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At least 541 records · Page 30

Numerical Study of Contaminant Effects on Combustion of Hydrogen, Ethane, and Methane in Air

A numerical study was performed to assess the effects of vitiated air on the chemical kinetics of hydrogen, ethane, and methane combustion with air. A series of calculations in static reacting systems was performed, where the initial temperature was specified and reactions occurred at constant pressure. Three different types of test flow contaminants were considered: NP, H2O, and a combustion of H2O and CO2. These contaminants are present in the test flows of facilities used for hypersonic propulsion testing. The results were computed using a detailed reaction mechanism and are presented in terms of ignition and reaction times. Calculations were made for a wide range of contaminant concentrations, temperatures and pressures. The results indicate a pronounced kinetic effect over a range of temperatures, especially with NO contamination and, to a lesser degree, with H2O contamination. In all cases studied, CO2 remained kinetically inert, but had a thermodynamic effect on results by acting as a third body. The largest effect is observed with combustion using hydrogen fuel, less effect is seen with combustion of ethane, and little effect of contaminants is shown with methane combustion.

Lai, H. T.↗

Numerical study of contaminant effects on combustion of hydrogen, ethane, and methane in air

A numerical study was performed to assess the effects of vitiated air on the chemical kinetics of hydrogen, ethane, and methane combustion with air. A series of calculations in static reacting systems was performed, where the initial temperature was specified and reactions occurred at constant pressure. Three different types of test flow contaminants were considered: NO, H2O, and a combination of H2O and CO2. These contaminants are present in the test flows of facilities used for hypersonic propulsion testing. The results were computed using a detailed reaction mechanism and are presented in terms of ignition and reaction times. Calculations were made for a wide range of contaminant concentrations, temperatures and pressures. The results indicate a pronounced kinetic effect over a range of temperatures, especially with NO contamination and, to a lesser degree, with H2O contamination. In all cases studied, CO2 remained kinetically inert, but had a thermodynamically effect on results by acting as a third body. The largest effect is observed with combustion using hydrogen fuel, less effect is seen with combustion of ethane, and little effect of contaminants is shown with methane combustion.

Lai, H. T.↗

Biogeochemistry simulations for the Salt Marsh Accretion Response to Temperature eXperiment (SMARTX)

Coastal ecosystems have been largely ignored in Earth system models but are important zones for carbon and nutrient processing. Interactions between water, microbes, soil, sediments, and vegetation are important for mechanistic representation of coastal processes and ecosystem function. To investigate the role of these feedbacks, we used a reactive transport model (PFLOTRAN) that has the capability to be connected to the Energy Exascale Earth System Model (E3SM). PFLOTRAN was used to incorporate redox reactions and track chemical species important for coastal ecosystems as well as define simple representations of vegetation dynamics. Our goal was to incorporate oxygen flux, salinity, pH, sulfur cycling, and methane production along with plant-mediated transport of gases and tidal flux. Using porewater profile and incubation data for model calibration and evaluation, we were able to create depth-resolved biogeochemical soil profiles for saltmarsh habitat and use this updated representation to simulate direct and indirect effects of elevated CO2 and temperature on subsurface biogeochemical cycling. We found that simply changing the partial pressure of CO2 or increasing temperature in the model did not fully reproduce observed changes in the porewater profile, but the inclusion of plant or microbial responses to CO2 and temperature manipulations was more accurate in representing porewater concentrations. This indicates the importance of characterizing tightly coupled vegetation-subsurface processes for developing predictive understanding and the need for measurement of plant-soil interactions on the same time scale to understand how hotspots or moments are generated.Included in this data package are PFLOTRAN input (PFLOTRAN input files and chemical database) files for simulating single column biogeochemistry, root, and tide interactions at the Global Change Research Wetland (Kirkpatrick Marsh; Edgewater, MD). The biogeochemical network includes soil organic matter decomposition, nitrogen, iron, and sulfur cycling, and methanogenesis. Reduced species can be oxidized and plant processes include oxygen and nutrient priming, methane release, and nutrient uptake.Inputs:TAI_database.dat - geochemical database for reactions, more information on database structure and variables can be found here https://www.pflotran.org/documentation/user_guide/cards/pages/geochemical_database.htmlswamp.in - input file for biogeochemical network in PFLOTRANswamp_eCO2.in - input file for biogeochemical network in PFLOTRAN with input gas partial pressures/concentrations adjusted for elevated CO2 treatmentsOutputs:swamp_obs_0.tec - hourly porewater concentrations from from multiple depths in the soil columnswamp_eCO2_obs_0.tec - hourly porewater concentrations from multiple depths in the soil column for elevated CO2 treatmentsPFLOTRAN code access: https://github.com/fmyuan/pflotran-elm-interface.git

54 ENVIRONMENTAL SCIENCES↗

Eddy Correlation Flux Measurement System (ECOR) Instrument Handbook

The eddy correlation (ECOR) flux measurement system provides in situ, half-hour measurements of surface turbulent fluxes of momentum, sensible heat, latent heat, and carbon dioxide (CO 2 ) at the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility sites. ARM’s ECORs also historically measured methane fluxes at Utqiaġvik and Oliktok Point, Alaska. The fluxes are obtained with the eddy covariance technique, which involves correlation of the vertical wind component with the horizontal wind component, the air temperature, the water vapor density, and the CO 2 concentration.

54 ENVIRONMENTAL SCIENCES↗

Methane flux across the air-water interface - Air velocity effects

Methane loss to the atmosphere from flooded wetlands is influenced by the degree of supersaturation and wind stress at the water surface. Measurements in freshwater ponds in the St. Marks Wildlife Refuge, Florida, demonstrated that for the combined variability of CH4 concentrations in surface water and air velocity over the water surface, CH4 flux varied from 0.01 to 1.22 g/sq m/day. The liquid exchange coefficient for a two-layer model of the gas-liquid interface was calculated as 1.7 cm/h for CH4 at air velocity of zero and as 1.1 + 1.2 v to the 1.96th power cm/h for air velocities from 1.4 to 3.5 m/s and water temperatures of 20 C.

Sebacher, D. I.↗

Transient heat transfer from shrinking LOX-drop

In order to achieve prescribed experimental conditions in wind tunnels, the nitrogen-oxygen mixture is enriched by injection of liquid oxygen (LOX) upstream of methane burners. The objective of the study is to determine the LOX drop evaporation rate, which is dominated by heat transfer from the air stream (mass transfer mechanism can be later coupled with the solution from the present work). Since the concentration of drops in the surrounding gas is quite high, the concept of infinite medium cannot be utilized. Drop evaporation, as part of system's mass balance, is an important source-term in the finite-difference 2/3-dimensional network terms of laboratory-system (Eulerian) coordinates, while individual drop behavior, including its thermal history, is analyzed in Lagrangian coordinates.

Kondic, Nenad N.↗

In Situ Measurements of N2O and CH4 During SOLVE on the ER-2 Using a New Tunable Diode Laser Instrument

This report is the final report for Cooperative Agreement NCC2-1105: 'In Situ Measurements of N2O and CH4 during SOLVE on the ER-2 using a new tunable diode laser instrument.' The tasks outlined in the proposal are listed below with a brief comment. The publications and the conference presentations are listed. Finally the important publications are attached. The Cooperative Agreement made possible a research effort to produce high precision and high accuracy in situ measurements of methane and nitrous oxide on the ER-2 during the SOLVE field campaign and to analyze these measurements. These measurements of CH4 and N2O were of utmost importance to studies of the ozone losses in the Arctic winter and spring. The concentrations measured over a large spatial and temporal range allowed the separation of the dynamical and chemical ozone loss. The most important results of the SOLVE program were contained in two scientific papers. This Cooperative Agreement allowed the participation of the Argus instrument in the program and the analysis of the data.

Jost, Hansjurg↗

Pre-industrial to End 21st Century Projections of Tropospheric Ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337+/-23 Tg, the ensemble mean burden for 1850 time slice is approx. 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16 %) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

Troposphere↗

Hythane production from brewery wastewater‐generated biogas using a membrane electrochemical cell

Converting organic wastes into hythane, a blend of hydrogen (5% to 25%) and methane (75% to 95%), will not only reduce waste discharge but also maximize energy recovery. Herein, a membrane electrochemical cell was investigated to produce hythane from biogas generated in anaerobic digestion of brewery wastewater (BW). The key parameters including current densities, electrolyte concentrations, and biogas flow rates were examined in batch tests. Under an optimal condition (210 mA, 100 mM electrolyte, 1 mL min −1 of biogas flow), the system achieved the production of hythane containing 70.6% ± 1.1% CH 4 , 27.3% ± 0.5% H 2 , and 2.1% ± 1.6% CO 2 (corresponding to 91.1% ± 6.4% CO 2 removal). Meanwhile, the H 2 S concentration was decreased from 513 to 2 ppm, 99.9% ± 0.2% removal. Energy efficiency of this system was estimated 61.8% ± 10.7%, and energy output increased by 54.4% ± 10.6% with biogas upgrading to hythane. Furthermore, these results encourage further exploration of electrochemical approach for simultaneous biogas upgrading and hythane production.

Rao, Yue [Washington University in St. Louis, MO (↗

Effect of swirl on premixed combustion

Combustion in a premixed swirl combustor composed of confined concentric jets (5 cm and 10 cm diameter) were studied. The inner flow is fuel and air; the outer flow is air. Both flows may contain swirl either in the same or opposite directions. The combustor operates at one atmosphere without preheat; methane and propane were used as fuels. Related analyses and experiments were also performed for water flows and isotherm air flows. In these studies, a number of important concepts regarding premixing/prevaporized, swirl stabilized combustion were developed. Some of the more significant are discussed.

Gouldin, F. C.↗

Methane and nitrous oxide fluxes in native, fertilized and cultivated grasslands

Measurements of CH4 uptake and N2O emissions in native, nitrogen-fertilized, and wheat-growing prairie soils from spring to late autumn, 1990 are reported. It is found that nitrogen fertilization and cultivation can both decrease CH4 uptake and increase N2O production, thereby contributing to the increasing atmospheric concentrations of these gases.

Mosier, A.↗

Reduced Equations for Calculating the Combustion Rates of Jet-A and Methane Fuel

Simplified kinetic schemes for Jet-A and methane fuels were developed to be used in numerical combustion codes, such as the National Combustor Code (NCC) that is being developed at Glenn. These kinetic schemes presented here result in a correlation that gives the chemical kinetic time as a function of initial overall cell fuel/air ratio, pressure, and temperature. The correlations would then be used with the turbulent mixing times to determine the limiting properties and progress of the reaction. A similar correlation was also developed using data from NASA's Chemical Equilibrium Applications (CEA) code to determine the equilibrium concentration of carbon monoxide as a function of fuel air ratio, pressure, and temperature. The NASA Glenn GLSENS kinetics code calculates the reaction rates and rate constants for each species in a kinetic scheme for finite kinetic rates. These reaction rates and the values obtained from the equilibrium correlations were then used to calculate the necessary chemical kinetic times. Chemical kinetic time equations for fuel, carbon monoxide, and NOx were obtained for both Jet-A fuel and methane.

Molnar, Melissa↗

Concentration Field of Reactants and Products Species in a Reacting Vortex Ring

The proposed paper will present experimental and numerical results on the concentration fields of both reactants and products species in a reacting vortex ring that is generated from the interaction between a diffusion flame and a laminar vortex ring. Flame-vortex interactions are canonical configurations used to study the underlying processes occurring in complicated turbulent reacting flows. This type of configuration contains many of the fundamental aspects of the coupling between fluid dynamics and combustion that could be investigated with more controllable conditions than are possible under direct investigations of turbulent flames. The current configuration has been studied experimentally by Chen and Dahm and Chen et al. under microgravity conditions, and by Park and Shin, and You et al. under normal gravity conditions. This configuration is similar to that used in the analyses of Karagozian and Manda of their 2-D vortex pair in which both fuel and entrained oxidizer are present. The vortex ring used in this study is generated by issuing methane into an air environment through the exit of an axisymmetric nozzle. The experiments were conducted under microgravity conditions in order to remove the undesirable effects of buoyancy that can affect both the flame structure and ring dynamics resulting in possibly asymmetric and nonrepeatable interactions. The experimental technique of diode laser wavelength modulation spectroscopy (WMS) is used to measure concentration fields of reactants, CH4 and O2, products, H2O, CO2, OH, and temperature fields which can be inferred from either line pairs of O2 or OH lines. This technique has been investigated previously by Silver and Bomse et al. This is the first time that the technique has been applied to reacting vortex rings under microgravity conditions. The effect of ring circulation and fuel volume on the species concentration fields will be investigated. The experimental results will be compared to the current numerical results, and used to validate the numerical studies. In addition, the existence of burned cores during the interactions will be determined, and the increase in reactant consumption with increased ring circulation will be examined. Numerical studies were also conducted by solving the Navier-Stokes and mixture fraction equations with the assumptions of unity Lewis and Schmidt numbers. Equilibrium chemistry and flamelet libraries were used to obtain the temperature and species mass fraction fields. The numerical results will serve as guidelines in conducting the experimental studies. Ring circulation and fuel volume effects on the interactions and species concentration fields will be investigated and compared to experimental results.

Chen, Shin-Juh↗

Cometabolic Vinyl Chloride Degradation at Acidic pH Catalyzed by Acidophilic Methanotrophs Isolated from Alpine Peat Bogs

Remediation of toxic chlorinated ethenes via microbial reductive dechlorination can lead to ethene formation; however, the process stalls in acidic groundwater, leading to the accumulation of carcinogenic vinyl chloride (VC). This study explored the feasibility of cometabolic VC degradation by moderately acidophilic methanotrophs. Furthermore, two novel isolates, Methylomonas sp. strain JS1 and Methylocystis sp. strain MJC1, were obtained from distinct alpine peat bogs located in South Korea. Both isolates cometabolized VC with CH 4 as the primary substrate under oxic conditions at pH at or below 5.5. VC cometabolism in axenic cultures occurred in the presence (10 μM) or absence (<0.01 μM) of copper, suggesting that VC removal had little dependence on copper availability, which regulates expression and activity of soluble and particulate methane monooxygenases in methanotrophs. The model neutrophilic methanotroph Methylosinus trichosporium strain OB3b also grew and cometabolized VC at pH 5.0 regardless of copper availability. Bioaugmentation of acidic peat soil slurries with methanotroph isolates demonstrated enhanced VC degradation and VC consumption below the maximum concentration level of 2 μg L –1 . Community profiling of the microcosms suggested species-specific differences, indicating that robust bioaugmentation with methanotroph cultures requires further research.

54 ENVIRONMENTAL SCIENCES↗

Can Vertical Profiles of Tropospheric Methane on Titan Be Derived from Radio-Occultation Soundings?

The intensity of the received signal at Earth in the radio occultations of Titan is attenuated both by refractive defocusing and pressure-induced absorption from N2-N2 and CH4-N2 pairs. Because the absorption strength is different for the two sets of pairs, matching the retrieved absorptivity profile can in principle yield the vertical variation in gaseous methane in the troposphere. There are two factors that make this difficult. The first is the propagation of noise in the phase and amplitude of the received signal in the absorption retrieval. The phase data is first inverted to retrieve vertical profiles of refractivity, from which the refractive defocusing is calculated. This is then subtracted from the observed. intensity attenuation of the received signal to generate a profile of atmospheric absorption. The second problem is the uncertainty in the pressure-induced absorption coefficients. Laboratory data at radio wavelengths is only available near room temperature (see, e.g., [1] for N2-N2), and the extrapolation to the low temperatures in Titan's troposphere is not well established. Ab initio calculations by Borysow et al. [2, 3] provide absorption coefficients at low temperatures and long wavelengths, but their accuracy has come into question. We present examples from Cassini radio occultations of Titan to illustrate the difficulties. For methane mole fractions in the lower troposphere comparable to that inferred from the Huygens probe (approximately 0.05), it will be difficult to separate the contributions of N2-N2 collisions from those of N2-CH4, collisions to the retrieved absorption. However, higher concentrations of CH4 and/or a higher signal-to-noise ratio from a future uplink experiment could result in a successful separation of the two components. However, key to this are highly accurate estimates of the absorption from a combination of laboratory measurements at love temperatures and long wavelengths, and possibly improved theoretical calculations.

Flasar, F. Michael↗

Microtopography Matters: Belowground CH 4 Cycling Regulated by Differing Microbial Processes in Peatland Hummocks and Lawns

Water table depth and vegetation are key controls of methane (CH 4 ) emissions from peatlands. Microtopography integrates these factors into features called microforms. Microforms often differ in CH 4 emissions, but microform-dependent patterns of belowground CH 4 cycling remain less clearly resolved. Here, to investigate the impact of microtopography on belowground CH 4 cycling, we characterized depth profiles of the community composition and activity of CH 4 -cycling microbes using 16S rRNA amplicon sequencing, incubations, and measurements of porewater CH 4 concentration and isotopic composition from hummocks and lawns at Sallie's Fen in NH, USA. Geochemical proxies of methanogenesis and methanotrophy indicated that microforms differ in dominant microbial CH 4 cycling processes. Hummocks, where water table depth is lower, had higher porewater redox potential (Eh) and higher porewater δ 13 C-CH 4 values in the upper 30 cm than lawns, where water table depth is closer to the peat surface. Porewater δ 13 C-CH 4 and δD-CH 3 D values were highest at the surface of hummocks where the ratio of methanotrophs to methanogens was also greatest. These results suggest that belowground CH 4 cycling in hummocks is more strongly regulated by methanotrophy, while in lawns methanogenesis is more dominant. We also investigated controls of porewater CH 4 chemistry. The ratio of the relative abundance of methanotrophs to methanogens was the strongest predictor of porewater CH 4 concentration and δ 13 C-CH 4 , while vegetation composition had minimal influence. As microbial community composition was strongly influenced by redox conditions but not vegetation, we conclude that water table depth is a stronger control of belowground CH 4 cycling across microforms than vegetation.

59 BASIC BIOLOGICAL SCIENCES↗

Infrared laboratory studies of synthetic planetary atmospheres

Topics covered include: the broadening of individual lines in the CO fundamental by various gases; total band absorptance as a function of absorber thickness and total effect pressure at various temperatures for bands of CO and N2O; nitric acid vapor content in the region of the ozone layer; optical properties of solid NH3; HSO4 concentration in Venus clouds; Burch's law of multiplicative transmittance for mixing absorbing gases when their lines are broadened by helium and hydrogen; ling strength and self-broadening parameters in the v3 fundamental of CO2 and N2O; optical constants of liquid ammonia, liquid methane, saturated hydrocarbons, ammonium hydride and ammonium salts.

Williams, D.↗

Method and apparatus for vapor detection

The method disclosed herein may be practiced by passing the vapors to be sampled along a path with halogen vapor, preferably chlorine vapor, heating the mixed vapors to halogenate those of the sampled vapors subject to halogenation, removing unreacted halogen vapor, and then sensing the vapors for organic halogenated compounds. The apparatus disclosed herein comprises means for flowing the vapors, both sample and halogen vapors, into a common path, means for heating the mixed vapors to effect the halogenation reaction, means for removing unreacted halogen vapor, and a sensing device for sensing halogenated compounds. By such a method and means, the vapors of low molecular weight hydrocarbons, ketones and alcohols, when present, such as methane, ethane, acetone, ethanol, and the like are converted, at least in part, to halogenated compounds, then the excess halogen removed or trapped, and the resultant vapors of the halogenated compounds sensed or detected. The system is highly sensitive. For example, acetone in a concentration of 30 parts per billion (volume) is readily detected.

Lerner, Melvin↗