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A vacuum system developed to study stratospheric gases reacting on Al2O3. Special attention was given to the reactions of HCl, SO2, and O3. Efforts were made to detect atoms and/or molecules produced by catalytic action of Al2O3 with mass spectrometer.
Several NASA sponsored remote sensors and possible airborne platforms were evaluated. Outputs of dispersion models for SO2 and CO pollution in the Washington, D.C. area were used with ground station data to establish the expected performance and limitations of the remote sensors. Aircraft/sensor support requirements are discussed. A method of optimum flight plan determination was made. Cost trade offs were performed. Conclusions about the implementation of various instrument packages as parts of a comprehensive air quality monitoring system in Washington are presented.
Air-quality data for metropolitan Cleveland, Ohio, from 1967 through 1972 were collated and statistically analyzed. Total suspended particulates (TSP) departed from lognormal distribution in 1972. Nitrogen dioxide and sulfur dioxide, departed significantly from lognormal distributions in 1972. In Cleveland the Ohio standards were not met. However, the data indicate a general improvement in air quality. Unusually high precipitation (43% above the average in 1972) may be responsible in lowering these values from the 1971 levels. The mean values of TSP, NO2, and SO2 are 104, 191, and 83 microgram/cu m respectively.
Evidence is presented that microwave rotational spectroscopy can be developed for use in air pollution monitoring, with the employment of a diode-cavity spectrometer capable of detecting small concentrations of NO2, SO2, H2CO, and HN3 gas with very high specificity. The theory behind the technique is discussed, together with its application and experimental results.
The potential of molecular fluorescence was assessed as a stratospheric monitor of the concentrations of various minor species. Seventeen molecules were considered and all spectral regions from the vacuum ultraviolet through to the infrared are included. The exercise has produced few surprises; however, further confirmation has emerged as to the feasibility of this sensitive technique for monitoring stratospheric OH, NO2, and SO2, sufficient to warrant its development as analytical flight hardware for these species. All the other molecules have been eliminated with the exception of C10 which appears to have promise but requires additional information before its detection limit can be calculated; its fluorescence spectrum is as yet uninvestigated. A handbook for molecular fluorescence is presented, and a compilation of all reported studies for simple molecules using line source excitation is included.
Progress is reported on experimental investigations of Lidar and the application of Lidar to environmental and atmospheric science. Specifically the following programs are considered: calibration and application of the LaRC 48-inch Lidar; efficient and certain detection of SO2 and other gases in the calibration tank using the Raman Stack Monitor Lidar; the potential of Lidar remote sensing from the space shuttle; and the planning and mounting of efforts to realize the promise of backscatter differential absorption Lidar.
Raman backscatter techniques proved to be a useful remote sensing tool, whose full potential has not been realized. The types of information available from laser probes in atmospheric studies are reviewed. Detection levels for known Raman cross sections are calculated using the laser radar equation. Laboratory experiments performed for H2O, N2, SO2, O2 and HCL indicate that accurate wavelength cross sections need to be obtained, as well as more emphasis on obtaining accurate Raman cross sections of molecular species at wavelengths in the ultraviolet spectra.
The development of agents suitable for removal of CO, NH3, NO2 SO2, and other spacecraft contaminants was approached. An extensive technology review was conducted, yielding a large number of potentially useful materials and/or concepts. Because the two toxic gases of greatest interest, CO and NH3, suggested the use of catalysis principles emphasis was placed on the intestigation of transition metals on various supports. Forty-three materials were prepared or obtained and 25 were tested. Gas chromatographic techniques were used to find seven candidates that effectively managed various combinations of the four toxic gases: none managed all. These candidates included six transition metal-containing preparations and a supported LiOH material. Three commercial charcoals showed some efficiency for the toxic gases and may constitute candidates for enhancement by doping with transition metals.
The pre-resonance Raman spectra of SO2, N2O, and H2S were investigated using the 4880 A, 4727 A, and 4579 A lines of the argon ion laser. Although these molecules have electronic absorption bands in the near ultraviolet, none exhibit any pre-resonance enhancement within our experimental error of + or - 10%. Possible explanations taking into account the current theories for resonance Raman are discussed.
The thermodynamic properties of several water-soluble gases are reviewed to determine the likely effect of the atmospheric water cycle on their vertical profiles. It is found that gaseous HCl, HNO3, and HBr are sufficiently soluble in water to suggest that their vertical profiles in the troposphere have a similar shape to that of water vapor. It is predicted that HCl, HNO3, and HBr exhibit a steep negative gradient with altitude roughly equal to the altitude gradient of water vapor. Therefore, ground-based sources of inorganic chlorine, odd nitrogen, and inorganic bromine compounds are not likely to affect the stratosphere directly in the mean. Calculations also show that while SO2 and NH3 are significantly affected by the atmospheric water cycle, their abundances may not decrease with altitude as rapidly as does that of water vapor.
Conjugated polyenes, and polyesters containing phthalocyanine in their backbone, were synthesized. These polymers were characterized by chemical analysis, thermogravimetric analysis, spectral analysis, and X-ray diffraction studies for crystallinity, as well as for their film-forming capability and gas/polymer interactions. Most of the polymers were relatively insensitive to water vapor up to 50 percent relative humidity, but the polyester/phthalocyanine (iron) polymer was relatively insensitive up to 100 percent RH. On the other hand, poly(p-dimethylaminophenylacetylene) was too conductive at 100 percent RH. Of the gases tested, the only ones that gave any evidence of interacting with the polymers were SO2, NOx, HCN and NH3. Poly(imidazole)/thiophene responded to each of these gases at all relative humidities, while the other polymers gave varying response, depending upon the RH. Thus, since most of these gases were electron-accepting, the electron-donating character of poly(imidazole)/thiophene substantiates the concept of electronegativity being the operating principle for interaction effects. Of the six polymers prepared, poly(imidazole)/thiophene first showed a very good response to smoldering cotton, but it later became nonresponsive; presumably due to oxidation effects.
The feasibility of detecting eight trace constituents (CH4, HCl, HF, HNO3, NH3, NO, NO2 and SO2) against the rest of the atmospheric background at various altitudes from infrared emission and absorption atmospheric spectra was studied. Line-by-line calculations and observational data were used to establish features that can be observed in the atmospheric spectrum due to each trace constituent. Model calculations were made for experimental conditions which approximately represent state of the art emission and absorption spectrometers.
The UV spectra of the sun, as well as the differences and ratios of planetary and solar spectra, are presented. The results indicate that SO, SO2 and ClO2 may be present in Venus' atmosphere, and Formaldehyde CH2O and ClO2 on Jupiter. The solar UV measurements were analyzed to deduce ozone concentration in the earth's atmosphere.
Atmospheric infrared emission and absorption spectra obtained from aircraft and balloon-borne spectrometers are presented. From such spectra, mixing ratio vs altitude profiles are derived for several minor constituents. Recent results for HNO3, CF2Cl2, CFCl3, and HF are presented. In addition, the feasibility of infrared detection of other trace constituents, such as HCl, HF, NH3, NO and SO2, against the rest of the atmospheric background is studied. From this study, made on a line-by-line basis for 'state of the art' airborne spectrometers, potential spectral features for detection of the trace constituents are isolated.
Light detection and ranging (LIDAR) technology was applied to the assessment of air quality, and its usefulness was evaluated by actual field tests. Necessary hardware was successfully constructed and operated in the field. Measurements of necessary physical parameters, such as SO2 absorption coefficients were successfully completed and theoretical predictions of differential absorption performance were reported. Plume modeling improvements were proposed. A full scale field test of equipment, data analysis and auxiliary data support was conducted in Maryland during September 1976.
The absolute integrated intensity of the IR vibration-rotation nu-1 SO2 band was measured using the linear portion of the curve of growth. Infrared spectroscopic-absorption cell measurements were performed on sulfur dioxide at partial pressures less than 0.15 torr with nitrogen added to give a total pressure of 705 torr, the path length being 4 mm. The absolute integrated intensity was determined to be 112.0 plus or minus 2.6/cm/sq (atm cm) at 296 K at the 95% confidence level.
A chemical engineering analysis is made of fluidized-bed combustor (FBC) performance, with FBC models developed to aid estimation of combustion efficiency and axial temperature profiles. The FBC is intended for combustion of pulverized coal and a pressurized FBC version is intended for firing gas turbines by burning coal. Transport phenomena are analyzed at length: circulation, mixing models, drifting, bubble wake lift, heat transfer, division of the FB reactor into idealized mixing cells. Some disadvantages of a coal FBC are pointed out: erosion of immersed heat-transfer tubing, complex feed systems, carryover of unburned coal particles, high particulate emission in off-streams. The low-temperature bed (800-950 C) contains limestone, and flue-gas-entrained SO2 and NOx can be kept within acceptable limits.
Times to incapacitation and death and LC50 values were determined for male Swiss albino mice exposed to different concentrations of sulfur dioxide in a 4.2 liter hemispherical chamber. The LC50 for a 30 minute exposure was about 3000 ppm SO2.