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DOE OSTI2020

Fundamental Studies of Oxidation Reactions on Model Catalysts. Final report

This report covers the reporting period from 08/15/2003 to 08/31/2019. The research activities were focused on the oxidation of methane, nitric oxide, and propylene in addition to contributions on the kinetics, synthesis, theory and characterization of various catalytic systems. As described in the report, we were able to formulate hypotheses, construct specialized equipment and carry out experimental and theoretical work to test the hypotheses. Major advances were accomplished in the fundamental understanding of these systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Pulse Detonation Engine for Advanced Oxy-Combustion of Coal-Based Fuel for Direct Power Extraction Applications

Pressure gain combustion and magnetohydrodynamic (MHD) systems have the potential to provide a step increase in the efficiency of combined-cycle power plants. Specific advantages include a net pressure increase to the system instead of a pressure drop, the high temperature of the detonation waves can increase the efficiency of power extraction compared to other processes, significant thermal energy can be released in a compact region, and the high velocities of the flow increase extraction of electrical power. In summary, a pressure gain combustor coupled with a MHD has the potential to be transformative. Despite the potential advantages, relatively little research has been conducted considering coupled pressure gain combustion systems with MHD systems. With this background and motivation, the overall goal of this effort was to advance the knowledge, technology, and computational tools associated with coupled detonation and MHD systems. A joint experimental and computational approach was used while seeking to accomplish the goals of this work. Specifically, two pulse detonation engines were developed and used for the experiments to produce detonations. Detonation speeds were measured for a variety of flow and fuel conditions (e.g., methane, propane, with coal particles). Preliminary electrical conductivity measurements were collected. An extensive amount of research was performed to identify sensitivities of detonation behaviors to the presence of combustion products. Computationally, a twofold approach was used in this work. First, a solver was developed for solving the governing equations for a reactive flow with coupled detonation and ionization chemistry. The solver was applied to study the impacts of seed material ionization on detonation. Second, a conservation element-solution element (CE-SE) based numerical solver for detonation studies with a reduced reaction mechanism for oxy-methane combustion was developed and verified on standard test cases. Key findings and contributions from this work are as follows. A system was developed for injecting powderized coal, or other seeding material, into a pulse-detonation system. The influence of a combustion product (i.e., CO 2 ) on detonation behavior was identified. Knowledge gained from this work is applicable to devices such as rotating detonation engines, where combustion products mix with fresh reactants. A system for measuring the electrical conductivity of the exhaust from a pulse-detonation engine was developed. The open-source solver, Clawpack, was extended to solve the reactive Euler equations for simulating detonations. A coupled combustion and ionization chemistry was developed in a single chemical kinetic model for methane oxidation. This model can be used to solve coupled MHD and detonation simulations. It was found that parasitic interactions from ionization chemistry with the magnetic field can reduce the detonation velocity by up to 8%, with a potential impact on power extraction of 15%. It is recommended that interactions between the detonation front and MHD field be considered. Higher gas temperatures and velocities were achieved owing to oxy-fuel detonations. Use of radical dissociation reactions in the reduced reaction mechanism, was found to be critical in predicting detonation temperature and velocity accurately.

01 COAL, LIGNITE, AND PEAT↗

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↗

DOE OSTI2020

Metagenomic Insight into Environmentally Challenged Methane-Fed Microbial Communities

In this study, we aimed to investigate, through high-resolution metagenomics and metatranscriptomics, the composition and the trajectories of microbial communities originating from a natural sample, fed exclusively with methane, over 14 weeks of laboratory incubation. This study builds on our prior data, suggesting that multiple functional guilds feed on methane, likely through guild-to-guild carbon transfer, and potentially through intraguild and intraspecies interactions. We observed that, under two simulated dioxygen partial pressures—low versus high—community trajectories were different, with considerable variability among the replicates. In all microcosms, four major functional guilds were prominently present, representing Methylococcaceae (the true methanotrophs), Methylophilaceae (the nonmethanotrophic methylotrophs), Burkholderiales, and Bacteroidetes. Additional functional guilds were detected in multiple samples, such as members of Opitutae, as well as the predatory species, suggesting additional complexity for methane-oxidizing communities. Metatranscriptomic analysis suggested simultaneous expression of the two alternative types of methanol dehydrogenases in both Methylococcaceae and Methylophilaceae, while high expression of the oxidative/nitrosative stress response genes suggested competition for dioxygen among the community members. The transcriptomic analysis further suggested that Burkholderiales likely feed on acetate that is produced by Methylococcaceae under hypoxic conditions, while Bacteroidetes likely feed on biopolymers produced by both Methylococcaceae and Methylophilaceae.

59 BASIC BIOLOGICAL SCIENCES↗

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.↗

NASA NTRS2000

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

Lin, K.-C.↗

NASA NTRS1994

Identification of Methanotrophic Biomarker Lipids in the Symbiont-Containing Gills of Seep Mussels

Mussels collected from hydrocarbon seeps in the Gulf of Mexico grow with methane as sole carbon and energy source due to a symbiotic association with methane-oxidizing bacteria. Transmission electron micrographs of mussel gills show cells with stacked intracytoplasmic membranes similar to type I methanotrophic bacteria. Methanotrophs are known to synthesize several types of cyclic triterpenes, hopanoids and methyl sterols, as well as unique monounsaturated fatty acid, double bond positional isomers that serve as biomarkers for this group. Lipid analysis of dissected mussels demonstrated the presence of these biomarkers predominantly in the gill tissue with much smaller amounts in mantle and remaining body tissues. Gill tissue contained 1150 micrograms/g dry wt. of hopanepolyol derivatives and diplopterol while the mantle tissue contained only 17 micrograms/g. The C16 monounsaturated fatty acids (16:1) characteristic of type I methanotrophic membranes dominated the gill tissue making up 53% of the total while only 5% 16:1 was present in the mantle tissue. The methyl sterol distribution was more dispersed. The predominant sterol in all tissues was cholesterol with lesser amounts of other desmethyl and 4-methyl sterols. The gill and mantle tissues contained 3461 micrograms (17% methyl) and 2750 micrograms (5% methyl) sterol per gm dry wt., respectively. Methyl sterol accounted for 44% of the sterol esters isolated from the gill, suggesting active demethylation of the methanotrophic sterols in this tissue. The use of lipid biomarkers could provide an effective means for identifying host-symbiont relationships.

Jahnke, L. L.↗