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NASA NTRS1994

Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

Gorzelska, K.↗
NASA NTRS1994

Ammonia on the prebiotic Earth: Iron(II) reduction of nitrite

Theories for the origin of life require the availability of reduced nitrogen. In the non-reducing atmosphere suggested by geochemical evidence, production in the atmosphere and survival of NH3 against photochemical destruction are problematic. Electric discharges and impact shocks would produce NO rather than HCN or NH3. Conversion of NO to nitrous and nitric acid (by way of HNO) and precipitation in acid rain would provide a source of fixed nitrogen to the early ocean. One solution to the NH3 problem may have been the reduction of nitrite/nitrate in the ocean with aqueous ferrous iron, Fe(2+): 6Fe(+2) + 7 H2O + NO2(-) yields 3Fe2O3 + 11 H(+) + NH3. We have measured the kinetics of this reaction as a function of temperature, pH, and concentrations of salts, Fe(+2), and NO2(-). Cations (Na(+), Mg(2+), K(+)) and anions (Cl(-), Br(-), SO4(2-)) increase the rate by factors of 4 to 8. Although a competing pathway yields N2, the efficiency of the conversion of nitrite to ammonia ranges from 25% to 85%. Nitrate reduction was not consistently reproducible; however, when it was observed, its rate was slower by at least 8X than that of nitrite reduction. If the prebiotic atmosphere contained 0.2 to 10 atmospheres CO2 as suggested by Walker (1985), the Fe(+2) concentration and the rate would have been limited by siderite (FeCO3) solubility.

Summers, David P.↗
NASA NTRS1994

Problems with Re-Os isochron determinations

We have developed closed-system techniques for the equilibration of Os isotopes and for the calibration of Re and Os tracers using high-purity metals. The results show reproducibility of +/- 0.5% for calibrations of Os using different chunks of the same high-purity Os metal produced by vacuum arc melting. On a Re-Os evolution diagram the analyses of Negrillos and of Tocopilla are displaced along horizontal lines and are not consistent with a well-defined isochron. We conclude that is unclear whether whole-rock samples of irons of individual classes of iron meteorites (including the IIA class) define isochrons.In light of these observations, one must consider the evidence for phases in which Re and Os may become redistributed. We note that the IIA irons are composed of large or single kamacite crystals and do not contain taenite. This may hinder redistribution of Re and Os and may allow the IIA irons to define isochrons in preference to other magmatic iron classes. However, the IIA irons also include ubiquitous rhabdites, up to 20 mm in length, and troilite-daubreelite nodules. It has been observed that rhabdites are extremely rich in Pt-group elements. In addition to these considerations, Negrillos and Tocopilla were found in nitrate deposits and show evidence of corrosion. Therefore, it is possible that different samples of these meteorites have been differentially weathered, although our samples appeared fresh. We conclude that it is important to identify the phases in which Re and the PGEs are located and to address in detail the evidence for Re and Os remobilization.

Papanastassiou, D. A.↗
NASA NTRS1993

The evolution of ClO and NO along air parcel trajectories

Back trajectory analysis of Arctic and Antarctic aircraft data reveals that high ClO concentrations are associated with predicted polar stratospheric cloud (PSCs) encounters. The ClO concentrations within the Arctic and Antarctic polar vortices vary widely but appear to be inversely related to parcel solar exposure since the last PSC interaction. These results imply that production of NO(x) from HNO3 photolysis and reaction with OH is the mechanism for the loss of chlorine radicals through the reformation of chlorine nitrate. Highly denitrified air parcels show no change in ClO with solar exposure. The recovery process is quantitatively duplicated using a model of chemistry along trajectories. Although PSC processing is the primary mechanism for producing elevated ClO amounts, back trajectories apparently unperturbed by PSC's also show slightly elevated ClO levels in 1992 compared to Arctic 1989 and Antarctic 1987 measurements presumably due to the presence of Pinatubo aerosol.

Schoeberl, M. R.↗
NASA NTRS1994

Origin of tropospheric NO(x) over subarctic eastern Canada in summer

The original of NO(X) in the summertime troposphere over subarctic eastern Canada is investigated by photochemical modeling of aircraft and ground-based measurements from the Arctic Boundary Layer Expedition (ABLE 3B). It is found that decomposition of peroxyacetyl nitrate (PAN) can account for most of the NO(X) observed between the surface and 6.2 km altitude (aircraft ceiling). Forest fires represent the principal source of PAN in the region, implying the same origin for NO(X). There is, however, evidence for an unidentified source of NO(X) in occasional air masses subsiding from the upper troposphere. Isoprene emissions from boreal forests maintain high NO(X) concentrations in the continental boundary layer over eastern Canada by scavenging OH and NO3, thus slowing down conversion of NO(X) to HNO3, both in the daytime and at night. This effect is partly compensated by the production of CH3CO3 radicals during isoprene oxidation, which slows down the decomposition of PAN subsiding from the free troposphere. The peroxy radical concentrations estimated from concurrent measurements of NO and NO2 concentrations during ABLE 3B are consistent with values computed from our photochemical model below 4 km, but model values are low at higher altitudes. The discrepancy may reflect either a missing radical source in the model or interferences in the NO2 measurement.

Fan, S.-M↗
NASA NTRS1994

Anomalous HNO3/NO(x) ratio of remote tropospheric air: Conversion of nitric acid to formic acid and NO(x)?

The N oxidation ratio, (HNO3)/(NO(x)), in the free troposphere is measured at approx. 1 to 9 (averaging approx. 5), consistently lower than the values of 15-100 which known theory suggests to be reached rapidly. This discrepancy casts doubt on current models' abilities to predict effects of NO sources on remote (NO), and so also (O3) and (OH). HNO3-to-NO(x) recycling processes involving HCHO in solution are appealing explanations for the ratio. Known chemical theory are illustrated using a Lagrangian box model of the mid-troposphere which simulates characteristic episodes form NO(x) input to HNO3 washout. Ratio and budget constraint equations for No(y) can usefully restrict conceivable explanations of missing chemistry of fast nitrogen cycling; most explanations could be called 'fast-cycles' or 're-NO(x)-ification.' These equations also show how current global models may suggest spuriously good N oxidation ratios and errors in OH. Aerosol or cloud droplets reactions with HCHO may produce (a) formic acid (which needs an appropriate source) and NO(x), or alternatively, (b) hydroxymethyl nitrate (or methyl dinitrate), which might supply a large, variable amount of 'missing NO(y) not currently measurable except by NO(y) instruments.

Chatfield, Robert B.↗
NASA NTRS1993

Measurements of atmospheric dimethylsulfide, hydrogen sulfide, and carbon disulfide during GTE/CITE 3

Measurements of atmospheric dimethylsulfide (DMS), hydrogen sulfide (H2S), and carbon disulfide (CS2) were made over the North and South Atlantic Ocean as part of the Global Tropospheric Experiment/Chemical Instrumentation Test and Evaluation (GTE/CITE 3) project. DMS and CS2 samples were collected and analyzed using an automated gas chromatography/flame photometric detection system with a sampling frequency of 10 min. H2S samples were collected using silver nitrate impregnated filters and analyzed by fluorescence quenching. The DMS data from both hemispheres have a bimodal distribution. Over the North Atlantic this reflects the difference between marine and continental air masses. Over the South Atlantic it may reflect differences in the sea surface source of DMS, corresponding to different air mass source regions. The median boundary layer H2S and CS2 levels were significantly higher in the northern hemisphere than the southern hemisphere, reflecting the higher frequency of samples influenced by pollutant and/or coastal emissions. Composite vertical profiles of DMS and H2S are similar to each other, are consistent with a sea surface source. Vertical profiles of CS2 have maxima in the free troposphere, implicating a continental source. The low levels of H2S and CS2 found in the southern hemisphere constrain the role of these compounds in global budgets to significantly less than previously estimated.

Cooper, David J.↗
NASA NTRS1995

A new process and equipment for waste minimization: Conversion of NO(x) scrubber liquor to fertilizer

A new emissions control system for the oxidizer scrubbers that eliminates the current oxidizer liquor waste and lowers the NO(x) emissions is described. Since fueling and deservicing spacecraft constitute the primary operations in which environmental emissions occur, this will eliminate the second largest waste stream at KSC. This effort is in accord with Executive Order No. 12856 (Federal Compliance with Right-to-Know Laws and Pollution Prevention Requirements, data 6 Aug. 1993) and Executive Order No. 12873 (Federal Acquisition, Recycling, and Waste Prevention, dated 20 Oct. 1993). A recent study found that the efficiencies of the oxidizer scrubbers during normal operations ranged from 70 percent to 99 percent. The new scrubber liquor starts with 1% hydrogen peroxide at a pH of 7 and the process control system adds hydrogen peroxide and potassium hydroxide to the scrubber liquor to maintain those initial conditions. The result is the formation of a solution of potassium nitrate, which is sold as a fertilizer. This report describes the equipment and procedures used to monitor and control the conversion of the scrubber liquor to fertilizer, while reducing the scrubber emissions.

Parrish, Clyde F.↗
NASA NTRS1995

Synthesis of low color, atomic oxygen resistant polyimides

The purpose of this project was to develop low color, atomic oxygen resistant polyimides for potential applications on spacecraft in low earth orbit. The material is needed in order to protect satellites and spacecraft from the gases and radiation found at those altitudes. Phosphorous containing polyimides have been shown to be especially resistant to corrosion and weight loss under oxygen plasma. Unfortunately the color of these phosphorous containing polyimides is still too high for them to be good heat insulators. While they are not as effective as teflon, the current material of choice. polyimides are much less dense than teflon and would be especially valuable if they could be made with low color. The approach taken was to synthesize a monomer which would contain the elements needed for giving the final polyimide its desired properties. In particular the monomer should incorporate phosphine or phosphine oxides and have bulky side groups to block any color forming charge transfer structures. The target molecule, 3,5-di-(trifluoromethylphenyl)-bis(3-aminophenyl) phosphine oxide, (containing both a phosphine oxide group and a bulky ditrifluoromethylphenyl group) was synthesized via three reactions in overall yield of 21 percent. In addition, a model compound, bis(3-phenylamine) phenyl phosphine oxide, was synthesized two different ways in order to establish the conditions for the nitration of phosphine oxides and their reduction to the amine. Finally, a trisubstituted phosphine oxide was synthesized. In all, seven phosphorus containing organic compounds were synthesized, purified and characterized. The model compound was reacted with oxydiphthalic anhydride to form a polyamic acid with inherent viscosity of 0.34. This material was cast into a film and heated, forming a normally colored fairly strong polyimide with a Tg of 240 C. The target compound was reacted with 6-fluorodiphthalic anhydride to give a polyamic acid with inherent viscosity of 0.19 and cast to give a heavily cracked colored film with a Tg of 230 C.

MacInnes, Dave↗
NASA NTRS1995

Effects of stress ethylene inhibitors on sweet clover (Melilotus Alba L.) seedling growth in microgravity

Previous experiments from our lab have shown that seeds of sweet clover, when germinated and grown within the Fluid Processing Apparatus (FPA) on a slow rotating clinostat produce significantly greater levels of the volatile stress hormone, ethylene, when compared to seeds treated the same but without clinorotation. In both conditions, carbon dioxide levels reached high levels and seedling growth was inhibited. However, clinorotation inhibited growth to a greater extent. To help determine to what extent microgravity influences stress ethylene production and to what extent ethylene inhibits seedling growth, we have extended the above experiments by growing sweet clover in the presence of aminooxyacetic acid (AOA) and silver nitrate (AgNO3), inhibitors of stress ethylene biosynthesis and action, respectively. Seeds of sweet clover were germinated and grown for five days in the FPA under two gravity conditions: under stationary conditions on Earth and in microgravity onboard the space shuttle, Discovery (STS-63), which launched Feb. 3, 1995. Upon recovery, gas samples were aspirated from the growth chambers and carbon dioxide and ethylene concentrations were measured using a gas chromatograph. Then the tissue was weighed, photographed and fixed, and is current undergoing further morphological and microscopic characterization.

Gallegos, Gregory L.↗
NASA NTRS1996

Spectral Quantitation Of Hydroponic Nutrients

Instrument continuously monitors hydroponic solution by use of absorption and emission spectrometry to determine concentrations of principal nutrients, including nitrate, iron, potassium, calcium, magnesium, phosphorus, sodium, and others. Does not depend on extraction and processing of samples, use of such surrograte parameters as pH or electrical conductivity for control, or addition of analytical reagents to solution. Solution not chemically altered by analysis and can be returned to hydroponic process stream after analysis.

Schlager, Kenneth J.↗
NASA NTRS1996

HAN-based monopropellant assessment for spacecraft

The growing cost of space missions, the need for increased mission performance, and concerns associated with environmental issues are changing rocket design and propellant selection criteria. Whereas a propellant's performance was once defined solely in terms of specific impulse and density, now environmental safety, operability, and cost are considered key drivers. Present emphasis on these considerations has heightened government and commercial launch sector interest in Hydroxylammonium Nitrate (HAN)-based liquid propellants as options to provide simple, safe, reliable, low cost, and high performance monopropellant systems.

Jankovsky, Robert S.↗
NASA NTRS1996

Effect of KOH Concentration and Anions on the Performance of a Ni-H2 Battery Positive Plate

The capacity and voltage behavior of electrochemically impregnated sintered nickel positive plates was examined by galvanostatic charging and discharging in a flooded electrolyte cell. Three different concentrations of potassium hydroxide (KOH) (40, 31, and 26 percent) and 31 percent KOH containing dissolved nitrate, sulfate, or silicate were investigated. The end-of-charge voltage at C/10 charge and at 10 degrees C showed the following order: 40 percent KOH greater than 31 percent KOH alone and in the presence of the anions greater than 26 percent KOH. The mid discharge voltage at C/2 discharge was higher in 26 percent KOH, almost the same for 31 percent KOH with and without added contaminants, and much lower for 40 percent KOH. The plate capacity was marginally affected by cycling in all cases except for 40 percent KOH, where the capacity declined after 1,000 cycles at 80 percent depth of discharge (DOD). At the end of cycling, all the plates tested experienced a weight loss, except in the case of 31 percent KOH, as a result of active material extrusion. Cyclic voltammetry of miniature electrodes in 31 percent KOH showed that the cathodic peak potentials are less polarized in the presence and absence of silicate at -5 degrees C compared to 25 degrees C indicating a slightly higher voltage during discharge in a Ni-H2 battery. Futhermore, the features of the current-potential profile were practically unchanged in the presence of silicate.

Vaidyanathan, Hari↗
NASA NTRS1997

HAN-Based Monopropellant Propulsion System with Applications

NASA is developing a new monopropellant propulsion system for small, cost-driven spacecraft with AV requirements in the range of 10-150 m/sec. This system is based on a hydroxylammonium nitrate (HAN)/water/fuel monopropellant blend which is extremely dense, environmentally benign, and promises good performance and simplicity. State-of-art (SOA) small spacecraft typically employ either hydrazine or high pressure stored gas. Herein, a 'typical' small satellite bus is used to illustrate how a HAN-based monopropellant propulsion system fulfills small satellite propulsion requirements by providing mass and/or volume savings of SOA hydrazine monopropellants with the cost benefits of a stored nitrogen gas.

Jankovsky, Robert S.↗
NASA NTRS1993

Sequence and Genetic Characterization of etrA, an fnr Analog that Regulates Anaerobic Respiration in Shewanella putrefaciens MR-1

An electron transport regulatory gene, etrA, has been isolated and characterized from the obligate respiratory bacterium Shewanella putrefaciens MR-l. The deduced amino acid sequence of etrA (EtrA) shows a high degree of identity to both the Fnr of Escherichia coli (73.6%) and the analogous protein (ANR) of Pseudomonas aeruginosa (50.8%). The four active cysteine residues of Fnr are conserved in EtrA, and the amino acid sequence of the DNA-binding domains of the two proteins are identical. Further, S.putrefaciens etrA is able to complement an fnr mutant of E.coli. In contrast to fnr, there is no recognizable Fnr box upstream of the etrA sequence. Gene replacement etr.A mutants of MR-1 were deficient in growth on nitrite, thiosulfate, sulfite, trimethylamine-N-oxide, dimethyl sulfoxide, Fe(III), and fumarate, suggesting that EtrA is involved in the regulation of the corresponding reductase genes. However, the mutants were all positive for reduction of and growth on nitrate and Mn(IV), indicating that EtrA is not involved in the regulation of these two systems. Southern blots of S.putrefaciens DNA with use of etrA as a probe revealed the expected etrA bands and a second set of hybridization signals whose genetic and functional properties remain to be determined.

Saffarini, Daad A.↗
NASA NTRS1996

A 850 GHz SIS receiver employing silicon micro-machining technology

A 850 GHz superconductor-insulator-superconductor (SIS) heterodyne receiver which uses a radiofrequency tuned niobium tunnel junction fabricated on a 1 micron thick silicon nitrate membrane, is reported. From video and heterodyne measurements, it was calculated that the niobium film loss in the radiofrequency matching network is about 6.8 dB at 822 GHz. These results are approximately a factor of two higher than the theoretical loss predicted by the Mattis-Bardeen theory in the extreme anomalous limit. The junction design and the receiver configuration are described, including the mixer block, the membrane construction and the cooled optics. The performance tests using a Fourier transform spectrometer to measure the response of the radiofrequency matching network, and the SIS simulations of the receiver response to cold and hot loads, the infrared noise contribution and the overall mixer conversion efficiency, are reported. It is concluded that the receiver response is limited by the absorption loss in the radiofrequency matching network.

Kooi, J. W.↗
NASA NTRS1995

Environmentally Sound Processing Technology: JANNAF Safety and Environmental Protection Subcommittee and Propellant Development and Characterization Subcommittee Joint Workshop

Topics covered include: Risk assessment of hazardous materials, Automated systems for pollution prevention and hazardous materials elimination, Study design for the toxicity evaluation of ammonium perchlorate, Plasma sprayed bondable stainless surface coatings, Development of CFC-free cleaning processes, New fluorinated solvent alternatives to ozone depleting solvents, Cleaning with highly fluorinated liquids, Biotreatment of propyleneglycol nitrate by anoxic denitrification, Treatment of hazardous waste with white rot fungus, Hydrothermal oxidation as an environmentally benign treatment technology, Treatment of solid propellant manufacturing wastes by base hydrolysis, Design considerations for cleaning using supercritical fluid technology, and Centrifugal shear carbon dioxide cleaning.

Pickett, Lorri A.↗
NASA NTRS1997

Anthropogenic Sulfate, Clouds, and Climate Forcing

This research work is a joint effort between research groups at the Battelle Pacific Northwest Laboratory, Virginia Tech University, Georgia Institute of Technology, Brookhaven National Laboratory, and Texas A&M University. It has been jointly sponsored by the National Aeronautics and Space Administration, the U.S. Department of Energy, and the U.S. Environmental Protection Agency. In this research, a detailed tropospheric aerosol-chemistry model that predicts oxidant concentrations as well as concentrations of sulfur dioxide and sulfate aerosols has been coupled to a general circulation model that distinguishes between cloud water mass and cloud droplet number. The coupled model system has been first validated and then used to estimate the radiative impact of anthropogenic sulfur emissions. Both the direct radiative impact of the aerosols and their indirect impact through their influence on cloud droplet number are represented by distinguishing between sulfuric acid vapor and fresh and aged sulfate aerosols, and by parameterizing cloud droplet nucleation in terms of vertical velocity and the number concentration of aged sulfur aerosols. Natural sulfate aerosols, dust, and carbonaceous and nitrate aerosols and their influence on the radiative impact of anthropogenic sulfate aerosols, through competition as cloud condensation nuclei, will also be simulated. Parallel simulations with and without anthropogenic sulfur emissions are performed for a global domain. The objectives of the research are: To couple a state-of-the-art tropospheric aerosol-chemistry model with a global climate model. To use field and satellite measurements to evaluate the treatment of tropospheric chemistry and aerosol physics in the coupled model. To use the coupled model to simulate the radiative (and ultimately climatic) impacts of anthropogenic sulfur emissions.

Ghan, Steven J.↗