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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
NASA NTRS1985

Adsorption of O2, SO2, and SO3 on nickel oxide. Mechanism for sulfate formation

Calculations based on the atom superposition and electron delocalization molecular orbital (ASED-MO) technique suggest that O2 will adsorb perferentially end-on at an angle 45 deg from normal on a nickel cation site on the (100) surface of NiO. SO2 adsorption is also stronger on the nickel site; SO2 bonds through the sulfur atom is a plane perpendicular to the surface. Adsorption energies for SO3 on the nickel and oxygen sites are comparable in the perferred orientation in which the SO3 plane is parallel to the surface. On activation, SO3 adsorbed to an O2(-) site forms a trigonal pyramidal SO4 species which yields, with a low barrier, a tetrahedral sulfate anion. Subsequently the anion reorients on the surface. Possibilities for alternative mechanisms which require the formation of Ni3(+) or O2(-) are discussed. NiSO4 thus formed leads to the corrosion of Ni at high temperatures in the SO2+O2/SO3 The SO2+O2/SO3 atmosphere, as discussed in the experimental literature.

Mehandru, S. P.↗
NASA NTRS1986

Adsorption of O2, SO2, and SO3, on nickel oxide - Mechanism for sulfate formation

Calculations based on the atom superposition and electron delocalization molecular orbital technique suggest that O2 will adsorb preferentially end-on at an angle 45 deg from normal on a nickel cation site on the (100) surface of NiO. SO2 adsorption is also stronger on the nickel site; SO2 bonds through the sulfur atom in a plane perpendicular to the surface. Adsorption energies for SO3 on the nickel and oxygen sites are comparable in the preferred orientation in which the SO3 plane is parallel to the surface. The calculations suggest that the strength of adsorption varies as O2 greater than SO2 greater than SO3. On activation, SO3 adsorbed to an O(2-) site forms a trigonal pyramidal SO4 species which yields, with a low barrier, a tetrahedral sulfate anion. Subsequently the anion reorients on the surface. Alternative mechanisms which require the formation of Ni(3+) or O(-) are discussed. NiSO4 thus formed may play a passivating role for the corrosion of Ni at low temperatures in the SO2 + O2 + SO3 atmospheres and an active role at high temperatures, as discussed in the experimental literature.

Mehandru, S. P.↗
NASA NTRS1987

Ferric sulfates on Mars

Evidence is presented for the possible existence of ferric sulfato complexes and hydroxo ferric sulfate minerals in the permafrost of Mars. A sequential combination of ten unique conditions during the cooling history of Mars is suggested which is believed to have generated an environment within Martian permafrost that has stabilized Fe(3+)-SO4(2-)-bearing species. It is argued that minerals belonging to the jarosite and copiapite groups could be present in Martian regolith analyzed in the Viking XRF measurements at Chryse and Utopia, and that maghemite suspected to be coating the Viking magnet arrays is a hydrolysate of dissolved ferric sulfato complexes from exposed Martian permafrost.

Burns, Roger G.↗
NASA NTRS1988

Regional aerosol chemistry of the Amazon Basin during the dry season

The distribution and chemical composition of the atmospheric aerosol over the Amazon Basin forest were determined during the 1985 July-August dry season, using data on the aerosol chemical constituent concentration collected during the NASA Global Tropospheric Experiment Amazon Boundary Layer Experiment 2A mission. The results of the analyses suggest that there is a remarkable compositional and spatial homogeneity of the atmospheric aerosol on an extensive regional scale. Particulate organic carbon is the dominant component of the atmospheric aerosol, exhibiting an average concentration of about 740 nmol/cu m in the mixed layer and about 220 nmol/cu m in free tropospheric air. Oxalate and SO4(2-) exhibited the greatest enrichment in the mixed layer, while Cl(-) showed essentially no enrichment. The aerosol in the Amazonian atmosphere is essentially acid-base neutral, primarily as a result of incorporation of NH(+), which is presumably derived from NH3 released by the forest ecosystem.

Talbot, R. W.↗
NASA NTRS1988

Biomass-burning emissions and associated haze layers over Amazonia

The characteristics of haze layers, which were visually observed over the central Amazon Basin during many of the Amazon Boundary Layer Experiment 2A flights in July/August 1985, were investigated by remote and in situ measurements, using the broad range of instrumentation and sampling equipment on board the Electra aircraft. It was found that these layers strongly influenced the chemical and optical characteristics of the atmosphere over the eastern Amazon Basin. Relative to the regional background, the concentrations of CO, CO2, O3, and NO were significantly elevated in the plumes and haze layers, with the NO/CO ratio in fresh plumes much higher than in the aged haze layers. The haze aerosol was composed predominantly of organic material, NH4, K(+), NO3(-), SO4(2-), and organic anions (formate, acetate, and oxalate).

Andreae, M. O.↗
NASA NTRS1988

Particulate emissions from a mid-latitude prescribed chaparral fire

Particulate emission from a 400-acre prescribed chaparral fire in the San Dimas Experimental Forest was investigated by collecting smoke aerosol on Teflon and glass-fiber filters from a helicopter, and using SEM and EDAX to study the features of the particles. Aerosol particles ranged in size from about 0.1 to 100 microns, with carbon, oxygen, magnesium, aluminum, silicon, calcium, and iron as the primary elements. The results of ion chromatographic analysis of aerosol-particle extracts (in water-methanol) revealed the presence of significant levels of NO2(-), NO3(-), SO4(2-), Cl(-), PO4(3-), C2O4(2-), Na(+), NH4(+), and K(+). The soluble ionic portion of the aerosol was estimated to be about 2 percent by weight.

Cofer, Wesley R., III↗
NASA NTRS1989

Bio-markers and the search for extinct life on Mars

In order to predict what biomarkers could be used on Mars, several biomarkers, or key signatures, of extinct life on earth are identified. Some of these biomarkers which may be applicable to Mars include reduced carbon and nitrogen compounds, CO3(2-), SO4(2-), NO3(-), Mg, Mn, Fe, and the isotopic ratios of C, N, and S. It is suggested that a fully equipped Mars rover might be able to perform analyses to measure most of these biomarkers while on the Martian surface.

Schwartz, D. E.↗
NASA NTRS1989

Condensed nitrate, sulfate, and chloride in Antarctic stratospheric aerosols

The 1987 Airborne Antarctic Ozone Experiment, in which the NO3, Cl, and SO4 contents of stratospheric aerosols were estimated, is discussed. The aerosol size and chemical composition measurements were carried out on samples collected during August 17 to September 4, 1987. The data indicate that condensed nitrate is found below a threshold temperature of 193.6 + or - 3.0 K, which is generally found at latitudes exceeding 64 deg S. A negative correlation exists between condensed nitrate and ozone correlation.

Pueschel, R. F.↗
NASA NTRS1989

Wet chemical techniques for passivation of YBa2Cu3O7(7-x)

Wet chemical techniques are described for treatment of YBa2Cu3O(7-x) surfaces, resulting in the formation of native compounds with little or no reactivity to water. Promising native compounds include CuI, BaSO4, CuS, Cu2S, and the oxalates, all of which are either insoluble or have very low solubility in water. Treatment with dilute HI results in the formation of a native iodide film which is 80-90 percent CuI with small amounts of YI3 and BaI2. Treatment with dilute H2SO4 results in the formation of a film which is 95 percent BaSO4 and 5 percent Y2(SO4)3. Cu2S is formed on the surface with a dilute Na2S solution. An oxalate film with equal amounts of Y2(C2O4)3 and BaC2O4 results from treatment with dilute oxalic acid. X-ray photoelectron spectra show no significant changes when the sulfide, sulfate, or oxalate films are dipped in water, while the iodide film shows evidence of Cu(OH)2 formation.

Vasquez, R. P.↗
NASA NTRS1991

Annular denuders for use in global climate and stratospheric measurements of acidic gases and particles

Measurements of acidic and basic gases that coexist with fine particle (less than 2.5 micron) may be useful for determining the impact of these species on global climate changes and determining species that influence stratospheric ozone levels. Annular denuders are well suited for this purpose. A new concentric annular denuder system, consisting of a three channel denuder, a Teflon coated cyclone preseparator, and a multistage filter pack was developed, evaluated, and shown to provide reliable atmospheric measurements of SO2, HNO2, HNO3, NH3, SO4(=), NH4(+), NO3(-), and H(+). For example, the precision of the annular denuder for the ambient measurements of HNO3 and nitrates at concentrations between 0.1 to 3 microgram/cu m was + or - 12 and 16 pct., respectively. The 120 x 25 mm three channel denuder is encased in a stainless steel sheath and has annular spaces that are 1 mm wide. This design was shown to have nearly identical capacity for removal of SO2 as conventional 210 x 25 mm single channel denuder configurations. The cyclone preseparator was designed and tested to have a D sub 50 cutoff diameter of 2.5 micron and minimal retention of HNO3.

Stevens, Robert K.↗
NASA NTRS1991

Composition and spectral characteristics of ambient aerosol at Mauna Loa Observatory

The spectral and the chemical characteristics of ambient aerosol at Mauna Loa Observatory (Hawaii) were determined in aerosol particles continuously sampled during an 8-day period in August 1986. During this period, the chemical species in the ambient aerosol varied considerably. During the major fraction of the sampling period, the aerosol was acidic due to predominance of (NH4)3H(SO4)2, NH4HSO4, or H2SO4. Aerosol samples showed much higher absorbance at 9.1 microns than at 10.6 microns. Moreover, changes in chemical composition from the neutral (NH4)2SO4 aerosol to more acidic sulphate forms were accompanied by substantial changes in the samples' absorbance at 9.1 microns (with lesser changes in the 10.6-micron absorptions).

Johnson, Stanley A.↗
NASA NTRS1991

Midinfrared spectral investigations of carbonates: Analysis of remotely sensed data

Recent airborne thermal infrared observations of Mars from the Kuiper Airborne Observatory (KAO) have provided evidence for the presence of carbonates, sulfates, and hydrates. Using the optical properties of calcite and anhydrite, it was estimated that CO3's and SO4's constituted about 1 to 3 and 10 to 15 wt. percent, repectively of the materials composing the atmospheric dust. Using the derived value as an estimate of total CO3 abundance, and making an assumption that the CO3's were uniformly distributed within the Martian regolith, it was estimated that such a CO3 reservoir could contain roughly 2 to 5 bars of CO2. While the results indicate that several volatile-bearing materials are present on Mars, the observations from the KAO are inherently limited in their ability to determine the spatial distributions of these materials. However, previous spacecraft observations of Mars provide both the spectral coverage necessary to identify these materials, as well as the potential for investigating their spatial variability. This has prompted us to pursue a reinvestigation of the Mariner 6 and 7 infrared spectrometer and Mariner 9 infrared interferometer spectrometer observations. The former data have been recently made available in digital format and calibration of wavelengths and intensities are almost complete. Additionally, we are pursuing the derivation of optical constants of more appropriate carbonates and sulfates.

Roush, T.↗
NASA NTRS1992

Understanding the variation in the millimeter-wave emission of Venus

Recent observations of the millimeter-wave emission from Venus at 112 GHz (2.6 mm) have shown significant variations in the continuum flux emission that may be attributed to the variability in the abundances of absorbing constituents in the Venus atmosphere. Such constituents include gaseous H2SO4, SO2, and liquid sulfuric acid (cloud condensates). Recently, Fahd and Steffes have shown that the effects of liquid H, SO4, and gaseous SO2 cannot completely account for this measured variability in the millimeter-wave emission of Venus. Thus, it is necessary to study the effect of gaseous H2SO4 on the millimeter-wave emission of Venus. This requires knowledge of the millimeter-wavelength (MMW) opacity of gaseous H2SO4, which unfortunately has never been determined for Venus-like conditions. We have measured the opacity of gaseous H2SO4 in a CO2 atmosphere at 550, 570, and 590 K, at 1 and 2 atm total pressure, and at a frequency of 94.1 GHz. Our results, in addition to previous centimeter-wavelength results are used to verify a modeling formalism for calculating the expected opacity of this gaseous mixture at other frequencies. This formalism is incorporated into a radiative transfer model to study the effect of gaseous H2SO4 on the MMW emission of Venus.

Fahd, Antoine K.↗
NASA NTRS1992

An experimental study of growth and phase change of polar stratospheric cloud particles

This report describes the progress made on understanding phase changes related to solutions which may comprise Polar Stratospheric Clouds. In particular, it is concerned with techniques for investigating specific classes of metastability and phase change which may be important not only in Polar Stratospheric Clouds but in all atmospheric aerosols in general. While the lower level atmospheric aerosol consists of mixtures of (NH4)(SO4)2, NH4HSO4, NaCl among others, there is evidence that aerosol at PSC levels is composed of acid aerosol, either injected from volcanic events (such as Pinatubo) or having diffused upward from the lower atmosphere. In particular, sulfuric acid and nitric acid are known to occur at PSC levels, and are suspected of catalyzing ozone destruction reactions by adsorption on surfaces of crystallized particles. The present study has centered on two approaches: (1) the extent of supercooling (with respect to ice) and supersaturation (with respect to hydrate) and the nature of crystal growth in acid solutions of specific molality; and (2) the nature of growth from the vapor of HNO3 - H2O crystals both on a substrate and on a pre-existing aerosol.

Hallett, John↗
NASA NTRS1992

Soluble species in the Arctic summer troposphere - Acidic gases, aerosols, and precipitation

The large-scale spatial distribution from 0.15-to 6 km altitude in the North American Arctic troposphere of several soluble acidic gases and major aerosol species during the summertime is reported. The distribution is found to be compositionally consistent on a large spatial scale. The summertime troposphere is an acidic environment, with HCOOH and CH3COOH the principal acidic gases while acidic sulfate aerosols dominate the particulate phase. There appears to be a surface source of NH3 over the pack ice which may originate from decay of dead marine organisms on the ice surface, evolution from surface ocean waters in open ice leads, or release from rotting sea ice. At low altitude over the pack ice this NH34 appears to partially neutralize aerosol acidity. Over sub-Arctic tundra in southeastern Alaska, inputs of marine biogenic sulfur from the Bering Sea appear to be an important source of boundary layer aerosol SO4(2-). The rainwater acidity over the tundra is typical of remote regions.

Talbot, R. W.↗
NASA NTRS1993

Rates of oxidative weathering on the surface of Mars

A model of acid weathering is proposed for the iron-rich basalts on Mars. Aqueous oxidation of iron sulfides released SO4(2-) and H(+) ions that initiated the dissolution of basaltic ferromagnesian silicates and released Fe(2+) ions. The Fe(2+) ions eventually underwent ferrolysis reactions and produced insoluble hydrous ferric oxide phases. Measurements of the time-dependence of acid weathering reactions show that pyrrhotite is rapidly converted to pyrite plus dissolved ferrous iron, the rate of pyrite formation decreasing with rising pH and lower temperatures. On Mars, oxidation rates of dissolved Fe(2+) ions in equatorial melt-waters in contact with the atmosphere are estimated to lie in the range 0.3-3.0 ppb Fe/yr over the pH range 2 to 6. Oxidation of Fe(2+) ions is estimated to be extremely slow in brine eutectic solutions that might be present on Mars and to be negligible in the frozen regolith.

Burns, Roger G.↗
NASA NTRS1994

Ion-assisted tropospheric OH measurement technique

The present technique measures atmospheric OH concentrations by first titrating OH into isotopically labeled H2(exp 34)SO4 by a series of gas phase reactions in an effectively wall-less flow tube reactor on a time-scale which is short in comparison to the OH lifetime. The gas phase H2SO4 concentration is then determined by reacting it with NO3(-)(center dot)HNO3 ions in a flow tube, and subsequently measuring the resulting (HSO4(-))/(NO3(-)) ion ratio. Since the determination of H2SO4 concentration does not depend on the measurement of an absolute photon flux or chemical concentration but rather only on the relative concentration measurement of two fairly similar mass ions in conjunction with a fixed reaction time and reaction rate coefficient, no in-field calibration technique should be required. The ion-assisted OH measurement technique provides a concentration measurement about once each 10 to 20 seconds and had a detection sensitivity less than or equal to 1 x 10(exp 5) molecules/cu cm (2 standard deviations) with an integration time of 5 minutes during the past field study. Typically, the total background signal level is in the low 10(exp 6) molecule/cu cm range with the scatter in this background (or background noise in 5 minutes) in the mid 10(exp 4) molecules/cu cm range.

Eisele, Fred L.↗
NASA NTRS1994

Copper-containing ceramic precursor synthesis: Solid-state transformations and materials technology

Three copper systems with relevance to materials technology are discussed. In the first, a CuS precursor, Cu4S1O (4-methylpyridine)(sub 4)- (4-MePy), was prepared by three routes: reaction of Cu2S, reaction of CuBr-SMe2, and oxidation of copper powder with excess sulfur in 4-methylpyridine by sulfur. In the second, copper powder was found to react with excess thiourea (H2NC(S)NH2) in 4-methylpyridine to produce thiocyanate (NCS(-)) complexes. Three isolated and characterized compounds are: Cu(NCS)(4-MePy)(sub 2), a polymer, (4-MePy-H)(Cu(NCS)(sub 3)(4-MePy)(sub 2)), a salt, and t-Cu(NCS)(sub 2)(4-MePy)(sub 4). Finally, an attempt to produce a mixed-metal sulfide precursor of Cu and Ga in N-methylimidazole (N-MeIm) resulted in the synthesis of a Cu-containing polymer, Cu(SO4)(N-MeIm). The structures are presented; the chemistry will be briefly discussed in the context of preparation and processing of copper-containing materials for aerospace applications.

Hepp, Aloysius F.↗