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NASA NTRS1994

Ozone response to enhanced heterogeneous processing after the eruption of Mt. Pinatubo

Increases in aerosol loading after the Pinatubo eruption are expected to cause additional ozone depletion. Even though aerosol loadings were highest in the winter of 1991-1992, recent analyses of satellite and ground-based ozone measurements indicate that ozone levels in the winter of 1992-1993 are the lowest recorded in recent years, raising the question of the mechanisms responsible for such behavior. We have incorporated aerosol surface areas derived from the Stratospheric Aerosol and Gas Experiment II (SAGE-II) measurements into our two-dimensional model. Inclusion of heterogeneous chemsitry on these enhanced aerosol surfaces yields maximum ozone reductions during the winter of 1992-1993 in the Northern Hemisphere, consistent with those derived from observations. This delayed behavior is due to the combination of the non-linear nature of the impact of heterogeneous reactions as a function of aerosol surface area, and the long time constants for ozone in the lower stratosphere. If heterogeneous mechanisms are primarily responsible for the low 1992-1993 ozone levels, we expect ozone concentrations to start recovering in 1994.

Rodriguez, Jose M.↗

NASA NTRS1999

A Model for Generation of Martian Surface Dust, Soil and Rock Coatings: Physical vs. Chemical Interactions, and Palagonitic Plus Hydrothermal Alteration

This model is one of many possible scenarios to explain the generation of the current surface material on Mars using chemical, magnetic and spectroscopic data from Mars and geologic analogs from terrestrial sites. One basic premise is that there are physical and chemical interactions of the atmospheric dust particles and that these two processes create distinctly different results. Physical processes distribute dust particles on rocks, forming physical rock coatings, and on the surface between rocks forming soil units; these are reversible processes. Chemical reactions of the dust/soil particles create alteration rinds on rock surfaces or duricrust surface units, both of which are relatively permanent materials. According to this model the mineral components of the dust/soil particles are derived from a combination of "typical" palagonitic weathering of volcanic ash and hydrothermally altered components, primarily from steam vents or fumeroles. Both of these altered materials are composed of tiny particles, about 1 micron or smaller, that are aggregates of silicates and iron oxide/oxyhydroxide/sulfate phases. Additional information is contained in the original extended abstract.

Bishop, J. L.↗

NASA NTRS1987

The spectroscopic chemical and photophysical properties of Martian soils and their analogs

The program of research outlined should advance significantly the understanding of the spectral signal of montmorillonites in general and the variations produced in it by structural and surface ferric and ferrous iron and interlayer water as a function of several environmental conditions that are different between Earth and Mars. In addition, an extensive data base was collected providing spectral characterization of several features (iron, both surface and structural, OH-groups, both structural and from adsorbed water and O(-) centers) that are known, or thought to be, influential in directing the surface activity of these important materials. With this data base with which to assess the results of the Viking labeled release simulation studies, it should be possible to gain important insights into the mechanisms of surface reactivity for this important chemical reaction. The results to be gained from these studies will provide a significant body of ground base truth from which to assess: the presence of smectite clays on Mars; the mineralogical form in which the Martian iron is bound; establish upper limits on the present surface water content of Martian soils; perhaps provide insights on the Martian surface radiation history; and to make strong predictions about the nature of surface chemistry on Mars, if iron-bearing clays are a significant component of the surface mineralogical assemblage.

Coyne, Lelia M.↗

NASA NTRS1990

The effect of H2O and pretreatment on the activity of a Pt/SnO2 catalyst

CO oxidation catalysts with high activity at 25 C to 100 C are important for long-life, closed-cycle operation of pulsed CO2 lasers. A reductive pretreatment with either CO or H2 has been shown to significantly enhance the activity of a commercially available platinum on tin (IV) oxide (Pt/SnO2) catalyst relative to an oxidative or inert pretreatment or no pretreatment. Pretreatment at temperatures of 175 C and above causes an initial dip in the observed CO2 yield before the steady-state yield is attained. This dip has been found to be caused by dehydration of the catalyst during pretreatment and is readily eliminated by humidifying the catalyst or the reaction gas mixture. It is hypothesized that the effect of humidification is to increase the concentration of OH groups on the catalyst surface which play a role in the reaction mechanism.

Vannorman, John D.↗

NASA NTRS1989

The effects of pretreatment conditions on a Pt/SnO2 catalyst for the oxidation of CO in CO2 lasers

CO oxidation catalysts with high activity at 25 to 100 C are important for long life, closed cycle operation of pulsed CO2 lasers. A reductive pretreatment with either CO or H2 was shown to significantly enhance the activity of a commercially available platinum on tin (IV) oxide (Pt/SnO2) catalyst relative to an oxidative or inert pretreatment of no pretreatment. Pretreatment at temperatures of 175 C and above causes an initial dip in the observed CO2 yield before the steady state yield is attained. This dip was found to be caused by dehydration of the catalyst during pretreatment and is readily eliminated by humidifying the catalyst or the reaction gas mixture. It is hypothesized that the effect of humidification is to increase the concentration of OH groups on the catalyst surface which play a role in the reaction mechanism.

Schryer, David R.↗

NASA NTRSDate not supplied

Multiscale Modeling of the Uptake of Hydrogen Chloride on Anodized Aluminum in Relevance to Spacecraft Fire Safety

Fire safety is a critical component of space missions. An electrical fire within the spacecraft often produces gaseous hydrogen chloride (HCl) from the smoldering of wire insulation. These gases tend to stick to the interior materials of the spacecraft, which is often comprised of treated aluminum. Determining the rate of uptake for HCl by aluminum helps the safe design of the spacecraft to reduce catastrophic mission risk. Our previous studies showed that a one-step global reaction model for adsorption of HCl on aluminum is incapable of predicting the experimentally measured HCl uptake of anodized aluminum, compared to other treatments with thinner oxide layers. X-ray photoelectron spectroscopy revealed that aluminum chloride is found deep in the oxide layer of the anodized aluminum, implying that the transport of HCl within the oxide layer covering the aluminum surface must be considered. This work uses a multiscale modeling approach to predict the uptake of HCl. A pore model is developed wherein the HCl reacts with the aluminum oxide pore walls to create an aluminum chloride layer. The HCl then diffuses through that layer for further reaction, until the diffusion resistance grows too large, and the surface is said to be saturated. The pore model is then coupled with the reactor-scale model to predict overall HCl uptake. Results show that this new multiscale approach predicts the uptake of HCl far more accurately than previously used single-scale models.

Modeling↗

NASA NTRS1987

Selected materials issues associated with Space Station

Compatibility of Space Station hardware with the space environment is one of the major materials development issues. The projected long life of the Space Station elements (about 30 years for structural components and 20 years for power systems), the large number of day/night thermal cycles that have to be withstood during the life of the Station, and the effects of atomic oxygen and UV irradiation on exposed surfaces demand new considerations in selection of materials. Reaction efficiencies of materials for Space Station applications derived from LEO experiments are presented together with surface recession predictions for various Space Station components. Developments in the areas of protective coatings and of laboratory facilities for evaluating the effects of atomic oxygen are discussed.

Leger, L.↗

NASA NTRS1972

High-pressure liquid-monopropellant strand combustion.

Examination of the influence of dissolved gases on the state of the liquid surface during high-pressure liquid-monopropellant combustion through the use of a strand burning experiment. Liquid surface temperatures were measured, using fine-wire thermocouples, during the strand combustion of ethyl nitrate, normal propyl nitrate, and propylene glycol dinitrate at pressures up to 81 atm. These measurements were compared with the predictions of a variable-property gas-phase analysis assuming an infinite activation energy for the decomposition reaction. The state of the liquid surface was estimated using a conventional low-pressure phase equilibrium model, as well as a high-pressure version that considered the presence of dissolved combustion-product gases in the liquid phase. The high-pressure model was found to give a superior prediction of measured liquid surface temperatures. Computed total pressures required for the surface to reach its critical mixing point during strand combustion were found to be in the range from 2.15 to 4.62 times the critical pressure of the pure propellant. Computed dissolved gas concentrations at the liquid surface were in the range from 35 to 50% near the critical combustion condition.

Faeth, G. M.↗

NASA NTRS2003

The electrochemical properties of the purine bases : at the interface between biological conjugates to inorganic surfaces

The study of the charge transfer and interfacial reactions of the purine bases in physiological solutions provides valuable knowledge, as these processes are relevant to the origins of life. It has been proposed that the adsorption of the adsorption of the purine bases on an inorganic surface could serve as a template for specifying the arrangement of amino acids in peptides.

purines↗

NASA NTRS2011

Carbon Isotope Measurements of Experimentally-Derived Hydrothermal Mineral-Catalyzed Organic Products by Pyrolysis-Isotope Ratio Mass Spectrometry

We report results of experiments to measure the C isotope composition of mineral catalyzed organic compounds derived from high temperature and high pressure synthesis. These experiments make use of an innovative pyrolysis technique designed to extract and measure C isotopes. To date, our experiments have focused on the pyrolysis and C isotope ratio measurements of low-molecular weight intermediary hydrocarbons (organic acids and alcohols) and serve as a proof of concept for making C and H isotope measurements on more complicated mixtures of solid-phase hydrocarbons and intermediary products produced during high temperature and high pressure synthesis on mineral-catalyzed surfaces. The impetus for this work stems from recently reported observations of methane detected within the Martian atmosphere [1-4], coupled with evidence showing extensive water-rock interaction during Martian history [5-7]. Methane production on Mars could be the result of synthesis by mineral surface-catalyzed reduction of CO2 and/or CO by Fischer-Tropsch Type (FTT) reactions during serpentization reactions [8,9]. Others have conducted experimental studies to show that FTT reactions are plausible mechanisms for low-molecular weight hydrocarbon formation in hydrothermal systems at mid-ocean ridges [10-12]. Further, recent experiments by Fu et al. [13] focus on examining detailed C isotope measurements of hydrocarbons produced by surface-catalyzed mineral reactions. Work described in this paper details the experimental techniques used to measure intermediary organic reaction products (alcohols and organic acids).

Socki, Richard A.↗

NASA NTRS1989

Venus volcanism: Rate estimates from laboratory studies of sulfur gas-solid reactions

Thermochemical reactions between sulfur-bearing gases in the atmosphere of Venus and calcium-, iron-, magnesium-, and sulfur-bearing minerals on the surface of Venus are an integral part of a hypothesized cycle of thermochemical and photochemical reactions responsible for the maintenance of the global sulfuric acid cloud cover on Venus. SO2 is continually removed from the Venus atmosphere by reaction with calcium bearing minerals on the planet's surface. The rate of volcanism required to balance SO2 depletion by reactions with calcium bearing minerals on the Venus surface can therefore be deduced from a knowledge of the relevant gas-solid reaction rates combined with reasonable assumptions about the sulfur content of the erupted material (gas + magma). A laboratory program was carried out to measure the rates of reaction between SO2 and possible crustal minerals on Venus. The reaction of CaCO3(calcite) + SO2 yields CaSO4 (anhydrite) + CO was studied. Brief results are given.

Ehlers, K.↗

NASA NTRS1987

Antarctic stratospheric chemistry of chlorine nitrate, hydrogen chloride, and ice - Release of active chlorine

The reaction rate between atmospheric hydrogen chloride (HCl) and chlorine nitrate (ClONO2) is greatly enhanced in the presence of ice particles; HCl dissolves readily into ice, and the collisional reaction probability for ClONO2 on the surface of ice with HCl in the mole fraction range from about 0.003 to 0.010 is in the range from about 0.05 to 0.1 for temperatures near 200 K. Chlorine is released into the gas phase on a time scale of at most a few milliseconds, whereas nitric acid (HNO3), the other product, remains in the condensed phase. This reaction could play an important role in explaining the observed depletion of ozone over Antarctica; it releases photolytically active chlorine from its most abundant reservoir species, and it promotes the formation of HNO3 and thus removes nitrogen dioxide from the gas phase. Hence it establishes the necessary conditions for the efficient catalytic destruction of ozone by halogenated free radicals.

Molina, Mario J.↗

NASA NTRS2003

Universal Responses of Cyclic-Oxidation Models Studied

Oxidation is an important degradation process for materials operating in the high-temperature air or oxygen environments typical of jet turbine or rocket engines. Reaction of the combustion gases with the component material forms surface layer scales during these oxidative exposures. Typically, the instantaneous rate of reaction is inversely proportional to the existing scale thickness, giving rise to parabolic kinetics. However, more realistic applications entail periodic startup and shutdown. Some scale spallation may occur upon cooling, resulting in loss of the protective diffusion barrier provided by a fully intact scale. Upon reheating, the component will experience accelerated oxidation due to this spallation. Cyclic-oxidation testing has, therefore, been a mainstay of characterization and performance ranking for high-temperature materials. Models simulate this process by calculating how a scale spalls upon cooling and regrows upon heating (refs. 1 to 3). Recently released NASA software (COSP for Windows) allows researchers to specify a uniform layer or discrete segments of spallation (ref. 4). Families of model curves exhibit consistent regularity and trends with input parameters, and characteristic features have been empirically described in terms of these parameters. Although much insight has been gained from experimental and model curves, no equation has been derived that can describe this behavior explicitly as functions of the key oxidation parameters.

Smialek, James L.↗

NASA NTRS1986

Isotopic effects in the collinear reactive FHH system

Exact quantum reaction probabilities for a collinear model of the F + HH, HD, DD and DH reactions on the MV potential energy surface have been computed using hyperspherical coordinates. The results, obtained up to a total energy of 1.8 eV, show three main features: (1) resonances, whose positions and widths are analyzed simply in the hyperspherical formalism; (2) a slowly varying background increasing for FHD, decreasing for FDH, and oscillating for FHH and FDD, whose variations are interpreted by classical dynamics; and (3) partial reaction probabilities revealing decreasing vibrational adiabaticity in the order FHH-FDD-FHD-FDH.

Lepetit, B.↗

NASA NTRS1984

Interaction of atomic oxygen with solid surfaces at orbital altitudes (A0114)

The basic approach to this experiment is to expose a wide variety of material surfaces to the atomic flux in orbit. The experiment is passive and depends on preflight and postflight measurements of the test surfaces in the laboratory. The experiment will also include a reflectometer device to measure atomic beam reflection angles and thus momentum accommodations, and a unique passive spacecraft attitude sensor. Samples consisting of solid disks or thin film coatings on substrate disks will be mounted in a panel. The face of this panel will be flown on Long Duration Exposure Facility normal to the incident stream of oxygen atoms. Each disk will have part of its front surface masked so exposure to the atomic-oxygen reaction will be limited to selected areas, the shadowed areas being used as control surfaces in the measurements. A typical sample is an optically flat quartz disk overcoated with a film of the material of interest. These include Ag, Au, Pt, Nb, Ni, Al, C, Si, Ge, LiF, and a few engineering materials. Some materials for which the expected removal rate is high, such as carbon, will be solid disks rather than thin films.

Gregory, J. C.↗

NASA NTRS2006

Understanding Surface Processes on Mars Through Study of Iron Oxides/Oxyhydroxides: Clues to Surface Alteration and Aqueous Processes

We are performing oxidation and reduction reactions on hydrated ferric oxide minerals in order to investigate how these might alter under a variety of conditions on the surface of Mars. Preliminary experiments on ferrihydrite and goethite showed that heating these minerals in a dry oxidizing environment produces fine-grained hematite, while heating these minerals in a reducing environment produces fine-grained magnetite. Under Mars-like oxidation levels this magnetite then oxidizes to maghemite. These reactions are dependent on the presence of water and organic material that can act as a reductant. We are using reflectance and Mossbauer spectroscopy to characterize the reaction products and TEM to analyze the sample texture. Our preliminary results indicate that magnetite and maghemite could be formed in the soil on Mars from ferrihydrite and goethite if organics were present on early Mars.

Bishop, J. L.↗

NASA NTRS1971

The kinetics of reaction of the by-products of ablative materials at high temperatures and the rate of heat transfer between hot surfaces and reactive gases

Research has been conducted by means of laboratory experiments to enhance understanding of the fundamental mechanisms of heterogeneous and homogeneous chemical reactions taking place during ablative processes that accompany the reentry or manned space vehicles into planetary atmospheres. Fundamental mechanisms of those chemical reactions believed to be important in the thermal degradation of ablative plastic heat shield materials, and the gases evolved, are described.

Spokes, G. N.↗

NASA NTRS1992

Theoretical research program to study chemical reactions in AOTV bow shock tubes

Effort continued through this period to refine and expand the SIRIUS/ABACUS program package for CASSCF and RASSCF second derivatives. A new approach to computing the Gaussian integral derivatives that require much of the time in gradient and Hessian calculations was devised. Several different studies were undertaken in the area of application calculations. These include a study of proton transfer in the HF trimer, which provides an analog of rearrangement reactions, and the extension of our previous work on Be and Mg clusters to Ca clusters. In addition, a very accurate investigation of the lowest-lying potential curves of the O2 molecule was completed. These curves are essential for evaluating different models of the terrestrial atmosphere nightglow. The most effort this year was devoted to a large scale investigation of stationary points on the C4H4 surface, and the thermochemistry of acetylene/acetylene reaction.

Taylor, Peter↗