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All sourcesNASA NTRSDOE OSTI
NASA NTRS1988

Stratospheric feedback from continued increases in tropospheric methane

Tropospheric concentrations of methane have increased steadily over the past ten years at an average rate of 16.5 ppbv per year, to a value in January 1988 of 1.69 ppmv. Measurements of CH sub 4 concentrations in air bubbles trapped in ice cores have shown concentrations of about 0.7 ppmv 200 years ago, with little further change for thousands of years before that. Interpolation earlier into this century suggests a concentration of about 1.1 to 1.2 ppmv in the 1940's. The only important pathway believed to be important for transfer of air from the troposphere to the stratosphere in through the tropical tropopause which is cold enough to reduce the mixing ratio of H sub 2 O in that air to about 3 ppmv. The only other major pathway for the delivery of H to the stratosphere is through the simultaneous injection of gaseous CH sub 4 in the same rising air. The formation of clouds in the stratosphere is dependent upon very low temperatures, and generally upon the amount of water vapor available. The possibility of a positive feedback exists, especially in well-oxidized methane air, that clouds are easier to form than earlier. This could mean enhancement of PSCs in both Antarctic and Arctic locations. Additional H sub 2 O in the stratosphere can also add to some of the greenhouse calculations.

Rowland, F. Sherwood↗
NASA NTRS1994

Spread of denitrification from 1987 Antarctic and 1988-1989 Arctic stratospheric vortices

Vertical profiles of N2O and NO(y) taken by the ER-2 outside the vortex are used to construct average vertical profiles of F(NO(y)) = NO(y)/(A-N2O), where A is the tropospheric content of N2O three years prior to the measurements. The southern hemisphere had less nitrous oxide in the range 400 less than Theta less than 470 K, by up to 25% relative to the northern hemisphere. F(NO(y)) is the ratio of NOy produced to N2O lost in a stratospheric air mass since entry from the troposphere. The profiles of F(NO(y)) have the following characteristics: (1) Relative to 1991-1992, a year without denitrification inside or outside the vortex, the northern hemisphere in 1988-1989 showed denitrification outside the vortex ranging up to 25% and averaging 17% above Theta = 425 K. (2) Relative to the northern hemisphere in 1991-1992, the southern hemisphere in 1987 showed denitrification outside the vortex ranging up to 32% and averaging 20% above Theta = 400 K. (3) Below Theta = 400 K the southern hemisphere showed enhancements of F(NO(y)) relative to the northern hemisphere in 1991-1992 ranging up to 200% at Theta = 375 K, outside the vortex. Corresponding profiles of residual water, R(H2O) = H2O - 2(1.6 - CH4), are considered and shown to be consistent with those of F(NO(y)) in the sense that they show deficits outside the Antarctic vortex, which was both dehydrated and denitrified, but not outside the 1988-1989 Arctic vortex, which was denitrified but not dehydrated. R(H2O) is the water content of stratospheric air with the contribution from methane oxidation subtracted. Comparison of F(NO(y)) and R(H2O) below 400 K outside the Antarctic vortex leads to the suggetion that dehydration in the Antarctic vortex occurs by the sedimentation of ice crystals large enough to fall out of the stratosphere, whereas denitrification occurs mainly on mixed nitric acid-water crystals which evaporate below the base of the vortex at Theta = 400 K but above the tropopause.

Tuck, A. F.↗
DOE OSTI2024

Microbial Community Changes across Time and Space in a Constructed Wetland

Constructed wetlands are artificial ecosystems designed to replicate natural wetland processes. Microbial communities play a pivotal role in cycling essential elements, particularly sulfur, which is crucial for trace metal fixation and remobilization in these ecosystems. By their response to their environment, microbial communities act as biological indicators of the wetland performance. To address knowledge gaps pertinent to the changes in trace metal bioavailability in relation to microbial activities in the H-02 constructed wetland, we performed this study to investigate temporal and spatial variations in microbial communities by using molecular biology tools. Quantitative polymerase chain reaction and next generation sequencing techniques were employed to analyze archaeal and bacterial groups associated with sulfur and methane cycling. Alpha diversity indices were used to assess species richness, evenness, and dominance. Results indicated high gene abundance of Desulfuromonas (5.37 × 10 6 g.cell –1 ), methane oxidizing bacteria (6.92 × 10 6 g.cell –1 ), and methanogenic microorganisms (3.02 × 10 5 g.cell –1 ) during cool months. Warm months were marked by sulfate reducing bacteria dominance (3.31 × 10 6 g.cell –1 ), potentially due to competitive interactions and environmental conditions, higher temperatures, and lower redox potential. Spatial variability among microbial groups was insignificant, but trends in gene abundance indicated complex factors influencing these groups. Next generation sequencing data demonstrated Firmicutes as the most abundant phylum with over 50% regardless of the season or sampling location. Cool months exhibited higher alpha diversity than warm months. Overall, this study showed that seasonal changes significantly impacted the microbial communities in the H-02 constructed wetland that are associated with the sulfur cycle and eventually trace metal biogeochemistry, revealing two distinct mechanisms of the sulfur cycle between the two main seasons, whereas spatial variability effects were not conclusive.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

On the Relationship Between Methane Production in Anaerobic Incubations of Peat Material and In Situ Methane Emissions

Anaerobic incubations of peat have been widely used to explore soil processes, but this in vitro technique raises many questions as to how well it reproduces in situ conditions. To investigate this, we conducted 60–100 days (+25 days pre‐incubation) anaerobic, temperature‐controlled incubation experiments across a temperature range of 1–26°C on samples from bog and fen habitats, at two different depths (9–19 and 25–35 cm). Here, we observed exponential increases in CO 2 and methane production with temperature in all conditions. We then compared field‐based measurements of methane emission with modeled expectations by extrapolating incubation‐determined methane production rates based on (a) soil temperature profiles, (b) the observed incubation temperature‐methane production relationship, and (c) seasonal thaw depth from each site. The resulting incubation‐extrapolated methane production agreed with measured emission rates within a factor of two at both sites and corresponded to 182 ± 54% and 59 ± 14% of the measured average yearly fluxes from the field for the bog and fen, respectively. The underestimation of fen methane fluxes may be due to the lack of living plant root‐derived dissolved organic carbon inputs in incubations, a key process in fens. Conversely, the overestimation in bogs could be attributed to methane oxidation in the field, which is absent in anaerobic incubation conditions. Nonetheless incubations predicted greenhouse gas emissions from a northern peatland within a factor of two.

Biological and medical sciences,Geosciences,Enviro↗
DOE OSTI2024

Novel, active, and uncultured hydrocarbon-degrading microbes in the ocean

ABSTRACT Given the vast quantity of oil and gas input to the marine environment annually, hydrocarbon degradation by marine microorganisms is an essential ecosystem service. Linkages between taxonomy and hydrocarbon degradation capabilities are largely based on cultivation studies, leaving a knowledge gap regarding the intrinsic ability of uncultured marine microbes to degrade hydrocarbons. To address this knowledge gap, metagenomic sequence data from the Deepwater Horizon (DWH) oil spill deep-sea plume was assembled to which metagenomic and metatranscriptomic reads were mapped. Assembly and binning produced new DWH metagenome-assembled genomes that were evaluated along with their close relatives, all of which are from the marine environment (38 total). These analyses revealed globally distributed hydrocarbon-degrading microbes with clade-specific substrate degradation potentials that have not been reported previously. For example, methane oxidation capabilities were identified in all Cycloclasticus . Furthermore, all Bermanella encoded and expressed genes for non-gaseous n -alkane degradation; however, DWH Bermanella encoded alkane hydroxylase, not alkane 1-monooxygenase. All but one previously unrecognized DWH plume member in the SAR324 and UBA11654 have the capacity for aromatic hydrocarbon degradation. In contrast, Colwellia were diverse in the hydrocarbon substrates they could degrade. All clades encoded nutrient acquisition strategies and response to cold temperatures, while sensory and acquisition capabilities were clade specific. These novel insights regarding hydrocarbon degradation by uncultured planktonic microbes provides missing data, allowing for better prediction of the fate of oil and gas when hydrocarbons are input to the ocean, leading to a greater understanding of the ecological consequences to the marine environment. IMPORTANCE Microbial degradation of hydrocarbons is a critically important process promoting ecosystem health, yet much of what is known about this process is based on physiological experiments with a few hydrocarbon substrates and cultured microbes. Thus, the ability to degrade the diversity of hydrocarbons that comprise oil and gas by microbes in the environment, particularly in the ocean, is not well characterized. Therefore, this study aimed to utilize non-cultivation-based ‘omics data to explore novel genomes of uncultured marine microbes involved in degradation of oil and gas. Analyses of newly assembled metagenomic data and previously existing genomes from other marine data sets, with metagenomic and metatranscriptomic read recruitment, revealed globally distributed hydrocarbon-degrading marine microbes with clade-specific substrate degradation potentials that have not been previously reported. This new understanding of oil and gas degradation by uncultured marine microbes suggested that the global ocean harbors a diversity of hydrocarbon-degrading bacteria, which can act as primary agents regulating ecosystem health.

Howe, Kathryn L.↗
DOE OSTI2024

Harnessing photoautotroph-methanotroph interactions for biogas conversion to fuels and chemicals using binary consortia (Project Final Technical Report)

Industrial, municipal, and agricultural waste streams containing stranded organic carbon represent a significant and underutilized feedstock to produce fuels and chemicals. With anaerobic digestion deployed at large scales to capture organic waste streams, over 6 million tons of biogas are available today. However, the utilization of biogas represents a significant challenge due to its low pressure and presence of contaminants such as H 2 S, ammonia, and volatile organic carbon compounds. To tap into this immense potential, effective biotechnologies that co-utilize both CO 2 and CH 4 are needed. Recent studies demonstrated that, in nature, microbial communities have developed a highly efficient way to recover energy and capture carbon from both CH 4 and CO 2 through metabolic coupling of methane oxidation to oxygenic photosynthesis. Using two synthetic methanotroph – photoautotroph (M-P) co-cultures that exhibit stable growth under a broad range of cultivation conditions, in this project we proposed to harness the interspecies interactions within these cocultures for biogas conversion to fuels and chemicals. To facilitate this overarching objective, we aim to develop experimental and computational tools to gain qualitative and quantitative understandings on the interactions and dynamics of the coculture at both systems and molecular levels, and to validate our findings through experiments and mutant development. The fundamental understanding on the interactions and dynamics of the photoautotroph-methanotroph will lay the foundation for the design and optimization of synthetic binary consortia for production of fuels and chemicals from biogas. We expect the knowledge gained from this project may be generally applicable to other cross-feeding binary consortium, and the tools developed can be adapted to study the interactions and dynamics of other multi-organism platforms.

09 BIOMASS FUELS↗
NASA NTRS1973

A photochemical theory of tropospheric ozone

We present a photochemical theory for tropospheric ozone in which the methane oxidation chain constitutes a large local source. This source produces about one trillion odd oxygen molecules per square centimeter per second and implies a photochemical lifetime for ozone of about 1 day, much shorter than characteristic mixing times. The photochemical model reproduces the altitude and seasonal dependence of ozone at 30 deg N. It also gives qualitative agreement with observed day-to-day variations of the ozone density.

Chameides, W.↗
NASA NTRS1976

Greenhouse effects due to man-made perturbations of trace gases

Nitrous oxide, methane, ammonia, and a number of other trace constituents of the earth's atmosphere have infrared absorption bands in the spectral range from 7 to 14 microns. Despite their small amounts, these gases can have a significant effect on the thermal structure of the atmosphere by transmitting most of the thermal radiation from the earth's surface to the lower atmosphere. In the present paper, this greenhouse effect is computed for a number of trace gases. The nature and climatic implications of possible changes in the concentrations of N2O, CH4, NH3, and HNO3 are discussed.

Wang, W. C.↗
NASA NTRS1983

Distribution, abundance and carbon isotopic composition of gaseous hydrocarbons in Big Soda Lake, Nevada - An alkaline, meromictic lake

The study of the distribution and isotopic composition of low molecular weight hydrocarbon gases at the Big Soda Lake, Nevada, has shown that while neither ethylene nor propylene were found in the lake, ethane, propane, isobutane and n-butane concentrations all increased with water column depth. It is concluded that methane has a biogenic origin in both the sediments and the anoxic water column, and that C2-C4 alkanes have biogenic origins in the monimolimnion water and shallow sediments. The changes observed in delta C-13/CH4/ and CH4/(C2H6 + C3H8) with depth in the water column and sedimeents are probably due to bacterial processes, which may include anaerobic methane oxidation and different rates of methanogenesis, and C2-to-C4 alkane production by microorganisms.

Oremland, R. S.↗
NASA NTRS1984

Implications of the stratospheric water vapor distribution as determined from the Nimbus 7 LIMS experiment

The LIMS experiment on Nimbus 7 has provided new results on the stratospheric water vapor distribution. The data show (1) a latitudinal gradient with mixing ratios that increase by a factor of 2 from equator to + or - 60 degrees at 50 mb, (2) most of the time there is a fairly uniform mixing ratio of 5 ppmv at high latitudes, but more variation exists during winter, (3) a well-developed hygropause at low to midlatitudes of the lower stratosphere, (4) a source region of water vapor in the upper stratospehere to lower mesosphere that is consistent with methane oxidation chemistry, at least within the uncertainties of the data, (5) an apparent zonal mean H2O distribution that is consistent with the circulation proposed by Brewer in 1949, and (6) a zonal mean distribution in the lower stratosphere that is consistent with the idea of quasi-isentropic transport by eddies in the meridional direction. Limits to the use of the data in the refinement of our understanding of the stratospheric water vapor budget are noted.

Remsberg, E. E.↗
NASA NTRS1986

Emissions of N2O, CH4 and CO2 from tropical forest soils

Emissions of nitrous oxide, methane, and carbon dioxide were measured at diverse locations in tropical forests of Brazil, Ecuador, and Puerto Rico using a static open chamber technique. Mean fluxes to the atmosphere were 1.7 x 10 to the 10th, -0.7 x 10 to the 10th, and 1.5 x 10 to the 14th molecules/sq cm per s for N2O, CH4, and CO2, respectively. The data indicate that tropical forests contribute a significant fraction of the global source for atmospheric N2O, about 40 percent of the current source, and possibly 75 percent of the preindustrial source. Methane is consumed by soils on average, but the sink is an insignificant part (less than 5 percent) of the atmospheric cycle for the gas. Emissions of CO2 from forest soils are higher at equatorial sites than at middle or high latitudes, as expected from ecological considerations. Soils emit CO2 at rates more than twice as large as the rate of carbon infall in litter; hence much of the emitted CO2 must arise from root metabolism.

Keller, Michael↗
NASA NTRS1988

CH(A, B-X) fluorescence from vacuum ultraviolet excitation of CH3

The fluorescence due to single-photon and two-photon excitation of CH3 produced by the reaction of CH4 with F or Cl in a flow tube is investigated experimentally. The excitation source is an excimer laser operating with pulse duration 6 nsec and repetition rate 20 Hz, and the fluorescence is observed using a 0.25-m spectrometer and a 1024-channel diode array; the results are presented graphically. Emission is detected at 157 nm (with approximate cross section 8 x 10 to the -19th sq cm) and 193 nm, but not at 248 nm. The applicability of these data to studies of hydrocarbon combustion, the methane oxidation cycle in the atmosphere, interstellar molecule formation, and diamond film fabrication is indicated.

Ye, Chao↗
NASA NTRS1990

A comparison of ER-2 measurements of stratospheric water vapor between the 1987 Antarctic and 1989 Arctic Airborne missions

Vertical profiles of water vapor inside the Antarctic vortex have been compared with those taken outside it over Punta Arenas (53 deg S, 71 deg W). A similar exercise was performed with Arctic vortex profiles and those taken over Stavanger (59 deg N, 6 deg E). Residual water, defined as the stratospheric water vapor mixing ratio with the contribution from methane oxidation subtracted, is also shown as profiles inside and outside the vortex for both missions. The Arctic and Antarctic profiles of water vapor and residual water are compared. Locally dehydrated air was evident both inside and outside the Antarctic vortex, but such dehydration was not evident in and around the Arctic vortex. Arctic profiles of residual water are consistent with nontropical entry for some air.

Kelly, K. K.↗
NASA NTRS1990

Ecosystem approach to a global nitrous oxide budget

An approach using relationships among soil fertility, nitrogen cycling, and nitrous oxide production is presented in order to estimate nitrous oxide flux from humid tropical forests. The effects of human disturbance are also investigated. It is noted that recent estimates suggest that 6-10 million ha. of tropical forest are cleared permanently each year. The results of measurements of nitrous oxide flux from cleared and burned sites in Costa Rica and Brazil, in conjunction with satellite-based classifications of ecosystem types, are used to calculate average hourly fluxes for a given region. In the NASA intensive site near Manaus, Brazil, it was found that although pasture areas cover only 11 percent of the region they account for 40 percent of the nitrous oxide flux. This analysis of the fluxes of trace gases through consideration of the gradients of factors that control both fluxes and ecosystem properties and processes will prove useful for extrapolating fluxes and for calculating budgets of nitrous oxide, methane, nonmethane hydrocarbons, and carbon dioxide.

Matson, P. A.↗
NASA NTRS1993

A carbon isotope mass balance for an anoxic marine sediment: Isotopic signatures of diagenesis

A carbon isotope mass balance was determined for the sediments of Cape Lookout Bight, NC to constrain the carbon budgets published previously. The diffusive, ebullitive and burial fluxes of sigma CO2 and CH4, as well as the carbon isotope signatures of these fluxes, were measured. The flux-weighted isotopic signature of the remineralized carbon (-18.9 plus or minus 2.7 per mil) agreed with the isotopic composition of the remineralized organic carbon determined from the particulate organic carbon (POC) delta(C-13) profiles (-19.2 plus or minus 0.2), verifying the flux and isotopic signature estimates. The measured delta(C-13) values of the sigma CO2 and CH4 diffusive fluxes were significantly different from those calculated from porewater gradients. The differences appear to be influenced by methane oxidation at the sediment-water interface, although other potential processes cannot be excluded. The isotope mass balance provides important information concerning the locations of potential diagenetic isotope effects. Specifically, the absence of downcore change in the delta(C-13) value of the POC fraction and the identical isotopic composition of the POC and the products of remineralization indicate that no isotopic fractionation is expressed during the initial breakdown of the POC, despite its isotopically heterogeneous composition.

Boehme, Susan E.↗
NASA NTRS1999

Observations of Middle Atmosphere CO from the UARS ISAMS during the Early Northern Winter 1991/92

Structure and kinematics of carbon monoxide in the upper stratosphere and lower mesosphere (10-0.03 hPa) are studied for the early northern winter 1991/92 using the Upper Atmosphere Research Satellite Improved Stratospheric and Mesospheric Sounder (ISAMS) measurements. The study is aided by data from a 6-week parameterized-chemistry run of the Goddard Space Flight Center 3D Chemistry and Transport Model (CTM), initialized on 8 December 1991. Generally, CO mixing ratios increase with height due to the increasing source contribution from CO, photolysis. In the tropical upper stratosphere. however, a local maximum in CO mixing ratio occurs. A simple photochemical model is used to show that this feature results largely from methane oxidation. In the extratropics the photochemical lifetime of CO is long, and therefore its evolution is dictated by large-scale motion of air. evidenced by strong correlation with Ertel potential vorticity. This makes CO one of the few useful observable tracers at the stratopause level and above. Thus CO maps are used to study the synoptic evolution of the polar vortex in early January 1992. Modified Lagrangian mean mixing diagnostics are applied to ISAMS and CTM data to examine the strength of the mixing barrier at the polar vortex edge. It is demonstrated that planetary wave activity weakens the barrier. promoting vortex erosion. The vortex erosion first appears in the lower mesosphere and subsequently descends through the upper stratosphere. and is attributed to effects of planetary wave dissipation. Agreement between ISAMS and CTM is good in the horizontal distribution of CO throughout the examined period, but vertical CO gradients in the CTM weaken with time relative to the ISAMS observations.

Allen, D. R.↗
NASA NTRS2000

Hydrogen Biogeochemistry in Anaerobic and Photosynthetic Ecosystems

The simple biochemistry of molecular hydrogen is central to a large number of microbial processes, affecting the interaction of organisms with each other and with the environment. In anoxic sediments, a great majority of microbial redox processes involve hydrogen as a reactant, product or potential by-product. Accordingly, the energetics (thermodynamics) of each of these processes is affected by variations in local H2 concentrations. It has long been established that this effect is important in governing microbe-microbe interactions and there are multiple demonstrations that "interspecies hydrogen transfer" can alter the products of, inhibit/stimulate, or even reverse microbial metabolic reactions. In anoxic sediments, H2 concentrations themselves are thought to be controlled by the thermodynamics of the predominant H2-consuming microbial process. In sediments from Cape Lookout Bight, this relationship quantitatively describes the co-variation of H2 concentrations with temperature (for methanogens and sulfate reducers) and with sulfate concentration (for sulfate reducers). The quantitative aspect is import= for two reasons: 1) it permits the modeling of H2-sensitive biogeochemistry, such as anaerobic methane oxidation or pathways of organic matter remineralization, as a function of environmental controls; 2) for such a relationship to be observed requires that intracellular biochemistry and bioenergetics are being directly expressed in a component of the extracellular medium. H2 could therefore be utilized a non-invasive probe of cellular energetic function in intact microbial ecosystems. Based on the latter principle we have measured down-core profiles of H2 and other relevant physico-chemical parameters in order to calculate the metabolic energy yields (DG) that support microbial metabolism in Cape Lookout Bight sediments. Methanogens in this system apparently function with energy yields significantly smaller than the minimum requirements suggested by pure culture studies. Our recent work has extended the study of hydrogen to cyanobacterial mat communities. The large amounts of reducing power generated during photosynthetic activity carry the potential to contribute a swamping term to the H2 economy of the anaerobic microbial populations within the mat - and thereby to alter the population structure and biogeochemical function of the mat as a whole. In hypersaline microbial mats, we observe a distinct diel cycle in H2 production and a substantial corresponding flux. On an early Earth dominated by microbial mats, this transmission of photosynthetic reducing power may have carried important implications for both biospheric and atmospheric evolution.

Hoehler, Tori M.↗
NASA NTRS2000

Structure of Laminar Permanently Blue, Opposed-Jet Ethylene-Fueled Diffusion Flames

The structure and state relationships of laminar soot-free (permanently blue) ethylene-fueled diffusion flames at various strain rates were studied both experimentally and computationally using an opposed-jet configuration. Measurements of gas velocities, temperatures, and compositions were carried out along the stagnation stream line. Corresponding predictions of flame structure were obtained, based on numerical simulations using several contemporary reaction mechanisms for methane oxidation. Flame conditions studied included ethylene-fueled opposed-jet diffusion flames having stoichiometric mixture fractions of 0.7 with measurements involving strain rates of 60-240/s and predictions involving strain rates of 0-1140/s at normal temperature and pressure. It was found that measured major gas species concentrations and temperature distributions were in reasonably good agreement with predictions using mechanisms due to GRI-Mech and Peters and that effects of preferential diffusion significantly influence flame structure even when reactant mass diffusivities are similar. Oxygen leakage to fuel-rich conditions and carbon monoxide leakage to fuel-lean conditions both increased as strain rates increased. Furthermore, increased strain rates caused increased fuel concentrations near the flame sheet, decreased peak gas temperatures, and decreased concentrations of carbon dioxide and water vapor throughout the flames. State relationships for major gas species and gas temperatures were found to exist over a broad range of strain rates, providing potential for significant computational simplifications for modeling purposes in some instances.

Lin, K.-C.↗