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NASA NTRS1979

Isothermal-desorption-rate measurements in the vicinity of the Curie temperature for H2 chemisorbed on nickel films

Measurements of the isothermal desorption rate of H2 chemisorbed onto polycrystalline nickel films made for temperatures spanning the Curie temperature of the nickel film are presented. Desorption kinetics were followed by measuring the decay of the change in resistance of the nickel film brought about by hydrogen chemisorption after gas-phase H2 had been rapidly evacuated. The desorption rate is found to undergo an anomalous decrease in the vicinity of the Curie temperature, accompanied by an increase in the desorption activation energy and the equilibrium constant for the chemisorbed hydrogen. The results are interpreted in terms of anomalous variations in rate constants for the formation of the precursor molecular adsorbed state and the chemisorbed atomic state due to the phase transition in the nickel. The changes in rate constants are also considered to be in qualitative agreement with theoretical predictions based on a spin coupling between the adatom and the magnetic substrate.

Shanabarger, M. R.↗

NASA NTRS1979

New observations of interstellar abundances and depletions of boron, vanadium, chromium, and cobalt

New observations of interstellar lines of boron, vanadium, chromium, and cobalt in the spectra of Zeta Oph and Xi Per have been obtained with the Copernicus satellite. Chromium has been detected for the first time toward a reddened star, and cobalt has been seen for the first time in any interstellar line of sight. New limits have been obtained for boron and vanadium. These new data, along with limits on scandium and other species from the literature, have been compared with models for the depletion process. No fully conclusive test of depletion models is yet possible, but the new data on boron appear to favor the hypothesis that the depletions are dominated by accretion of gas-phase particles onto grains, rather than being due to grain condensation under pressure equilibrium. The impact of these new data on the study of grain surface properties is described.

Snow, T. P., Jr.↗

NASA NTRS1979

The determination of electron abundances in interstellar clouds

An independent method is proposed for the determination of electron abundances in dense clouds based upon the abundance ratio of HCO(+) and CO. The method is derived from a simple application of gas phase ion molecule interstellar chemistry. It is noted that unlike the fractionation of deuterated molecules, it applies to warm as well as to cool clouds. The method is illustrated with the results of the recent abundance survey of Wooten et al. (1978). Finally, it is shown that in cases where deuterium enhancement is measured, an upper limit can be obtained for the cosmic ray ionization rate.

Wootten, A.↗

NASA NTRS1979

Formation and deposition of volcanic sulfate aerosols on Mars

The paper considers the formation and deposition of volcanic sulfate aerosols on Mars. The rate limiting step in sulfate aerosol formation on Mars is the gas phase oxidation of SO2 by chemical reactions with O, OH, and HO2; submicron aerosol particles would circuit Mars and then be removed from the atmosphere by gravitational forces, globally dispersed, and deposited over a range of equatorial and mid-latitudes. Volcanic sulfate aerosols on Mars consist of liquid droplets and slurries containing sulfuric acid; aerosol deposition on a global or hemispheric scale could account for the similar concentrations of sulfur within surficial soils at the two Viking lander sites.

Settle, M.↗

NASA NTRS1979

Iron and the formation of astrophysical dust grains

Condensation of metallic iron or the iron carbide cohenite Fe3C is proposed as the source of the approximately 1000 K dust condensate in nova shells, Wolf-Rayet stars, and other objects. Iron grains may serve as nucleation sites for carbon in carbon-star ejecta; however, nucleation of graphite at its equilibrium saturation temperature is almost certainly kinetically inhibited. A gas phase rich in CO, C2H2, and HCN is produced instead.

Lewis, J. S.↗

NASA NTRS1980

Oxidation state of the atmosphere and crust of Venus from Pioneer Venus results

Recent spacecraft observations of Venus permit a detailed model of sulfur chemistry in the atmosphere-lithosphere system. Pioneer Venus experiments confirm that, as predicted, COS and H2S are dominant over SO2 in the lower atmosphere, and that the equilibrium concentrations of S2 and S3 are significant. Many criteria serve to bracket the oxidation state of the crust: it is nearly certain that the S2(2-)/SO4(2-) buffer regulates the oxygen fugacity, and that FeO is at least as abundant as F2O3 in crustal silicates. A highly oxidized crust (as, for example, would result from O2 absorption complementary to escape of vast amounts of H2) is incompatible with the gas-phase sulfur chemistry. If the Pioneer Venus mass spectrometer estimates of the abundance of sulfur gases are correct, earth-like models for the bulk composition of Venus are seriously in error, and a far lower FeO content is required for Venus.

Lewis, J. S.↗

NASA NTRS1980

Analysis of solid propellant combustion in a closed vessel including secondary reaction

A theory for combustion of solid propellants in a closed vessel is presented allowing for residual exothermic chemical reaction in the bulk of the gas in the vessel. Particular attention is given to propellants exhibiting thick gaseous flame zones such as nitrocellulose, double-base and nitramine propellants. For these, the reaction at high pressures is assumed to involve mainly the oxidation of residual hydrocarbons by NO. It is shown that the direct dynamic coupling between the exothermicity, the molecular weight reduction and the changing pressure can influence the dp/dt-p traces obtained, in a manner not directly related to mass burning rate of the solid. Energy and species conservation equations are derived for the bulk of the vessel in differential form; the system is solved numerically. The results show the effect of extended chemical reaction upon measurable combustion characteristics such as dp/dt-p and burn rate pressure exponent, demonstrating its potential importance in interpretation of closed vessel firing data, depending on the pace of the residual gas phase reactions.

Benreuven, M.↗

NASA NTRS1980

Effect of propellant deformation on ignition and combustion processes in solid propellant cracks

A comprehensive theoretical model was formulated to study the development of convective burning in a solid propellant crack which continually deforms due to burning and pressure loading. In the theoretical model, the effect of interrelated structural deformation and combustion processes was taken into account by considering (1) transient, one dimensional mass, momentum, and energy conservation equations in the gas phase; (2) a transient, one dimensional heat conduction equation in the solid phase; and (3) quasi-static deformation of the two dimensional, linear viscoelastic propellant crack caused by pressure loading. Partial closures may generate substantial local pressure peaks along the crack, implying a strong coupling between chamber pressurization, crack combustion, and propellant deformation, especially when the cracks are narrow and the chamber pressurization rates high. The maximum pressure in the crack cavity is generally higher than that in the chamber. The initial flame-spreading process is not affected by propellant deformation.

Kumar, M.↗

NASA NTRS1979

Design and fabrication of a four-man capacity urine wick evaporator system

The integrated system was tested to determine the performance characteristics and limitations of the dual catalyst concept. The primary objective of the dual catalyst concept is to remove ammonia and other noxious substances in the gas phase and thereby eliminate the need for and current practice of chemically or electrochemically pretreating urine prior to distillation.

Source record↗

NASA NTRS1980

Precision of NO2 photolysis rate measurements

Gas-phase kinetic calculations indicate that actinometric measurements of the rate of solar photolysis of NO2 in nitrogen can be in error by +5 to -15% or more, unless odd oxygen N2O5 chemistry, and trace oxygen content are considered. A field experiment confirms that the effect of the quartz tube on the measured photolysis rate is less than 1.7%.

Dickerson, R. R.↗

NASA NTRS1980

A matrix-isolation-infrared spectroscopic study of the reactions of nitric oxide with oxygen and ozone

An investigation of the oxidation of NO to NO2 by trapping the products of the gas-phase reactions with excess oxygen and ozone identified the transient species by their infrared spectra. The primary products of the NO + NO2 reactions were NO2, N2O3(A), N2O3(B), N2O4, and peroxy nitrate (OONO). The primary products of the NO + O3 reactions were NO2 and peroxy NO3 with the higher nitric oxides in low concentrations compared with the NO + O2 reactions. Isotopic oxygen and ozone were used to identify the infrared absorption frequency of the peroxy nitrate.

Bhatia, S. C.↗

NASA NTRS1980

Evaluated kinetic and photochemical data for atmospheric chemistry

This paper contains a critical evaluation of the kinetics and photochemistry of gas phase chemical reactions of neutral species involved in middle atmosphere chemistry (10-55 km altitude). Data sheets have been prepared for 148 thermal and photochemical reactions, containing summaries of the available experimental data with notes giving details of the experimental procedures. For each reaction a preferred value of the rate coefficient at 298 K is given together with a temperature dependency where possible. The selection of the preferred value is discussed, and estimates of the accuracies of the rate coefficients and temperature coefficients have been made for each reaction. The data sheets are intended to provide the basic physical chemical data needed as input for calculations which model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available data on enthalpies of formation of the reactant and product species.

Baulch, D. L.↗

NASA NTRS1980

Abundance determinations for interstellar gas

The results of general abundance studies, using the Copernicus satellite are reviewed. The general pattern of depletion of some elements such as Si, Al, Mn, Fe, and Mg, near the sun is described. Techniques for obtaining abundances for various species are discussed, as are the aspects of the analysis which are uncertain. Variations in gas phase abundance from region to region are found for Fe and Si, similar to variations now known to exist for Ca and Ti based on visible spectra. A new generation of space instruments, with higher efficiency and resolution, in particular for 920-1400 A, can provide detailed interstellar line profiles.

York, D. G.↗

NASA NTRS1980

Interstellar sulfur chemistry

The results of a chemical model of SO, CS, and OCS chemistry in dense clouds are summarized. The results are obtained from a theoretical study of sulfur chemistry in dense interstellar clouds using a large-scale time-dependent model of gas-phase chemistry. Among the results are the following: (1) owing to activation energy, the reaction of CS with O atoms is efficient as a loss mechanism of CS during the early phases of cloud evolution or in hot and oxygen-rich sources such as the KL nebula; (2) if sulfur is not abnormally depleted in dense clouds, then the observed abundances of SO, SO2, H2S, CS, OCS, H2CS, and SiS indicate that sulfur is mostly atomic in dense clouds; and (3) OCS is stable against reactions with neutral atoms and radicals in dense clouds.

Prasad, S. S.↗

NASA NTRS1981

Recent observations of HF and HCl in the upper stratosphere

Concentrations of gas phase hydrofluoric acid and hydrochloric acid have been determined in the upper stratosphere from near-infrared solar spectra recorded in the course of balloon flights from Palestine, Texas, in October 1978 and in September 1979. The average mixing ratios for HF deduced respectively from these flights are (4.8 plus or minus .3) x 10 to the -10th ppv above 30.3km and (6.2 plus or minus .5) x 10 to the -10th ppv above 36.8km. This observed difference is ascribed to an increase in the HF concentration out to at least 37km. The HCl mixing ratios deduced from the 1978 flight yield (4.5 plus or minus .6) x 10 to the -10th ppv at 21.7km, (7.5 plus or minus .7) x 10 to the -10th ppv at 27.5 km and (2.1 plus or minus .4) x 10 to the -9th ppv above 30.5km. Observations in 1979 imply an average HCl mixing ratio above 36.8km of (2.4 plus or minus .4) x 10 to the -9th ppv. Our data do not indicate a measurable temporal trend of the HCl concentration above 30km.

Zander, R.↗

NASA NTRS1981

Matrix spectroscopic studies of chlorine atom-ozone reaction products

A spectroscopic study is presented of the matrix-isolated products of the direct combination reaction of chlorine atoms with ozone and of the microwave discharge reaction of chlorine and oxygen. Infrared spectra in the wavenumber range 2000 to 200 per cm were recorded for reaction products trapped by the condensation of a matrix of solid argon. Evidence for the formation of the ClO radical as well as the ClOO and ClClO radicals during the direct chlorine-ozone reaction is obtained, however no evidence is found for the presence of asymmetric ClO3 under conditions thought favorable for its formation. The ClO molecule is also observed following the microwave discharge reaction of chlorine and oxygen in argon in the isotopic forms (Cl-35)(O-16), (Cl-37)(O-16), (Cl-35)(O-18), and (Cl-37)(O-18). It is noted that the vibrational frequency for the (Cl-35)(O-16) radical at 849.2 per cm is blue-shifted 5 per cm above its gas-phase fundamental.

Carter, R. O., III↗

NASA NTRS1981

Vibrational disequilibrium in low pressure clouds

Steady state vibrational populations of SiO and CO in several dilute blackbody radiation fields have been calculated as a function of total pressure, kinetic temperature, and chemical composition of the gas. An approximate calculation for polyatomic molecules has also been carried out. Vibrational disequilibrium becomes increasingly significant as the total pressure and radiation density decrease. Many regions of postulated grain formation are found to be far out of thermal equilibrium before the onset of condensation. The use of classical nucleation theory and equilibrium thermodynamics to predict the onset of condensation and the composition of the solids or the molecular composition of the gas phase in such regions therefore is very questionable and needs to be examined for each case.

Nuth, J. A.↗

NASA NTRS1981

The optical and ultraviolet spectrum of the planetary nebula NGC 2440

New measurements of the optical and ultraviolet emission-line intensities of the high-excitation planetary nebula NGC 2440 in the wavelength range 1240-8578 A are analyzed with the aid of photoionization models. The observed O III and N II forbidden-line temperatures (13,800 K and 10,000 K, respectively) differ by more than the models predict. Inclusion of charge-transfer reactions at published rates improves agreement between calculated and observed abundances of many ions, but worsens the agreement for several highly ionized ions. Nitrogen shows a larger overabundance N(N)/N(O) approximately equal to 1.0, whereas ultraviolet lines give a carbon abundance close to the solar value. The refractory elements magnesium, calcium, and iron have similar gas-phase depletions of approximately 1.5 dex. The abundances of oxygen, neon, sodium, sulfur, chlorine, potassium, and argon are rougly solar.

Shields, G. A.↗