbon exchange, simultaneous detection of aerosols with these key carbon cycle gases offers a uniquely comprehensive measurement approach. Laser heterodyne radiometry is a technique for detecting weak signals that was adapted from radio receiver technology. In a radio receiver, a weak input signal from a radio antenna is mixed with a stronger local oscillator signal. The mixed signal (beat note, or intermediate frequency) has a frequency equal to the difference between the input signal and the local oscillator. The intermediate frequency is amplified and sent to a detector that extracts the audio from the signal. In the LHR instrument described here, sunlight that has undergone absorption by the trace gas is mixed with laser light at a frequency matched to a trace gas absorption feature in the infrared (IR). Mixing results in a beat signal in the RF (radio frequency) region that can be related to the atmospheric concentration. For a one-second integration, the estimated column sensitivities are 0.1 ppmv for CO2, and <1 ppbv for CH4. In addition to producing a standalone ground measurement product, this instrument could be used to calibrate/validate four Earth observing missions: ASCENDS (Active Sensing of CO2 Emissions over Nights, Days, and Seasons), OCO-2 (Orbiting Carbon Observatory), OCO-3, and GOSAT (Greenhouse gases Observational SATellite). The only network that currently measures CO2 and CH4 in the atmospheric column is TCCON (Total Carbon Column Observing Network), and only two of its 16 operational sites are in the United States. TCCON data is used for validation of GOSAT data, and will be used for OCO-2 validation. While these Fourier-transform spectrometers (FTS) can measure the largest range of trace gases, the network is severely limited due to the high cost and extreme size of these instruments (these occupy small buildings and require personnel for operation). The LHR/AERONET instrument offers a significantly smaller (carry-on luggage size) autonomous instrument that can be incorporated into AERONET s much larger (450 instruments) global network.

Steel, Emily↗

NASA NTRS1991

Profiles of alpha 13 C and alpha D in methane from the lower stratosphere

Methane is an important greenhouse gas of biogenic and anthropogenic origin for which global budgets are being constructed from a variety of data. One approach to the global methane budget is the use of the stable isotopes C-13 and D, and the radionuclide C-14 as tracers. The authors measured the isotopic composition of methane from various sources and in tropospheric air for a number of locations. Here, the authors report on the isotopic composition of methane from the lower stratosphere. Measurements of this concentration in the stratosphere can yield estimates for the kinetic isotope effects in the methane destruction reactions. These effects have to be known for quantitative isotopic methane budgets.

Wahlen, Martin↗

NASA NTRS1994

On the relevance of the methane oxidation cycle to ozone hole chemistry

High concentrations of active chlorine are clearly responsible for the observed ozone depletion during the Antarctic polar spring. However, the mechanism behind the activation of chlorine from the reservoirs species HCl and ClONO2 and the maintenance of extremely high levels of active chlorine after polar sunrise is less well understood. Here, we focus on the influence of the methane oxidation cycle on 'ozone hole' chemistry through its effect on HOx and ClOx radicals. We demonstrate the great potential importance of the heterogeneous reaction HCl + HOCl yields Cl2 + H2O and the gasphase reaction ClO + CH3O2 yields ClOO + CH3O under sunlight conditions in polar spring. Under these conditions, the heterogeneous reaction is the main sink for HOx radicals. Through this channel, the HCl reservoir may be almost completely depleted. The gas phase reaction may control the levels of the CH3O2 radical, provided that high levels of ClO exist. Otherwise this radical initiates a sequence of reactions leading to a considerable loss of active chlorine. Moreover, the production of HOx radicals is reduced, and thereby the efficiency of the heterogeneous reaction limited. The two reactions together may accomplish the complete conversion of HCl into active chlorine, thereby leading to a rapid destruction of ozone.

Mueller, Rolf↗