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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
NASA NTRS1988

Antarctic ozone - Meteoric control of HNO3

Atmospheric circulation leads to an accumulation of debris from meteors in the Antarctic stratosphere at the beginning of austral spring. The major component of meteoric material is alkaline, comprised predominantly of the oxides of magnesium and iron. These metals may neutralize the natural acidity of stratospheric aerosols, remove nitric acid from the gas phase, and bond it as metal nitrates in the aerosol phase. Removal of nitric acid vapor has been previously shown to be a critical link in the photochemical depletion of ozone in the Antarctic spring, by allowing for increased catalytic loss from chlorine and bromine.

Prather, Michael J.↗
NASA NTRS1995

Phase equilibria of H2SO4, HNO3, and HCl hydrates and the composition of polar stratospheric clouds

Thermodynamic properties and phase equilibria behavior for the hydrates and coexisting pairs of hydrates of common acids which exist in the stratosphere are assembled from new laboratory measurements and standard literature data. The analysis focuses upon solid-vapor and solid-solid-vapor equilibria at temperatures around 200 K and includes new calorimetric and vapor pressure data. Calculated partial pressures versus 1/T slopes for the hydrates and coexisting hydrates agree well with experimental data where available.

Wooldridge, Paul J.↗
NASA NTRS1995

Phase Equilibria of H2SO4, HNO3, and HCl Hydrates and the Composition of Polar Stratospheric Clouds

Thermodynamic properties and phase equilibria behavior for the hydrates and coexisting pairs of hydrates of common acids which exist in the stratosphere are assembled from new laboratory measurements and standard literature data. The analysis focuses upon solid-vapor and solid-solid-vapor equilibria at temperatures around 200 K and includes new calorimetric and vapor pressure data. Calculated partial pressures versus 1/T slopes for the hydrates and coexisting hydrates agree well with experimental data where available.

Wooldridge, Paul J.↗
NASA NTRS2004

Trajectory Studies of Large HNO3-Containing PSC Particles in the Arctic: Evidence for the Role of NAT

Large (5 to >20 micron diameter) nitric-acid-containing polar stratospheric cloud (PSC) particles were observed in the Arctic stratosphere during the winter of 1999-2000. We use a particle growth and sedimentation model to investigate the environment in which these particles grew and the likely phase of the largest particles. Particle trajectory calculations show that, while simulated nitric acid dihydrate (NAD) particle sizes are significantly smaller than the observed maximum particle sizes, nitric acid trihydrate (NAT) particle trajectories are consistent with the largest observed particle sizes.

McKinney, K. A.↗
NASA NTRS2004

Nitric Acid Uptake on Subtropical Cirrus Cloud Particles

The redistribution of HNO3 via uptake and sedimentation by cirrus cloud particles is considered an important term in the upper tropospheric budget of reactive nitrogen. Numerous cirrus cloud encounters by the NASA WB-57F high-altitude research aircraft during CRYSTAL-FACE were accompanied by the observation of condensed-phase HNO3 with the NOAA chemical ionization mass spectrometer. The instrument measures HNO3 with two independent channels of detection connected to separate forward- and downward-facing inlets that allow a determination of the amount of HNO3 condensed on ice particles. Subtropical cirrus clouds, as indicated by the presence of ice particles, were observed coincident with condensed-phase HNO3 at temperatures of 197 K - 224 K and pressures of 122 hPa - 224 hPa. Maximum levels of condensed-phase HNO3 approached the gas-phase equivalent of 0.8 ppbv. Ice particle surface coverages as high as 1.4- 10(exp 14) molecules/sq cm were observed. A dissociative Langmuir adsorption model, when using an empirically derived HNO3 adsorption enthalpy of -11.0 kcal/mol, effectively describes the observed molecular coverages to within a factor of 5. The percentage of total HNO3 in the condensed phase ranged from near zero to 100% in the observed cirrus clouds. With volume-weighted mean particle diameters up to 700 pm and particle fall velocities up to 10 m/s, some observed clouds have significant potential to redistribute HNO3 in the upper troposphere.

Source record↗
NASA NTRS2004

Nitric Acid Uptake on Subtropical Cirrus Cloud Particles

The redistribution of HNO3 via uptake and sedimentation by cirrus cloud particles is considered an important term in the upper tropospheric budget of reactive nitrogen. Numerous cirrus cloud encounters by the NASA WB-57F high-altitude research aircraft during the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) were accompanied by the observation of condensed-phase HNO3 with the NOAA chemical ionization mass spectrometer. The instrument measures HNO3 with two independent channels of detection connected to separate forward and downward facing inlets that allow a determination of the amount of HNO3 condensed on ice particles. Subtropical cirrus clouds, as indicated by the presence of ice particles, were observed coincident with condensed-phase HNO3 at temperatures of 197-224 K and pressures of 122-224 hPa. Maximum levels of condensed-phase HNO3 approached the gas-phase equivalent of 0.8 ppbv. Ice particle surface coverages as high as 1.4 # 10(exp 14) molecules/ square cm were observed. A dissociative Langmuir adsorption model, when using an empirically derived HNO3 adsorption enthalpy of -11.0 kcal/mol, effectively describes the observed molecular coverages to within a factor of 5. The percentage of total HNO3 in the condensed phase ranged from near zero to 100% in the observed cirrus clouds. With volume-weighted mean particle diameters up to 700 ?m and particle fall velocities up to 10 m/s, some observed clouds have significant potential to redistribute HNO3 in the upper troposphere.

Popp, P. J.↗
NASA NTRS1990

Measurements of tropospheric nitric acid over the Western United States and Northeastern Pacific Ocean

Over 240 measurements of nitric acid (HNO3) were made in the free troposphere as well as in the boundary layer. Marine HNO3 measurement results were strikingly similar to results from GAMETAG and other past atmospheric field experiments. The marine boundary layer HNO3 average, 62 parts-per-trillion by volume (pptv), was 1/3 lower than the marine free tropospheric average, 108 pptv, suggesting that the boundary layer is a sink for tropospheric nitric acid, probably by dry deposition. Nitric acid measurements on a nighttime continental flight gave a free tropospheric average of 218 pptv, substantially greater than the daytime continental free tropospheric 5-flight average of 61 pptv. However, the nighttime results may be influenced by highly convective conditions that existed from thunderstorms in the vicinity during that night flight. The continental boundary layer HNO3 average of 767 pptv is an order of magnitude greater than the free tropospheric average, indicating that the boundary layer is a source of free tropospheric HNO3. The distribution of continental boundary layer HNO3 data, from averages of 123 over rural Nevada and Utah to 1057 pptv in the polluted San Joaquin Valley of California suggest a close tie between boundary layer HNO3 and anthropogenic activity.

Lebel, P. J.↗
DOE OSTI2025

Generation and Study of Am(IV) by Temperature-Controlled Electron Pulse Radiolysis

Used nuclear fuel (UNF) separation techniques that strive to separate radiotoxic americium (Am) from trivalent lanthanide fission products through oxidation state control have increased research efforts surrounding Am(V) and Am(VI). However, equivalent knowledge of the tetravalent state, Am(IV), has remained elusive, particularly in conditions more representative of UNF reprocessing, i.e., in concentrated nitric acid (HNO3). With this in mind, we have used electron pulse radiolysis to study the radiation-induced redox reaction of Am(III) with the oxidizing nitrate radical (NO3?) in 6 M HNO3: Am(III) + NO3? ? Am(IV) + NO3? . These experiments enabled us to observe the growth and decay of Am(IV) in a concentrated acidic solution for the first time. The transient Am(IV) species was found to have a lifetime of ~16 µs?sufficiently long-lived to play a critical mechanistic role in UNF reprocessing systems. Additionally, we performed the first-ever temperature-dependent kinetics study of an actinide element, elucidating unprecedented Arrhenius and Eyring activation parameters for the reaction of Am(III) with NO3?. This new knowledge provides much-needed molecular-level insights into the radiation-induced behavior of Am.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
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

Laboratory studies of HNO3/H2O mixtures at low temperatures

The possibility of stratospheric HN3 condensing out of the gas-phase at low temperatures has become important in the chemical explanations of the rapid loss of Antarctic ozone in spring. Consequently, knowledge about the behavior of the vapor pressures of water and HNO3 over HNO3/water mixtures at stratospheric temperatures is needed to determine if HNO3 could condense, and by how much the HNO3 vapor pressure could be depressed. Laboratory investigations of vapor pressures above HNO3/water mixtures are described. Vapor pressures were initially measured over liquid and frozen bulk mixtures contained in a glass still which was attached to a stainless steel vacuum chamber. The total pressure in the chamber was monitored with a precision pressure sensor, and the vapor pressures of HNO3, water and impurities were analyzed with a mass spectrometer beam system. In a second set of experiments, vapor deposits were made to produce ice and the mono- and trihydrate of HNO3. Further data and conclusions are presented.

Hanson, David↗
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

Heterogeneous reactions of chlorine nitrate and hydrogen chloride on type I polar stratospheric clouds

A fast-flow reactor coupled with a quadrupole mass spectrometer was used to study the heterogeneous reactions ClONO2 + HCl yields Cl2 + HNO3 (1) and ClONO2 + H2O yields HOCl + HNO3 (2) on vapor-deposited HNO3-H2O ice substrates. It was found that the sticking coefficient of HCl on these substrates was a strong function of the substrate composition, ranging from about 2 x 10 exp -5 at nitric acid trihydrate composition to 6 x 10 exp -3 at 45 wt pct HNO3. The HNO3-H2O ice substrates were found to have large internal surface areas, and corrections for gas-phase diffusion within the porous ices were applied to observed loss rates.

Leu, Ming-Taun↗