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At least 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
NASA NTRS1990

Possible atmospheric lifetimes and chemical reaction mechanisms for selected HCFCs, HFCs, CH3CCl3, and their degradation products against dissolution and/or degradation in seawater and cloudwater

For a wide variety of atmospheric species including CO2, HNO3, and SO2, dissolution in seawater or cloudwater followed by hydrolysis or chemical reaction represents a primary pathway for removal from the atmosphere. In order to determine if this mechanism can also remove significant amounts of atmospheric chlorofluorocarbons (HCFC's), fluorocarbons (HFC's), and their degradation products, an investigation was undertaken as part of the Alternative Fluorocarbons Environmental Acceptability Study (AFEAS). In this investigation, the rates at which CHCl2CF3 (HCFC-123), CCl2FCH3 (HCFC-141b), CClF2CH3 (HCFC-142b), CHClF2 (HCFC-22), CHClFCF3 (HCFC-124) CH2FCF3 (HFC-134a) CHF2CH3 (HFC-152a), CHF2CF3 (HFC-125), and CH3CCl3 can be dissolved in the oceans and in cloudwater were estimated from the species' thermodynamic and chemical properties using simple mathematical formulations to simulate the transfer of gases from the atmosphere to the ocean or cloudwater. The ability of cloudwater and rainwater to remove gas phase degradation products of these compounds was also considered as was the aqueous phase chemistry of the degradation products. The results of this investigation are described.

Wine, P. H.↗
NASA NTRS1990

Natural chlorine and fluorine in the atmosphere, water and precipitation

The geochemical cycles of chlorine and fluorine are surveyed and summarized as framework for the understanding of the global natural abundances of these species in the atmosphere, water, and precipitation. In the cycles the fluxes into and out of the atmosphere can be balanced within the limits of our knowledge of the natural sources and sinks. Sea salt from the ocean surfaces represent the predominant portion of the source of chlorine. It is also an important source of atmospheric fluorine, but volcanoes are likely to be more important fluorine sources. Dry deposition of sea salt returns about 85 percent of the salt released there. Precipitation removes the remainder. Most of the sea salt materials are considered to be cyclic, moving through sea spray over the oceans and either directly back to the oceans or deposited dry and in precipitation on land, whence it runs off into rivers and streams and returns to the oceans. Most of the natural chlorine in the atmosphere is in the form of particulate chloride ion with lesser amounts as gaseous inorganic chloride and methyl chloride vapor. Fluorine is emitted from volcanoes primarily as HF. It is possible that HF may be released directly form the ocean surface but this has not been confirmed by observation. HCl and most likely HF gases are released into the atmosphere by sea salt aerosols. The mechanism for the release is likely to be the provision of protons from the so-called excess sulfate and HNO3. Sea salt aerosol contains fluorine as F(-), MgF(+), CaF(+), and NaF. The concentrations of the various species of chlorine and fluorine that characterize primarily natural, unpolluted atmospheres are summarized in tables and are discussed in relation to their fluxes through the geochemical cycle.

Friend, James P.↗
NASA NTRS1989

Trends in stratospheric minor constituents

Photochemical models predict that increasing source gas concentrations are also expected to lead to changes in the concentrations of both catalytically active radical species (such as NO2, ClO, and OH) and inactive reservoir species (such as HNO3, HCl, and H2O). For simplicity, we will refer to all these as trace species. Those species that are expected to have increasing concentration levels are investigated. Additionally, the trace species concentration levels are monitored for unexpected changes on the basis of the measure increase in source gases. Carrying out these investigations is difficult due to the limited data base of measurements of stratospheric trace species. In situ measurements are made only infrequently, and there are few satelliteborne measurements, most over a time space insufficient for trend determination. Instead, ground-based measurements of column content must be used for many species, and interpretation is complicated by contributions from the troposphere or mesosphere or both. In this chapter, we examine existing measurements as published or tabulated.

Stolarski, R. S.↗
NASA NTRS1992

Natural Cycles, Gases

The major gaseous components of the exhaust of stratospheric aircraft are expected to be the products of combustion (CO2 and H2O), odd nitrogen (NO, NO2 HNO3), and products indicating combustion inefficiencies (CO and total unburned hydrocarbons). The species distributions are produced by a balance of photochemical and transport processes. A necessary element in evaluating the impact of aircraft exhaust on the lower stratospheric composition is to place the aircraft emissions in perspective within the natural cycles of stratospheric species. Following are a description of mass transport in the lower stratosphere and a discussion of the natural behavior of the major gaseous components of the stratospheric aircraft exhaust.

Douglass, Anne R.↗
NASA NTRS1991

Application of physical adsorption thermodynamics to heterogeneous chemistry on polar stratospheric clouds

Laboratory isotherms for the binding of several nonheterogeneously active atmospheric gases and for HCl to water ice are translated into adsorptive equilibrium constants and surface enthalpies. Extrapolation to polar conditions through the Clausius Clapeyron relation yields coverage estimates below the percent level for N2, Ar, CO2, and CO, suggesting that the crystal faces of type II stratospheric cloud particles may be regarded as clean with respect to these species. For HCl, and perhaps HF and HNO3, estimates rise to several percent, and the adsorbed layer may offer acid or proton sources alternate to the bulk solid for heterogeneous reactions with stratospheric nitrates. Measurements are lacking for many key atmospheric molecules on water ice, and almost entirely for nitric acid trihydrate as substrate. Adsorptive equilibria enter into gas to particle mass flux descriptions, and the binding energy determines rates for desorption of, and encounter between, potential surface reactants.

Elliott, Scott↗
NASA NTRS1991

Infrared spectra of solid films formed from vapors containing water and nitric acid

The paper presents infrared spectra recorded at 188 K for crystalline mono- and trihydrates of nitric acid formed by vapor deposition, along with spectra of fully deuterated forms of these compounds. The spectra are interpreted in terms of the known ionic structures of the hydrates and the known spectra of oxonium and nitrate ions. Two additional species were identified: a molecular hydrogen-bonded HNO3-H2O complex, stable only at temperatures below 120 or 150 K, and a substance considered to be a crystalline mixtgure of trihydrate and ice. The relevance of these findings to the stratospheric ozone hole problem is discussed.

Smith, Roland H.↗
NASA NTRS1991

Future aircraft and potential effects on stratospheric ozone and climate

Initial studies with LLNL models of global atmospheric chemical, radiative, and transport processes have indicated that substantial decreases in stratospheric ozone concentrations could result from emissions of NO(x) from aircraft flying in the stratosphere, depending on fleet size and magnitude of the engine emissions. These studies used homogeneous chemical reaction rates (e.g., gas-phase chemistry). Recent evidence indicates that reactions on particles in the stratosphere may be important. Heterogeneous chemical reactions convert NO(x) (NO and NO2) molecules to HNO3. This decreases the odd oxygen loss from the NO(x) catalytic cycle and increases the odd oxygen loss from the Cl(x) catalytic cycle. By including these heterogeneous reactions in the LLNL model, the relative partitioning of odd oxygen loss between these two families changes, with the result that emissions of NO(x) from proposed aircraft fleets flying in the stratosphere now increase ozone. Having these heterogeneous processes present also increases ozone concentration in the troposphere relative to gas-phase only chemistry calculations for emissions of NO(x) from subsonic aircraft.

Kinnison, Douglas E.↗
NASA NTRS1992

More rapid polar ozone depletion through the reaction of HOCl with HCl on polar stratospheric clouds

The direct reaction of HOCl with HCl is shown here to play a critical part in polar ozone loss. Observations of high levels of OClO and ClO in the springtime Antarctic stratosphere confirm that most of the available chlorine is in the form of ClO(x). But current photochemical models have difficulty converting HCl to ClO(x) rapidly enough in early spring to account fully for the observations. Here, a chemical model is used to show that the direct reaction of HOCl with HCl provides the missing mechanism. As alternative sources of nitrogen-containing oxidants have been converted in the late autumn to inactive HNO3 by known reactions on the sulfate layer aerosols, the reaction of HOCl with HCl on polar stratospheric clouds becomes the most important pathway for releasing that stratospheric chlorine which goes into polar night as HCl.

Prather, Michael J.↗
NASA NTRS1992

Visible luminescence from silicon wafers subjected to stain etches

Etching of Si in a variety of solutions is known to cause staining. These stain layers consist of porous material similar to that produced by anodic etching of Si in HF solutions. In this work, photoluminescence peaked in the red from stain-etched Si wafers of different dopant types, concentrations, and orientations produced in solutions of HF:HNO3:H2O was observed. Luminescence is also observed in stain films produced in solutions of NaNO2 in HF, but not in stain films produced in solutions of CrO3 in HF. The luminescence spectra are similar to those reported recently for porous Si films produced by anodic etching in HF solutions. However, stain films are much easier to produce, requiring no special equipment.

Fathauer, R. W.↗
NASA NTRS1991

Improved Limb Atmospheric Spectrometer (ILAS) for polar stratospheric trace gas measurements

The Improved Limb Atmospheric Spectrometer (ILAS) is a grating spectrometer designed to measure vertical profiles of high latitude stratospheric constituents in a solar occultation mode. ILAS measurement gases are ozone (03), methane (CH4), nitrous oxide (N2O), nitric acid (HNO3), water vapor (H2O), nitrogen dioxide (NO2), and CFC-11 using an IR channel. Temperature, pressure, and aerosol are also measured using a visible channel. The IR channel consists of 44 detector elements which cover the spectral range 6.2 to 11.8 microns, and the visible channel is composed of 1024 pixels that cover 753 to 784 nm. ILAS will be installed on the Advanced Earth Observing Satellite (ADEOS) which will be launched in 1995. Instrument design data are outlined.

Yokota, Tatsuya↗
NASA NTRS1992

Photochemical partitioning of the reactive nitrogen and chlorine reservoirs in the high-latitude stratosphere

The correlated set of measurements in the lower stratosphere from polar missions of the NASA ER-2 is used to derive partitioning of the major components of the reactive nitrogen and inorganic chlorine reservoirs. The results provide a consistent method for comparing distributions, and hence the controlling processes, between different areas of the near-polar regions. Clear evidence of the effects of heterogeneous processes in the atmosphere is found. Values for NO2, ClONO2, N2O5, and Cl2O2 are derived in a simplified steady-state model based on in situ NO, ClO, O3, temperature, and pressure measurements, laboratory-measured reaction rates; and modeled photodissociation rates. Values for the reservoir totals are independently derived from measurements of N2O, organic chlorine, and total reactive nitrogen. The relative abundances of the measured and derived species within the reservoirs are calculated, and the longer-lived species HCl and HNO3 are estimated as the residuals of their respective reservoirs.

Kawa, S. R.↗
NASA NTRS1992

A case of type I polar stratospheric cloud formation by heterogeneous nucleation

The NASA ER-2 aircraft flew on January 24, 1989, from Stavanger to Spitsbergen, Norway, at the 430-440 K potential temperature surface (19.2-19.8 km pressure altitude). Aerosols were sampled continuously by an optical particle counter (PMS-FSSP300) for concentration and size analyses, and during five 10-min intervals by four wire and one replicator impactor for concentration, size, composition, and phase analysis. During sampling, the air saturation of H2O with respect to ice changed from 20 to 100 percent, and of HNO3 with respect to nitric acid trihydrate (NAT) from subsaturation to supersaturation. Data from both instruments indicate a condensation of hydrochloric acid and, later, nitric acid on the background aerosol particles as the ambient temperature decreases along the flight track. This heterogeneous nucleation mechanism generates type I polar stratospheric cloud particles of 10-fold enhanced optical depth, which could play a role in stratospheric ozone depletion.

Pueschel, R. F.↗
NASA NTRS1992

Characterisation of Q-gases and other noble gas components in the Murchison meteorite

Noble gases in several HF/HCl resistant residues of the CM2 chondrite Murchison were measured by closed-system stepped etching, in order to study the planetary gases in their major carrier 'Q'-an ill-defined minor phase, perhaps merely a set of adsorption sites. Neon, Ar, Kr, Xe, and probably also He in 'Q' of Murchison have the same isotopic and nearly the same elemental abundances as their counterparts in Allende (CV3). The isotopic composition of Ne-Q is consistent with mass-dependent fractionation of either solar wind Ne or Ne from solar energetic particles. Unlike Allende, Murchison during HNO3 attack release, besides Q-gases, large amounts of two other Ne-components, Ne-E and Ne-A3, a third subcomponent of Ne-A. This work confirms that Q-gases of well-defined composition were an important noble gas component in the early solar system an are now found in various classes of meteorites, such as carbonaceous chondrites, ureilites, and ordinary chondrites. Ne-Q may have played a role in the formation of noble gas reservoirs in terrestrial planets.

Wieler, Rainer↗
NASA NTRS1991

High performance etchant for thinning p(+)-InP and its application to p(+)n InP solar cell fabrication

An etchant, namely (o-H3PO4)u: (HNO3)v: (H2O2)t: (H2O)1-(u+v+t) is developed for thinning, after contacting, the p(+) emitter layer of p(+)n InP structures made by thermal diffusion. Varying u, v, and t, reproducible etch rates of 5 to 110 nm/min are obtained. After thinning the 0.6- to 2.5-micron thick p(+) InP layer down to 60-250 nm, specular surfaces are obtained at up to 80 nm/min etch rate. Due to its intrinsic qualities the resisual P-rich oxide after thinning the emitter layer provides surface passivation of p(+) InP surfaces and can also serve as a first-layer AR coating.

Faur, Maria↗
NASA NTRS1991

Heterogeneous processes: Laboratory, field, and modeling studies

The efficiencies of chemical families such as ClO(x) and NO(x) for altering the total abundance and distribution of stratospheric ozone are controlled by a partitioning between reactive (active) and nonreactive (reservoir) compounds within each family. Gas phase thermodynamics, photochemistry, and kinetics would dictate, for example, that only about 1 percent of the chlorine resident in the lower stratosphere would be in the form of active Cl or ClO, the remainder existing in the reservoir compounds HCl and ClONO2. The consistency of this picture was recently challenged by the recognition that important chemical transformations take place on polar regions: the Airborne Antarctic Ozone Experiment (AAOE) and the Airborne Arctic Stratospheric Expedition (AASA). Following the discovery of the Antarctic ozone hole, Solomon et al. suggested that the heterogeneous chemical reaction: ClONO2(g)+HCl(s) yields Cl2(g)+HNO3(s) could play a key role in converting chlorine from inactive forms into a species (Cl2) that would rapidly dissociate in sunlight to liberate atomic chlorine and initiate ozone depletion. The symbols (s) and (g) denote solid phase, or adsorbed onto a solid surface, and gas phase, respectively, and represent the approach by which such a reaction is modeled rather than the microscopic details of the reaction. The reaction was expected to be most important at altitudes where PSC's were most prevalent (10 to 25 km), thereby extending the altitude range over which chlorine compounds can efficiently destroy ozone from the 35 to 45 km region (where concentrations of active chlorine are usually highest) to lower altitudes where the ozone concentration is at its peak. This chapter will briefly review the current state of knowledge of heterogeneous processes in the stratosphere, emphasizing those results obtained since the World Meteorological Organization (WMO) conference. Sections are included on laboratory investigations of heterogeneous reactions, the characteristics and climatology of PSC's, stratospheric sulfate aerosols, and evidence of heterogeneous chemical processing.

Poole, Lamont R.↗
NASA NTRS1992

Stratospheric aircraft exhaust plume and wake chemistry studies

This report documents progress to date in an ongoing study to analyze and model emissions leaving a proposed High Speed Civil Transport (HSCT) from when the exhaust gases leave the engine until they are deposited at atmospheric scales in the stratosphere. Estimates are given for the emissions, summarizing relevant earlier work (CIAP) and reviewing current propulsion research efforts. The chemical evolution and the mixing and vortical motion of the exhaust are analyzed to track the exhaust and its speciation as the emissions are mixed to atmospheric scales. The species tracked include those that could be heterogeneously reactive on the surfaces of the condensed solid water (ice) particles and on exhaust soot particle surfaces. Dispersion and reaction of chemical constituents in the far wake are studied with a Lagrangian air parcel model, in conjunction with a radiation code to calculate the net heating/cooling. Laboratory measurements of heterogeneous chemistry of aqueous sulfuric acid and nitric acid hydrates are also described. Results include the solubility of HCl in sulfuric acid which is a key parameter for modeling stratospheric processing. We also report initial results for condensation of nitric acid trihydrate from gas phase H2O and HNO3.

Miake-Lye, R. C.↗
NASA NTRS1992

Crop growth and associated life support for a lunar farm

Supporting human life on a lunar base will require growing many different food crops. This paper investigates the growth dynamics of four crops (wheat, soybeans, potatoes, and lettuce) for general similarities and differences, along with associated material flows of the gases, liquids, and solids in a lunar farm. The human dietary requirements are compared with the protein, carbohydrate, and lipid contents of these hydroponically grown, high-productivity crops to derive a lunar farm diet. A simple and general analytical model is used to calculate the mass fluxes of CO2, H2O, HNO3, and O2 during the life cycle of each of the four crops. The resulting farm crop areas and corresponding biomass production rates are given. One significant conclusion of this study is that there is a 'lipid problem' associated with the incorporation of these four crops into a viable diet.

Volk, Tyler↗
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↗