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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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NASA NTRS1979

The photolysis of chlorine in the presence of ozone, nitric acid and nitrogen dioxide

The following three systems were investigated: the Cl2-O3 system, the Cl2-O2-NO system and the Cl2-NO2-M system. In the first system, the reaction between ClO and O3, the reaction between OClO and O3, and the mechanism of the Cl2-O3 system were studied. In the second system, the reaction between ClOO and NO was investigated. In the last system, the reaction between Cl and NO2 was investigated as well as the kinetics of the chemiluminescence of the Cl-NO2-O3 reaction. In the first system, Cl2 was photolyzed at 366 nm in the presence of O3 within the temperature range 254-297 K. O3 was removed with quantum yields of 5.8 + or - 0.5, 4.0 + or - 0.3, 2.9 + or - 0.3 and 1.9 + or - 0.2 at 297, 283, 273, and 252 K respectively, invariant to changes in the initial O3 or Cl2 concentration, the extent of conversion or the absorbed intensity, I sub a. The addition of nitrogen had no effect on -phi(03). The Cl2 removal quantum yields were 0.11 + or - 0.02 at 297 K for Cl2 conversions of about 30%, much higher than expected from mass balance considerations based on the initial quantum yield of 0.089 + or - 0.013 for OClO formation at 297 K. The final chlorine-containing product was Cl2O7. It was produced at least in part through the formation of OClO as an intermediate which was also observed with an initial quantum yield of phi sub i(OClO) = 2500 exp(-(3025 + or - 625)/T) independent of (O3) or I sub a.

Stuper, W. W.↗
NASA NTRS1986

On the atmospheric photochemistry of nitric acid

Measurements of the temporal and spatial variations in HNO3, particularly those from the Nimbus 7 limb IR monitor of the stratosphere (LIMS) satellite experiment, are compared to both a two-dimensional chemical/dynamical model and to chemistry/parcel trajectory analyses. Significant discrepancies are found between the observed and modeled variations in the winter season, especially in the polar night region. The study of the evolution of HNO3 suggests that an important source exists for this species in the high-latitude winter stratosphere that is not included in presently accepted photochemical schemes. Possible reactions to account for this discrepancy are explored.

Austin, J.↗
NASA NTRS1986

Pressure and temperature dependences of the reaction of OH with nitric acid

Rate constants for the reaction of OH with HNO3 have been measured by using a laser flash photolysis resonance absorption technique at 298 and 248 K in the presence of 10-730 Torr of He, N2, and SF6. A dependence on total pressure was observed with rate constant values increasing at 298 K from 1.11 x 10 to the -13th cu cm/molecule/s at 10 Torr to 1.45 x 10 to the -13th cu cm/molecule/s at 730 Torr, and at 248 K from 1.87 x 10 to the -13th cu cm/molecule/s at 10 Torr to 3.07 x 10 to the -13th cu cm/molecule/s at 730 Torr with helium as the diluent gas. Falloff behavior occurred at lower pressures with SF6 or N2 as the diluent gas. Extrapolated zero pressure rate constants were determined and correspond to an Arrhenius activation energy of E/R = -710 K.

Stachnik, R. A.↗
NASA NTRS1987

Nitric acid forecast experiments

Results of two three-dimensional forecasts of the time evolution of the distribution of HNO3 in the stratosphere are reported. The first is for the February 1979 stratospheric warming, and the second is for a period in March, 1979 when the relative importance of photochemistry and dynamics is thought to be rapidly changing. The zonal mean results of the model calculations are in general qualitative agreement with the LIMS HNO3 observations. However, the calculated three-dimensional fields show significant differences from the observations. The results provide insight into what must be done to form a successful constituent forecast model and provide information on the modeling technique and the self-consistency of the observed dynamical and constituent fields.

Rood, Richard B.↗
NASA NTRS1988

Heterogeneous interactions of chlorine nitrate, hydrogen chloride, and nitric acid with sulfuric acid surfaces at stratospheric temperatures

The heterogeneous interactions of ClONO2, HCl, and HNO3 with sulfuric acid surfaces were studied using a Knudsen cell flow reactor. The surfaces studied, chosen to simulate global stratospheric particulate, were composed of 65-75 percent H2SO4 solutions at temperatures in the range -63 to -43 C. Heterogeneous loss, but not reaction, of HNO3 and HCl occurred on these surfaces; the measured sticking coefficients are reported. Chlorine nitrate reacted on the cold sulfuric acid surfaces, producing gas-phase HOCl and condensed HNO3. CLONO2 also reacted with HCl dissolved in the 65-percent H2SO4 solution at -63 C, forming gaseous Cl2. In all cases studied, the sticking and/or reaction coefficients were much larger for the 65-percent H2SO4 solution at -63 C than for the 75-percent solution at -43 C.

Tolbert, Margaret A.↗
NASA NTRS1988

Laboratory studies of the nitric acid trihydrate - Implications for the south polar stratosphere

Vapor pressures of HNO3 and H2O have been measured over the trihydrate crystal, formed by vapor deposit on a glass surface. In the temperature range 190 to 205 K the two phase-equilibrium trihydrate/vapor was studied by adding and removing H2O. Coexistence equilibria vapor pressures of trihydrate/solid solutions of HNO3 in ice and of mono-/trihydrate were also measured. Results show that for typical mixing ratios of H2O and HNO3 found in the lower stratosphere (3 ppm H2O, 5 ppb HNO3) the trihydrate would start to form at temperatures about 7 K higher than the ice point. The pressure of atmospheric HNO3 would rapidly decrease as the atmosphere cools without large changes in partial pressures of H2O. These laboratory results provide information on the formation of polar stratospheric clouds containing H2O and HNO3.

Hanson, David↗
NASA NTRS1988

The rotational spectrum of nitric acid - The first five vibrational states

The details of work on the nu(8) vibrational state, which arise from the NO2 out-of-plane vibration, are reported. For this state, over 210 transitions have been measured in the millimeter and submillimeter spectral region and analyzed with Watson's A-reduced centrifugal distortion Hamiltonian. Also included in this work is a comparison of all these spectra and an overview of the millimeter and submillimeter spectra associated with these states. Although at the high sensitivity available in laboratory experiments, many additional lines are observable, all arise from vibrational states whose populations are more than 100 times lower than the ground state. The most prominent of these are due to the states which give rise to the perturbed 2 nu(9) and nu(5) bands near 11 microns. These results provide a significant data base for both atmospheric remote sensing experiments and spectral analyses of data in other spectral regions, especially the IR.

Crownover, Richard L.↗
NASA NTRS1990

Operational overview of NASA GTE/CITE 2 airborne instrument intercomparisons - Nitrogen dioxide, nitric acid, and peroxyacetyl nitrate

This paper provides the rationale, objectives, approach, and a brief description of the instrumentation included in the second airborne Chemical Instrumentation Test and Evaluation (CITE 2) mission conducted on NASA's Electra aircraft. CITE 2 intercompared data from instruments measuring NO2, HNO3, and PAN in the troposphere. This study, conducted in August 1986, encountered marine and continental air with free tropospheric mixing ratios of NO2, HNO3, and PAN typically less than 120, 150, and 200 parts per trillion by volume, respectively.

Hoell, James M., Jr.↗
NASA NTRS1990

An intercomparison of airborne nitric acid measurements

Results are reported on the performance of (1) denuder-tube/chemiluminescent, (2) nylon-filter/ion-chromatography, and (3) tunable-diode-laser/multipath-absorption HNO3 measurement instruments during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 (CITE 2) program in summer 1986. The instrument designs, test protocols, and CITE 2 flights are described, and the results are presented in extensive graphs and discussed in detail. The data obtained with the three instruments are shown to be in very poor agreement at mixing ratios below 150 parts per trillion by volume (pptv), with significant discrepancies even at higher levels. Instrument (3) gave systematically higher values than (1) and (2). It is concluded that none of the instruments is accurate enough for reliable use at normal atmospheric HNO3 levels (around 100 pptv).

Gregory, G. L.↗
NASA NTRS1990

Measurements of tropospheric nitric acid over the western United States and northeastern Pacific Ocean

HNO3 measurements obtained in the free troposphere (FT) and boundary layer (BL) over the western U.S. and the NE Pacific during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 (CITE 2) program in summer 1986 are reported. The CITE 2 HNO3 instruments and flight protocols are described, and the results are presented in tables and graphs. Over the ocean, the average HNO3 mixing ratios were found to be 108 parts per trillion by volume (pptv) in the FT and 62 pptv in the BL, suggesting removal of HNO3 from the BL by dry deposition. The corresponding values over land were 61 pptv for the FT and 767 pptv for the BL, and the horizontal distribution of BL HNO3 indicated an anthropogenic origin.

Lebel, P. J.↗
NASA NTRS1991

HCl dissolved in solid mixtures of nitric acid and ice - Implications for the polar stratosphere

The solubility of HCl in polar stratospheric cloud (PSC) particles plays an important role in the heterogeneous chemistry of the lower polar stratosphere. New laboratory studies are reported showing a strong dependence of the HCl solubility on the HNO3 content in ice particles. At 200 K and a partial HCl pressure of 10 exp -6 torr, the HCl content in NAT is 0.35 mol pct, decreasing about a factor of 3 for every ten-fold decrease in the substrate's HNO3 content. At an HCl pressure of 10 exp -7 torr, the content is about 40 percent of that at 10 exp -6 torr. HCL dissolved in pure water ice at these partial pressures is less than 0.002 mol pct. The surface coverage of HCl on small ice samples was estimated to be about 0.1 monolayer at 10 exp -6 torr exposure.

Marti, James↗
NASA NTRS1991

Ammonia and nitric acid emissions from wetlands and boreal forest fires

Tests conducted during three (one boreal and two wetland) ecosystem fires have established the NH3- and HNO3-determination effectiveness of the 'tungsten oxide denuder' technique, using a low-flying helicopter to fly through biomass-burn smoke plumes. Both species were found to be present in the smoke plumes at levels much higher than background. Despite the differences between boreal and wetland ecosystems, HNO3 emissions were comparable; NH3 emissions, by contrast, were 5-8 times greater in the boreal fire than in the wetland fires. Biomass burning is found to make a significant role in the tropospheric ammonia budget.

Lebel, Peter J.↗