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At least 541 records · Page 30

Thermospheric nitric oxide and its role in thermospheric dynamics and composition

The global distribution of thermospheric nitric oxide has been measured under different geophysical conditions by the Atmosphere Explorer (AE) and Solar Mesosphere Explorer (SME) satellites. These observations show a great variability in the NO concentration but the existence of a latitudinal gradient is clearly evidenced by statistical maps of the NO meridional distribution. A two dimensional zonally averaged chemical-dynamical model was used to investigate the importance of nitric oxide 5.3 micrometer cooling and its role on thermospheric temperature, dynamics and major gas composition. For this purpose, a 2-D background atmosphere code and an odd nitrogen code were coupled and run to steady state. The NO distribution obtained is in good agreement with the AE-D global picture calculated at solstice for solar minimum activity. The importance of each term in the thermodynamic equation was studied spatially. It is found that the NO I.R. cooling term competes with conduction in the upper thermosphere and reaches its maximum value near 200 km at high summer latitudes. The primary effect of including the NO cooling term is to increase the temperature in the upper winter thermosphere and decrease it in the other hemisphere, if the global average temperature is fixed. In general, the strength of the circulation is decreased and the thermal gradient is smoother. As a consequence of these changes in the wind and temperature fields, the O2, N2 and O densities also react to the effect of the NO cooling. The importance of this process depends on the level of solar activity which controls the NO distribution.

Gerard, J. C.↗

On the secondary instability of Taylor-Goertler vortices to Tollmien-Schlichting waves in fully-developed flows

There are many flows of practical importance where both Tollmien-Schlichting waves and Taylor-Goertler vortices are possible causes of transition to turbulence. The effect of fully nonlinear Taylor-Goertler vortices on the growth of small amplitude Tollmien-Schlichting waves is investigated. The basic state considered is the fully developed flow between concentric cylinders driven by an azimuthal pressure gradient. It is hoped that an investigation of this problem will shed light on the more complicated external boundary layer problem where again both modes of instability exist in the presence of concave curvature. The type of Tollmein-Schlichting waves considered have the asymptotic structure of lower branch modes of plane Poisseulle flow. Whilst instabilities at lower Reynolds number are possible, the latter modes are simpler to analyze and more relevant to the boundary layer problem. The effect of fully nonlinear Taylor-Goertler vortices on both two-dimensional and three-dimensional waves is determined. It is shown that, whilst the maximum growth as a function of frequency is not greatly affected, there is a large destabilizing effect over a large range of frequencies.

Bennett, James↗

On the secondary instability of Taylor-Goertler vortices to Tollmien-Schlichting waves in fully developed flows

There are many flows of practical importance where both Tollmien-Schlichting waves and Taylor-Goertler vortices are possible causes of transition to turbulence. The effect of fully nonlinear Taylor-Goertler vortices on the growth of small amplitude Tollmien-Schlichting waves is investigated. The basic state considered is the fully developed flow between concentric cylinders driven by an azimuthal pressure gradient. It is hoped that an investigation of this problem will shed light on the more complicated external boundary layer problem where again both modes of instability exist in the presence of concave curvature. The type of Tollmien-Schlichting waves considered have the asymptotic structure of lower branch modes of plane Poiseuille flow. Whilst instabilities at lower Reynolds number are possible, the latter modes are simpler to analyze and more relevant to the boundary layer problem. The effect of fully nonlinear Taylor-Goertler vortices on both two-dimensional and three-dimensional waves is determined. It is shown that, whilst the maximum growth as a function of frequency is not greatly affected, there is a large destabilizing effect over a large range of frequencies.

Bennett, James↗

Visualization of Microbial Biomarkers by Scanning Electron Microscopy

We are developing tools to link the biochemical structure of selected biomarkers with putative biogenic structures observed in mineralized samples. The detection of evidence of life on Mars and other planets will rely on methods that can discriminate compounds formed exclusively by living organisms. While biogenic compounds, such as amino acids and nucleotides have been discovered in extraterrestrial sources, such as meteorites and comets, their formation can be explained by abiotic means. The formation of cellular structures, or more elaborate organic molecules, such as complex lipids, proteins or nucleic acids, however, is strongly correlated to the presence of even the most primitive life processes. Recent evidence lends support to the hypothesis that life may have once existed on Mars. Carbonate globules and ppm concentrations of polycyclic aromatic hydrocarbons (PAHs) have been described in ALH84001, a meteorite originating from Mars ejecta captured by Earth over 13,000 years ago. The localized high concentration of PAHs that follow an increasing gradient from the intact fusion crust towards the interior corresponds to microgram quantities of hydrocarbon. Even though ALH84001 and other similar meteorites have withstood the forces capable of ejecting rock through Mars' escape velocity, upon entering Earth's atmosphere, their core temperatures are likely not to have been raised significantly, as evidenced by the survival of remanent magnetic signatures. Ideal biomarkers of ancient or modern biological life would include molecules that are (or were) pervasive and highly resistant to degradation. Also, requisite methods of detection should be simple, extremely sensitive and broadly inclusive (NASA SP-530). Lipopolysaccharide (LPS), peptidoglycan or pseudopeptidoglycan and beta-glucan are microbial cell wall components which together cover the entire microbial spectrum of eubacteria, archea and fungi. They are all remarkably resistant to thermal degradation. Fortunately, many antimicrobial defense systems of higher organisms require sensitive detection to combat microbial pathogens. We employ here the primitive immune system of the evolutionarily ancient horseshoe crab, Limulus polyphemus. This species relies on multi-enzyme signal amplification detection of cell wall molecules and they can be applied to the development of useful detectors of life. An extension of this work includes the visualization of microbial signatures by labeling LAL components with chromogenic or electron dense markers. The protein Limulus Anti-LPS Factor (LALF) has an extremely high affinity for LPS. By coupling LALF binding with colloidal gold labels we demonstrate a correlation of the structures visible by electron microscopy with biochemical evidence of microbial cell wall materials. Pure silica particles were mixed with cultures of E. coli (10(exp 6) cfu/mL). Samples were washed sequentially with buffered saline, LALF, antibody to LALF and finally colloidal gold-labeled Protein A. Negative controls were not exposed to E. coli but received identical treatment otherwise. Samples were coated with carbon and imaged on a JEOL JSM-840 scanning electron microscope with LaB6 source in the back scatter mode with the JEOL annular back scatter detector. 20 nm-scale black spots in this contrast-reversed image originate from electrons back-scattered by gold atoms. Negative controls did not give any signal. Future work will expand application of this technique to soil simulants and mineralized rock samples.

Wainwright, Norman R.↗

Seasonal Changes in Titan's Meteorology

The Cassini Imaging Science Subsystem has observed Titan for 1/4 Titan year, and we report here the first evidence of seasonal shifts in preferred locations of tropospheric methane clouds. South \polar convective cloud activity, common in late southern summer, has become rare. North \polar and northern mid \latitude clouds appeared during the approach to the northern spring equinox in August 2009. Recent observations have shown extensive cloud systems at low latitudes. In contrast, southern mid \latitude and subtropical clouds have appeared sporadically throughout the mission, exhibiting little seasonality to date. These differences in behavior suggest that Titan s clouds, and thus its general circulation, are influenced by both the rapid temperature response of a low \thermal \inertia surface and the much longer radiative timescale of Titan s cold thick troposphere. North \polar clouds are often seen near lakes and seas, suggesting that local increases in methane concentration and/or lifting generated by surface roughness gradients may promote cloud formation. Citation

Turtle, E. P.↗

Effect of fluctuating redox conditions on trace metal release from wetland soils from South Carolina and stream sediments from Tennessee

Natural aquatic systems undergo fluctuating redox conditions due to microbial activity, varying water saturation levels, and nutrients dynamics. With fluctuating oxic and anoxic conditions, trace metals can be mobilized or sequestered in response to changes in iron and sulfur speciation and the concentrations and lability of organic carbon. We conducted a systematic laboratory-based microcosm study to examine the effect of redox fluctuations on trace metal mobility in samples collected from two different natural aquatic systems: riparian wetlands and a stream. We incubated water-saturated soils under three cycles of anoxic-oxic conditions (τanoxic:τoxic = 3) spanning 24 days and monitored the change in dissolved and bioavailable metal (copper (Cu), nickel (Ni), zinc (Zn), cobalt (Co), iron (Fe), and manganese (Mn)) concentrations. The dataset includes the results of the variation in metal concentrations due to redox fluctuations in wetland soils and stream sediments. Additionally, the variation in the bioavailable concentration of metals obtained using passive samplers based on diffuse gradient in thin-films technique is included in the dataset. We have also reported the change in the pH values and dissolved oxygen concentrations in the microcosms during the entire study of 24 days. The dataset also contains the dissolved organic carbon and sulfate concentrations, and the data on fractions of metals bound to reducible and oxidizable phases. For materials from both the wetlands and the stream, anoxic conditions favored Co and Zn release, which corresponded with the reductive dissolution of iron oxides. In contrast, dissolved Cu concentrations increased under oxic conditions for both sites and correlated positively with the release of sulfate. In wetland soils, dissolution of Fe (hydr)oxides increased Ni solubility; however, in stream sediments, Ni release occurred when sulfides or organic matter were oxidized. For stream sediments, each subsequent redox cycle increased the bioavailability of trace metals. Upon redox fluctuations in wetland soils, the bioavailability of Zn and Cu increased, whereas bioavailable Ni and Co decreased. This study illustrates that different trace metals display distinct bioavailability patterns during oxic-anoxic fluctuations in natural environments. The biogeochemical cycling of carbon and nitrogen in systems with redox fluctuations may be influenced by these patterns in trace metal availability in addition to the availability of electron donors and acceptors.

54 ENVIRONMENTAL SCIENCES↗

Flight Testing of the Forward Osmosis Bag for Water Recovery on STS-135

The Forward Osmosis Bag (FOB) is a personal water purification device for recovery of potable liquid from almost any non-potable water source. The FOB experiment was flown as a sortie mission on STS-135/ULF7 using flight-certified materials and a design based on the X-Pack(TradeMark) from Hydration Technology Innovations (Albany, OR). The primary objective was to validate the technology for use under microgravity conditions. The FOB utilizes a difference in solute concentration across a selectively permeable membrane to draw water molecules from the non-potable water while rejecting most chemical and all microbial contaminants contained within. Six FOB devices were tested on STS-135 for their ability to produce a potable liquid permeate from a feed solution containing 500 mL potassium chloride (15 g/L) amended with 0.1% methyl blue dye (w:v) tracer against an osmotic gradient created by addition of 60 mL of concentrate containing the osmolytes fructose and glucose, and 0.01% sodium fluorescein (w:v) tracer. Three FOB devices were physically mixed by hand for 2 minutes by a crewmember after loading to augment membrane wetting for comparison with three unmixed FOB devices. Hydraulic flux rate and rejection of salt and dye in microgravity were determined from a 60-mL sample collected by the crew on orbit after 6 hours. Post-flight analysis of samples collected on orbit demonstrated that the Forward Osmosis Bag achieved expected design specifications in microgravity. The hydraulic flux rate of water across the membrane was reduced approximately 50% in microgravity relative to ground controls that generated an average of 50 mL per hour using the same water and osmolyte solutions. The membrane rejected both potassium and chloride at >92% and methyl blue dye at >99.9%. Physical mixing of the FOB during water recovery did not have any significant effect on either flux rate or rejection of solutes from the water solution. The absence of buoyancy-driven convection in microgravity suggests that mass transport was dominated by diffusion, slowing the rate of permeate production across the membrane. It is possible that a predicted reduction in concentration polarization at the membrane surface that may have acted to increase the rate of permeate production in microgravity was negligible under the described test conditions.

Roberts, Michael S.↗

Finite difference solution for transient radiative cooling of a conducting semitransparent square region

Transient solutions were obtained for a square region of heat conducting semitransparent material cooling by thermal radiation. The region is in a vacuum environment, so energy is dissipated only by radiation from within the medium leaving through its boundaries. The effect of heat conduction during the transient is to partially equalize the internal temperature distribution. As the optical thickness of the region is increased, the temperature gradients increase near the boundaries and corners, unless heat conduction is large. The solution procedure must provide accurate temperature distributions in these regions to prevent error in the calculated radiation losses. Two-dimensional numerical Gaussian integration is used to obtain the local radiative source term. A finite difference procedure with variable space and time increments is used to solve the transient energy equation. Variable spacing was used to concentrate grid points in regions with large temperature gradients.

Siegel, R.↗

Deuterium in the daytime thermosphere

Ion concentration measurements for H(+) and D(+) from the magnetic ion mass spectrometer on the Atmosphere Explorer C satellite are used, in conjunction with other atmospheric data, to determine the concentrations of H and D in the nonpolar daytime thermosphere. The ratio of the observed D(+) to H(+) concentrations has essentially the same height dependence in the 300 to 800-km region as expected for their neutral counterparts, even in the presence of ion temperature gradients and probable large vertical ion fluxes. Rapid charge exchange with atomic oxygen ensures that D/H is about equal to D(+)/H(+) at the lower altitudes where the derived D to H concentration ratio is a factor of about 6 larger than its sea level value, for an exospheric temperature of 930 K. This relative enhancement of deuterium arises from the fact that hydrogen more readily escapes the earth, and a large vertical gradient in the H concentration relative to its diffusive equilibrium value is necessary to drive this upward flux through the lower thermosphere. If these planetary losses of hydrogen are much greater than those associated with evaporative escape, as is the current view, then correspondingly larger deuterium loss rates are also likely in order that the thermospheric D/H ratio not increase well above the observed value. The absolute winter daytime concentration of deuterium at 300 km is found to be 210 + or - 50 atoms/cu cm.

Breig, E. L.↗

Gradient Architecture Design in Scalable Porous Battery Electrodes

Because it has been demonstrated to be effective toward faster ion diffusion inside the pore space, low-tortuosity porous architecture has become the focus in thick electrode designs, and other possibilities are rarely investigated. Here, to advance current understanding in the structure-affected electrochemistry and to broaden horizons for thick electrode designs, we present a gradient electrode design, where porous channels are vertically aligned with smaller openings on one end and larger openings on the other. With its 3D morphology carefully visualized by Raman mapping, the electrochemical properties between opposite orientations of the gradient electrodes are compared, and faster energy storage kinetics is found in larger openings and more concentrated active material near the separator. As further verified by simulation, this study on gradient electrode design deepens the knowledge of structure-related electrochemistry and brings perspectives in high-energy battery electrode designs.

25 ENERGY STORAGE↗

Air quality impacts from the development of unconventional oil and gas well pads: Air toxics and other volatile organic compounds

Unconventional oil and natural gas development (UOGD) has expanded rapidly across the United States in recent decades and raised concerns about associated air quality impacts. While significant effort has been made to quantify methane emissions, relatively few observations have been made of Volatile Organic Compounds (VOCs), especially during drilling and completion of new wells. Extensive air monitoring during development of several large, multi-well pads in Broomfield, Colorado, in the Denver-Julesburg Basin, provides a novel opportunity to examine changes in local air toxics and other VOC concentrations during well drilling and completions and production. These operations offer an especially useful case to study as several management practices were implemented to reduce emissions (e.g., electrified, grid-powered drill rigs and closed loop fluid handling systems to reduce truck traffic and limit fluid handling on the pad). With simultaneous measurements of methane and 50 VOCs from October 2018 to December 2022 at as many as 19 sites near well pads, in adjacent neighborhoods, and at a more distant reference location, we identify impacts from each phase of well development and production. Use of weekly, time-integrated canisters, a Proton Transfer Reaction Mass Spectrometer (PTR-MS), continuous photoionization detectors (PID) to trigger canister collection upon detection of VOC-rich plumes, and an instrumented vehicle, provided a powerful suite of measurements to characterize both transient plumes and longer-term changes in air quality. Prior to the start of well development, VOC gradients were small across Broomfield. Once drilling commenced, concentrations of oil and gas (O&G) related VOCs, including alkanes and aromatics, increased around active well pads. Concentration increases were clearly apparent during certain operations, including drilling, coil tubing/millout operations, and production tubing installation. Emissions of C 8 –C 10 n-alkanes during drilling operations highlighted the importance of VOC emissions from synthetic drilling mud chosen to reduce odor impacts. More than 90 samples were collected of transient plumes. Using composition measurements, meteorological data, and information about well pad activities, these plumes were connected with specific UOGD operations including drilling, flowback, and production equipment maintenance. The chemical signatures of these plumes differed by operation type (e.g., C 8 –C 10 n-alkanes constituted a larger fraction of measured VOCs in drilling-related plumes). Concentrations of individual, oil and gas-related VOCs in these plumes were often several orders of magnitude higher than in background air, with maximum ethane and benzene concentrations of 79,600 and 819 ppbv, respectively. Because these plumes typically impact a monitoring site for just several minutes, they are easily missed by slower-responding instruments. Study measurements highlight future emission mitigation opportunities during UOGD operations, including better control of emissions from shakers that separate drill cuttings from drilling mud, production separator maintenance operations, and periodic emptying of sand cans during flowback operations.

54 ENVIRONMENTAL SCIENCES↗

Multi-fidelity is the new annealing: Gradient-free learning of posterior densities via transport maps

To tackle concentrated, multi-modal Bayesian inference problems, we propose using an annealed importance sampling procedure. To do this, we form a sequence of annealed distributions and employ transport maps to act as a surrogate of each distribution. This process is demonstrated on a few examples, favorably showing its potential for efficiently parallelizing the process of PDE evaluations and allowing for surrogates that we can sample from exactly.

van Bloemen Waanders, Bart G [Sandia National Labo↗

Performance characterization of metal-supported solid-oxide fuel cell stacks at elevated pressure

Here, in this paper, we present results on performance characterization of solid oxide fuel cell stacks at elevated pressures up to 6 bar a . Stacks are designed and built by Ceres Power, Ltd., and are rated at 1- and 5- kW e . Fuel streams include H 2 / N 2 mixtures, synthetic natural-gas reformate, and simulated anode tail-gas recycle. Elevated operating pressure serves to increase stack electrochemical performance, with the most-pronounced gains found up to 4 bar a . Pressurized operation reduces the extent of methane conversion, promoting more-uniform internal reforming and cooling within the stack. Such cooling is critical at higher-current conditions. A previously developed one dimensional computational stack model is used to provide insight into stack operation. Pressurization is found to slightly increase internal thermal gradients, while promoting more-uniform reactant-concentration profiles across the cell, reducing the likelihood of local fuel starvation. The high fuel dilution brought by anode recycle can modestly decrease stack performance; however, this decrease is recovered through elevated-pressure operation at 3 bar a . Anode recycle further promotes compositional uniformity across the cell. These results reflect that pressurized operation can promote stack performance, while potentially promoting long-term stack durability through uniformity in stack environmental conditions.

25 ENERGY STORAGE↗

An Integrative Model for Soil Biogeochemistry and Methane Processes. II: Warming and Elevated CO 2 Effects on Peatland CH 4 Emissions

Peatlands are one of the largest natural sources for atmospheric methane (CH 4 ), a potent greenhouse gas. Climate warming and elevated atmospheric carbon dioxide (CO 2 ) are two important environmental factors that have been confirmed to stimulate peatland CH 4 emissions; however, the mechanisms underlying enhanced emissions remain elusive. A data-model integration approach was applied to understand the CH 4 processes in a northern temperate peatland under a gradient of warming and doubled atmospheric CO 2 concentration. We found that warming and elevated CO 2 stimulated CH 4 emissions through different mechanisms. Warming initially stimulated but then suppressed vegetative productivity while stimulating soil organic matter (SOM) mineralization and dissolved organic carbon (DOC) fermentation, which led to higher acetate production and enhanced acetoclastic and hydrogenotrophic methanogenesis. Warming also enhanced surface CH 4 emissions, which combined with warming-caused decreases in CH 4 solubility led to slightly lower dissolved CH 4 concentrations through the soil profiles. Elevated CO 2 enhanced ecosystem productivity and SOM mineralization, resulting in higher DOC and acetate concentrations. Higher DOC and acetate concentrations increased acetoclastic and hydrogenotrophic methanogenesis and led to higher dissolved CH 4 concentrations and CH 4 emissions. Both warming and elevated CO 2 had minor impacts on CH 4 oxidation. A meta-analysis of warming and elevated CO 2 impacts on carbon cycling in wetlands agreed well with a majority of the modeled mechanisms. Finally, this mechanistic understanding of the stimulating impacts of warming and elevated CO 2 on peatland CH 4 emissions enhances our predictability on the climate-ecosystem feedback.

54 ENVIRONMENTAL SCIENCES↗

Marine Aerosol to Refinery Emissions: Transport and Evolution of CCN in the Houston Metropolitan Area and Their Impact on Cloud Formation

The Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) campaign aimed to untangle the impacts of contrasting aerosol sources on cloud microphysical properties within deep convective cells using airborne observations with the National Research Council Canada (NRC) Convair CV‐580 research aircraft. Horizontal and vertical gradients of aerosol number size distributions, total aerosol concentrations and cloud condensation nuclei (CCN) spectra were measured in the lower troposphere to quantify the impact of different aerosol sources on aerosol‐cloud interactions. This study focuses on a research flight dedicated to characterizing the aerosol and CCN properties in the Houston Metropolitan region and identifies five main categories of aerosols based on characteristics of aerosol number size distributions, their CCN properties and meteorological conditions. These categories encompassed more than two orders of magnitude differences in aerosol and CCN concentrations, yet their hygroscopic properties remained similar. Aerosol number size distributions and effective hygroscopicity parameters are used to generate continuous CCN spectra to represent the major aerosol types. The different CCN spectra are then incorporated into a 1‐D aerosol‐cloud parcel model using a large range of updrafts selected in the range of those observed during the ESCAPE campaign to assess the impact of the major aerosol sources in Houston on deep convective cloud microphysical properties.

aerosol-cloud interactions↗

Epitaxial gallium arsenide wafers

The preparation of GaAs epitaxial layers by a vapor transport process using AsCl3, Ga and H2 was pursued to provide epitaxial wafers suitable for the fabrication of transferred electron oscillators and amplifiers operating in the subcritical region. Both n-n(+) structures, and n(++)-n-n(+) sandwich structures were grown using n(+) (Si-doped) GaAs substrates. Process variables such as the input AsCl3 concentration, gallium temperature, and substrate temperature and temperature gradient and their effects on properties are presented and discussed.

Black, J. F.↗

Turbulent shear flow of continuum plasma.

The turbulence structure of weakly ionized, continuum plasma is analyzed with emphasis on the turbulent fluctuation and the transport properties of the ionized species. The mean gradients of the velocity and ionized-species concentrations are considered to be uniform. It is assumed that the turbulence Reynolds number is small and that the turbulence field is homogeneous in order to close the dynamic equations of turbulence. It was found that the ratio of the Debye shielding length to the local integral scale of turbulence must be sufficiently small in order for the detailed quasi-neutrality to prevail. The condition of the detailed quasi-neutrality is necessary, in addition to the equal mean concentrations of electrons and ions, in order for the turbulence properties involving the electrons to be the same as those involving the ions.

Chung, P. M.↗

Vapor growth of GeTe single crystals in micro-gravity

The positive effects of micro-gravity on crystal growth and fundamental properties of the vapor transport reaction were established by analyzing the results of GeSe and GeTe vapor transport experiments performed on board Skylab. The analysis was based on a direct comparison of GeSe and GeTe crystals and of mass transport rate data obtained on earth and in space. For this purpose, a total of six transport experiments employing different concentrations of transport agent (GeI4) and two temperature gradients were performed during the Skylab 3 and 4 missions. Extensive ground-based studies demonstrated that the crystal morphology and the mass transport rates of the above systems are affected by the transport conditions, in particular by gravity-driven convection. The results demonstrate unambiguously a considerable improvement of the space crystals in terms of surface perfection, crystalline homogeneity and defect density. The observation of greater mass transport rates than expected in micro-gravity environment is of basic scientific and technological significance. This indicates that conventional transport models are incomplete and demonstrates that crystals of improved quality can be grown at reasonable rates by this technique in space. Results are of practical importance for the modification of crystal growth techniques on earth.

Wiedemeier, H.↗