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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Chamber Flux and Porewater Concentration of CH4, CO2 and N2O, 2018, Columbia River bank at the Hanford site, WA, USA

This is the corresponding observations data for the paper: Jorge A Villa; Garrett J Smith; Yang Ju; Lupita Renteria; Jordan C Angle; Evan Arntzen; Samuel F Harding; Huiying Ren; Xingyuan Chen; Audrey H Sawyer; Emily B Graham; James C Stegen; Kelly C Wrighton; Gil Bohrer (2020) Methane and nitrous oxide porewater concentrations and surface fluxes of a regulated river. Science of the Total Environment.Greenhouse gas (GHG) emissions from rivers are a critical missing component of current global GHG models. Their exclusion is mainly due to a lack of in-situ measurements and a poor understanding of the spatiotemporal dynamics of GHG production and emissions, which prevents optimal model parametrization. We combined simultaneous observations of porewater concentrations along different beach positions and depths, and surface fluxes of methane and nitrous oxide at a plot scale in a large regulated river during three water stages: rising, falling, and low. Our goal was to gain insights into the interactions between hydrological exchanges and GHG emissions and elucidate possible hypotheses that could guide future research on the mechanisms of GHG production, consumption, and transport in the hyporheic zone (HZ). Results indicate that the site functioned as a net source of methane. Surface fluxes of methane during river water stages at three beach positions (shallow, intermediate and deep) correlated with porewater concentrations of methane. However, fluxes were significantly higher in the intermediate position during the low water stage, suggesting that low residence time increased methane emissions. Vertical profiles of methane peaked at different depths, indicating an influence of the magnitude and direction of the hyporheic mixing during the different river water stages on methane production and consumption. The site acted as either a sink or a source of nitrous oxide depending on the elevation of the water column. Nitrous oxide porewater concentrations peaked at the upper layers of the sediment throughout the different water stages. River hydrological stages significantly influenced porewater concentrations and fluxes of GHG, probably by influencing heterotrophic respiration (production and consumption processes) and transport to and from the HZ. Our results highlight the importance of including dynamic hydrological exchanges when studying and modeling GHG production and consumption in the HZ of large rivers.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Genomic and environmental controls on Castellaniella biogeography in an anthropogenically disturbed subsurface

Castellaniella species have been isolated from a variety of mixed-waste environments including the nitrate and multiple metal-contaminated subsurface at the Oak Ridge Reservation (ORR). Previous studies examining microbial community composition and nitrate removal at ORR during biostimulation efforts reported increased abundances of members of the Castellaniella genus concurrent with increased denitrification rates. Thus, we asked how genomic and abiotic factors control the Castellaniella biogeography at the site to understand how these factors may influence nitrate transformation in an anthropogenically impacted setting. We report the isolation and characterization of several Castellaniella strains from the ORR subsurface. Five of these isolates match at 100% identity (at the 16S rRNA gene V4 region) to two Castellaniella amplicon sequence variants (ASVs), ASV1 and ASV2, that have persisted in the ORR subsurface for at least 2 decades. However, ASV2 has consistently higher relative abundance in samples taken from the site and was also the dominant blooming denitrifier population during a prior biostimulation effort. We found that the ASV2 representative strain has greater resistance to mixed metal stress than the ASV1 representative strains. We attribute this resistance, in part, to the large number of unique heavy metal resistance genes identified on a genomic island in the ASV2 representative genome. Additionally, we suggest that the relatively lower fitness of ASV1 may be connected to the loss of the nitrous oxide reductase (nos) operon (and associated nitrous oxide reductase activity) due to the insertion at this genomic locus of a mobile genetic element carrying copper resistance genes. This study demonstrates the value of integrating genomic, environmental, and phenotypic data to characterize the biogeography of key microorganisms in contaminated sites.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1973

Reactions of O/1D/ with methane and ethane.

Mixtures of nitrous oxide and methane and mixtures of nitrous oxide and ethane were photolyzed with 1849-A light. The reaction products were analyzed chromatographically. It was found that the reaction of the excited atomic oxygen with methane gives mainly CH3 and OH radicals as initial products, along with about 9% of formaldehyde and molecular hydrogen. The reaction of the excited atomic oxygen with ethane gives C2H5, OH, CH3 and CH2OH as major initial products, with only a few per cent of molecular hydrogen.

Lin, C.-L.↗
NASA NTRS2014

Airborne Tropical TRopopause EXperiment (ATTREX) 2014 Western Pacific Campaign

The NASA Airborne Tropical TRopopause EXperiment (ATTREX) is a series of airborne campaigns focused on understanding physical processes in the Tropical Tropopause Layer (TTL) and their role in atmospheric chemistry and climate. ATTREX is using the high-altitude, long-duration NASA Global Hawk Unmanned Air System to make in situ and remote-sensing measurements spanning the Pacific. A particular ATTREX emphasis is to better understand the dehydration of air as it passes through the cold tropical tropopause region. The ATTREX payload contains 12 in situ and remote sensing instruments that measure water vapor, carbon dioxide, methane, nonmethane hydrocarbons, sulfur hexafluoride, chlorofluorocarbons, nitrous oxide), reactive chemical compounds (ozone, bromine, nitrous oxide), meteorological parameters, and radiative fluxes. During January-March, 2014, the Global Hawk was deployed to Guam for ATTREX flights. Six science flights were conducted from Guam (in addition to the transits across the Pacific), resulting in over 100 hours of Western Pacific TTL sampling and about 180 vertical profiles through the TTL. I will provide an overview of the dataset, with examples of the measurements including meteorological parameters, clouds and water vapor, and chemical tracers.

Airborne↗
NASA NTRS1991

Biospheric-atmospheric coupling on the early Earth

Theoretical calculations performed with a one-dimensional photochemical model have been performed to assess the biospheric-atmospheric transfer of gases. Ozone reached levels to shield the Earth from biologically lethal solar ultraviolet radiation (220-300 nm) when atmospheric oxygen reached about 1/10 of its present atmospheric level. In the present atmosphere, about 90 percent of atmospheric nitrous oxide is destroyed via solar photolysis in the stratosphere with about 10 percent destroyed via reaction with excited oxygen atoms. The reaction between nitrous oxide and excited oxygen atoms leads to the production of nitric oxide in the stratosphere, which is responsible for about 70 percent of the global destruction of oxygen in the stratosphere. In the oxygen/ozone deficient atmosphere, solar photolysis destroyed about 100 percent of the atmospheric nitrous oxide, relegating the production of nitric oxide via reaction with excited oxygen to zero. Our laboratory and field measurements indicate that atmospheric oxygen promotes the biogenic production of N2O and NO via denitrification and the biogenic production of methane by methanogenesis.

Levine, J. S.↗
NASA NTRS2012

Development and Testing of a Green-Propellant Micro-Hybrid Thruster with Electrostatic Ignition

As early as 1937 German scientists at Peenemunde experimented with highly unstable fuel blends of nitrous oxide (N2O) and ethanol. These early tests mostly resulted in explosions and destroyed rocket engines. More recently several companies have developed experimental nitrous oxide fuel blends (NOFB) with Isp exceeding 300 sec. Although NOFBx has recently been cleared for tests on the International Space Station, this propellant remains highly experimental and has not been cleared for commercial transport by the US DOT. Recent work by Karabeyoglu et al. has raised concerns about the safety risks of mixing hydrocarbons with N2O. Liquid oxidizer/fuel blends are highly explosive and require extreme care in transport and servicing. By adding small amounts of a liquid organic fuel such as alcohol or a hydrocarbon, the odds of an explosive decomposition event are significantly increased.iv The proposed solution mitigates the explosion hazards of NOFB by separating the oxidizer from the hydrocarbon fuel formed as of a small cylindrical section of ABS thermoplastic. As N2O vapor flows across the grain segment, current enters a 1000 VDC high-tension lead in the ABS fuel grain and produces an inductive spark that vaporizes a small amount of the material. The ablated fuel vapor plus residual energy from the spark seed a localized exothermic N2O dissociation that produces sufficient heat to initiate combustion. The process is also effective when gaseous oxygen is used. A low TRL (2-3) prototype demonstrating the feasibility of controlled hydrocarbon-seeding was recently tested at Utah State University.v The unit features a miniature 2.5 cm ABS fuel grain fabricated using a Stratasys Dimension 3-D printer. The 9-N thruster was pulse-fired up to 27 consecutive times on a single ABS grain segment. Ignition was achieved by as little as 12-15 Joules energy input. This value is contrasted with the typical 30-minute pre-heat requirement for the ECAPS LMP-103S ADN-based monopropellant, requiring an energy input of 14,850 Joules for catalytic dissociation. The hydrocarbon-seeded micro-hybrid was also adapted as a non-pyrotechnic ignitor for a 900 N (200-lbf) thrust hybrid motor. The motor was successfully ignited 4 consecutive times with no hardware swaps or propellant additions. The amount of ABS seed material that can be fit into the injector cap is the only limit to the number of available repeat firings. This series of tests marks the first time a hybrid motor was ever ignited by other than a solid-propellant pyrotechnic charge or bi-propellant flame ignitor. Nitrous oxide hybrid motors are typically difficult to ignite and usually require multiple solid-propellant charges to initiate combustion, so this nonpyrotechnic ignition is a significant accomplishment. The controlled hydrocarbon-seeding approach is fundamentally different from all other green propellant solutions offered by the aerospace industry. Although the proposed system is more correctly a hybrid technology; the system retains all the simple features of a monopropellant design. To date no optimization study has been performed to identify the best grain geometry for electrostatic ignition. Fortunately, because the grain segments are fabricated using rapid-prototyping technology, changing the grain geometry is as simple as modifying the 3-D printer CAD-file. Vacuum Isp exceeding 270 seconds has been demonstrated (Ref v), a value significantly higher than those offered by competing green monopropellant options. The propellants of choice, N2O/GOX and ABS are 100% non-toxic, non-explosive, and environmentally benign. Because the inert oxidizer and fuel components are mixed only within the combustion chamber, the system retains the inherent safety of a hybrid rocket and can be piggy-backed as a secondary payload with no overall mission risk increase to the primary payload, an excellent characteristic for secondary launch systems.

Whitmore, Stephen A.↗
NASA NTRS1978

Decomposition of N2O over particulate matter

Nitrous oxide is shown to undergo both a thermal and a photochemical decomposition at 296 K when it is adsorbed on various dry sands. The photochemical process occurs with light of wavelengths greater than 280 nm, where gaseous N2O does not absorb. At low pressures (less than 0.1 torr) the half-life for the thermal decomposition of nitrous oxide to nitrogen when placed in contact with about 5 gm of heat-treated Tunisian sand in a one-liter vessel was 350 + or - 35 days. Under certain photolytic conditions this half-life was reduced. The efficiency of the photolytic process for a particular sand depends on the pressure and on the wavelength of light. For Tunisian sand at 1.1 torr and with the full mercury arc, the destruction efficiency is about 0.00002 molecule/incident photon. These results indicate that particulate matter in the troposphere may be responsible for the decomposition of nitrous oxide and hence act as an atmospheric sink for N2O. However, moisture causes a drastic reduction in the number of molecules dissociated per incident photon.

Rebbert, R. E.↗
NASA NTRS1976

Study of removal of ammonia from urine vapor by dual catalyst

The feasibility of ammonia removal from urine vapor by a low temperature dual-catalyst system was investigated. The process is based on the initial catalytic oxidation of ammonia present in urine vapor to nitrogen and nitrous oxide, followed by a catalytic decomposition of the nitrous oxide formed into its elements. The most active catalysts for the oxidation of ammonia and for the decomposition of N2O, identified in screening tests, were then combined into dual catalyst systems and tested to establish their overall efficiencies for the removal of ammonia from artificial gas mixtures. Dual catalyst systems capable of ammonia removal from the artificial gas mixtures were then tested with the actual urine vapor produced by boiling untreated urine. A suitable dual catalyst bed arrangement was found that achieved the removal of ammonia and organic carbon, and recovered water of good quality from urine vapor.

Budininkas, P.↗
NASA NTRS1991

Energy, atmospheric chemistry, and global climate

Global atmospheric changes due to ozone destruction and the greenhouse effect are discussed. The work of the Intergovernmental Panel on Climate Change is reviewed, including its judgements regarding global warming and its recommendations for improving predictive capability. The chemistry of ozone destruction and the global atmospheric budget of nitrous oxide are reviewed, and the global sources of nitrous oxide are described.

Levine, Joel S.↗
NASA NTRS1993

Design of a high density cold gas attitude control system

A comparison of the experimental results of a nitrous oxide cold gas thruster with the predicted performance from a numerical simulation of nozzle operations is discussed. Tests were conducted in a vacuum chamber to verify analytical predictions of both nitrogen and nitrous oxide. Preliminary results indicate an Isp for N2O of 61, and an Isp of 69 for N2. Based on the results of this research, parameters are presented for a nitrous oxide-based reaction control system for a small spacecraft currently under development.

Hall, Sarah E.↗
NASA NTRS1984

The effect of oxygen on denitrification during steady-state growth of Paracoccus halodenitrificans

Steady-state cultures of Paracoccus halodenitrificans were grown anaerobically prior to establishing steady states at different concentrations of oxygen. In the absence of oxygen, nitrate-limited cultures produced dinitrogen, and as the oxygen supply increased, these cultures produced nitrous oxide, then nitrite. These changes reflected two phenomena: the inactivation of nitrous oxide reductase by oxygen and the diversion of electrons from nitrite to oxygen.

Hochstein, L. I.↗
DOE OSTI2021

Rock Fracturing Using High-Pressure Ethylene/Nitrous Oxide Detonations

The present work investigates high initial pressure detonations of a stoichiometric mixture of ethylene and nitrous oxide (C2H4 + 6N2O) as a method of fracturing rock beneath the ground surface. These tests were conducted at a test site operated by the Energetic Materials Research and Testing Center (EMRTC), Socorro, New Mexico. The volume under the surface used for testing (called the Down Hole Assembly) consists of a 0.438 in. ID x 50 ft. long stainless-steel tube running down from the test site to a well bore which is 3 in. ID x 10 ft. long and the rock in the well bore is exposed to the propagating combustion wave. The testing carried out at Zucrow Laboratories in the smaller, alloy steel combustion vessel provided a scaling of pressures expected in the well bore. The combustion is initiated by energizing an EBW (Exploding Bridge Wire) above the ground surface. The experimental setup accommodates one high pressure (100,000 psia) transducer to measure the pressure peak and is placed approximately 5 ft. above the ground surface and 5 ft. downstream of the EBW. The focus of this series of experiments is to investigate the dependence of fracture to the rock beneath the surface on initial pressures of the mixture of ethylene and nitrous oxide. Experiments were carried out at initial pressures varying between 125 psia and 300 psi. The transducer recorded elevated pressures, which were 2.3 to 2.6 times in excess of the CJ values. The experimental results are discussed and explained in this report.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

What Is the Right Level of Activation of a High-Spin {FeNO} 7 Complex to Enable Direct N–N Coupling? Mechanistic Insight into Flavodiiron NO Reductases

Flavodiiron nitric oxide reductases (FNORs), found in pathogenic bacteria, are capable of reducing nitric oxide (NO) to nitrous oxide (N 2 O) to detoxify NO released by the human immune system. Previously, we reported the first FNOR model system that mediates direct NO reduction (Dong, H. T.; et al. J. Am. Chem. Soc. 2018, 140, 13429-13440), but no intermediate of the reaction could be characterized. Here, we present a new set of model complexes that, depending on the ligand substitution, can either mediate direct NO reduction or stabilize a highly activated high-spin (hs) {FeNO} 7 complex, the first intermediate of the reaction. The precursors, [{Fe II (MPA-(RPhO) 2 )} 2 ] (1, R = H and 2, R = t Bu, Me), were prepared first and fully characterized. Complex 1 (without steric protection) directly reduces NO to N 2 O almost quantitatively, which constitutes only the second example of this reaction in model systems. Contrarily, the reaction of sterically protected 2 with NO forms the stable mononitrosyl complex 3, which shows one of the lowest N-O stretching frequencies (1689 cm -1 ) observed so far for a mononuclear hs-{FeNO} 7 complex. Here this study confirms that an N-O stretch & LE;1700 cm -1 represents the appropriate level of activation of the FeNO unit to enable direct NO reduction. The higher activation level of these hs-{FeNO} 7 complexes required for NO reduction compared to those formed in FNORs emphasizes the importance of hydrogen bonding residues in the active sites of FNORs to activate the bound NO ligands for direct N-N coupling and N2O formation. The implications of these results for FNORs are further discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1974

Absorption cross sections of stratospheric molecules

Two classes of molecular species must be considered in a calculation of photochemical rates in the stratosphere. The first class consists of molecular oxygen and ozone, while the second class contains the remainder of the minor constituents. If accurate values of the transmitted fluxes are required at large optical depths, the cross sections for molecular oxygen and ozone must be known to within a few per cent at least. On the other hand, the photochemical rates for the minor species are given simply by the relevant cross sections. A review of published cross sections is presented, giving attention to molecular oxygen, ozone, nitric oxide, nitrogen dioxide, nitrous oxide, nitric acid, ammonia, water vapor, hydrogen peroxide, carbon monoxide, carbon dioxide, and sulfur dioxide.

Hudson, R. D.↗
NASA NTRS2022

Mineral-Catalysed Formation of Marine NO and N 2 O on the Anoxic Early Earth

Microbial denitrification converts fixed nitrogen species into gases in extant oceans. However, it is unclear how such transformations occurred within the early nitrogen cycle of the Archean. Here 5we present experimental anoxic surface-catalyzed reduction of nitrite and nitrate via green rust and magnetite combined with diffusion and photochemical modeling. We find that in a Fe 2+ -rich marine environment, Fe minerals could have catalyzed abiotic denitrification reactions leading to the formation of nitric oxide (NO) and nitrous oxide (N 2 O). Nitrate did not exhibit reactivity in the presence of either mineral or aqueous Fe2+, however, both minerals induced rapid nitrite reduction 10to NO and N 2 O. While N 2 O escaped into the atmosphere (63% of nitrite-nitrogen, with green rust as catalyst), NO remained associated with precipitates (7%) serving as a potential shuttle to the benthic ocean.The modeling suggests that marine N 2 O emissions would have sustained 0.8-6 ppb of atmospheric N 2 O without a protective ozone layer. Our findings add detail to the as yet incompletely documented Archean nitrogen cycle, implying a globally distributed process driven 15by chemical kinetics similar to those of modern enzymatically mediated conversions.

Steffen Buessecker↗
DOE OSTI2022

Integrated Modeling of U.S. Agricultural Soil Emissions of Reactive Nitrogen and Associated Impacts on Air Pollution, Health, and Climate

Agricultural soils are leading sources of reactive nitrogen (Nr) species including nitrogen oxides (NO x ), ammonia (NH 3 ), and nitrous oxide (N 2 O). Here, the propensity of NO x and NH 3 to generate ozone and fine particulate matter (PM) and associated impacts on health are highly variable, whereas the climate impacts of long-lived N 2 O are independent of emission timing and location. However, these impacts have rarely been compared on a spatially-resolved, monetized basis. In this study, we update the nitrogen scheme in an agroecosystem model to simulate the agricultural emissions of Nr from across the United States. We then apply a reduced-form air pollution health effects model to assess air quality impacts from NO x and NH 3 and a social cost of N 2 O to assess the climate impacts. Assuming an $\$$8.2 million Value of a Statistical Life (VSL) and a $\$$13,100/ton social cost of N 2 O, the air quality impacts are a factor of ~7 to 15 times as large as the climate impacts in heavily populated coastal regions, whereas the ratios are closer to 2.5 in sparsely populated regions. Our results show that air pollution, health, and climate should be considered jointly in future assessments of how farming practices affect Nr emissions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Microbial Competition for Copper: Impacts on Carbon and Nitrogen Cycling

Activities from this DOE sponsored project focused on two general questions: (1) how does competition between microbes for copper affect emissions of greenhouse gasses, especially methane and nitrous oxide? and (2) how does a novel copper-binding compound (methanobactin) made by some methane-oxidizing bacteria bind and reduce metals, as well as what are the regulatory elements involved in controlling methanobactin synthesis? From these efforts, we have conclusively shown that microbial competition for copper does indeed exert significant control on microbial community composition, as well as affects how microbes produce and consume nitrous oxide. We have also developed much better insights into the basis for methanobactin activity, as well as how methanotrophs control its production.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Gas-phase ion-molecule interactions in a collision reaction cell with triple quadrupole-inductively coupled plasma mass spectrometry: Investigations with N 2 O as the reaction gas

Nitrous oxide (N 2 O) was used as a reaction gas to investigate the gas phase ion-molecule interactions using the Agilent 8900 QQQ-ICP-MS. A multi-element standard containing 45 elements with masses ranging from 9 to 208 u was measured in the presence and absence of N 2 O. The main product ion species observed were oxides and nitrides. Comparison of the N 2 O reaction results with similar measurements conducted with O 2 revealed that N 2 O was more effective at forming oxides in general: the elements Cd and Pb were shown to produce oxides with N 2 O where the reaction did not occur with O 2 . Nitrous oxide was also shown to produce a significant amount of nitride species in a few cases. The general reactivity was shown to be consistent with density functional theory (DFT)-predicted reaction enthalpies, such that all predicted exothermic reactions produced product ions at levels at least 1% of the unreacted ion. Our results show that reaction enthalpy is a reasonable predictor of reactivity with N2O on the timescales of the interactions in non-thermal ICP-MS/MS systems. Our work demonstrates the utility of two relatively new platforms (commercial elemental ICP-MS/MS and EMSL Arrows interface to the NWChem program suite), which allows for the study of a large number of elements within a short period. While DFT with the basis sets utilized here is not the most accurate computational method, it is also not computationally expensive and is shown to be suitable for predicting gas phase reactivity in the QQQ-ICP-MS for the majority of ions studied. Here, the ease and rapidity of data collection and DFT calculations has the potential to be very impactful for the identification of targeted reaction chemistries to be leveraged for analytical method development, such as for the inline separation of isobaric interferences from analytes of interest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗