The Atmospheric Chemistry Experiment (ACE) is a satellite mission for remote sensing of the Earth's atmosphere using the solar occultation technique. The primary instrument on this satellite is the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). ACE-FTS retrievals are described with a focus on the creation of <em>a priori</em> temperature and pressure profiles. ACE-FTS measurements are then used to investigate the chemistry, transport and trends of chlorine, fluorine and water in the stratosphere, leading to an improved understanding of processes affecting both stratospheric ozone depletion and global climate change. <br /><br /> Total chlorine (Cl_TOT) in the stratosphere is determined using ACE-FTS measurements of eleven chlorine-containing species, supplemented by both other measurements and models, to determine Cl_TOT as a function of altitude in five latitude zones. All resulting Cl_TOT profiles are nearly linear, with a slight slope. Mean Cl_TOT for 2004 is determined to be 3. 65 ppbv for both the northern and southern midlatitudes (with a precision and estimated accuracy of ±0. 09 and ±0. 13 ppbv, respectively). A slightly lower value of mean Cl_TOT is determined for the tropics and slightly higher values at high latitudes. Total fluorine (F_TOT) in the stratosphere is also determined primarily from ACE-FTS measurements using a similar approach, resulting in stratospheric F_TOT profiles which are nearly linear with mean values ranging from 2. 50 to 2. 59 ppbv for each latitude zone (with a precision of 0. 04-0. 07 ppbv and an estimated accuracy of 0. 15 ppbv). The observed slopes and pattern of latitudinal variation are evidence of the beginning of a decline in global stratospheric chlorine and of the continuing increase in global stratospheric fluorine levels. <br /><br /> The abundance of water in the stratosphere is investigated for the northern hemisphere midlatitudes in 2004 using ACE-FTS measurements. Potential water is determined as [H₂O]+2[CH₄] and from [H₂O] versus [CH₄] correlations, resulting in a value of 7. 14±0. 05 ppmv, which is used to determine a value of 3. 65±0. 15 ppmv for the mean abundance of water entering the stratosphere. Both values are compared directly with historical data from the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument (1985-1994) and show a negligible change, implying that the increases observed by ATMOS and other long-term measurements from that time period have not continued. <br /><br /> The removal of stratospheric water in the Arctic vortex is investigated using ACE-FTS measurements. Using derived quantities from a meteorological data assimilation, northern hemisphere occultations from early 2004 are classified as vortex, vortex edge or extravortex. [CH₄] versus [N₂O] correlations are used to further classify the extravortex occultations as tropical, subtropical or midlatitude. Comparisons between profiles of [N₂O], [CH₄] and [H₂O] inside and outside the Arctic vortex, give estimates of upper stratospheric and lower mesospheric descent rates, indicating that descent in the winter 2004 Arctic vortex was rapid, with evidence of descent at higher altitudes than in past years. <br /><br /> The dehydration of air in the tropical tropopause layer and mechanisms for the entry of water vapor into the stratosphere are investigated by an analysis of ACE-FTS profiles of temperature, water vapor and [HDO]/[H₂O]. Month-to-month comparisons for 2004 and 2005 reveal a clear pattern of seasonal variation and a correlation between minimum temperature and maximum HDO depletion. Further interpretation indicates that the gradual dehydration mechanism accompanied by lofting of ice particles in the tropical troposphere is the most likely explanation for the observed seasonal variation and the shape of the [HDO]/[H₂O] profiles.

A groundbased instrument to measure the Atmospheric airglow of the molecular oxygen infrared atmospheric band emission was designed, built, tested and operated. The two channel photometer constructed was based on the original design by Evans (1967) that had been used in balloon experiments. The two channel photometer system specifications are presented. The major difference between the presented design and the earlier two channel photometers is the detector. An Indium Gallium Arsenide (InGaAs) photodiode provided better signal to noise in the conversion of the infrared light signal to an electronic signal than the previously used Lead Sulphide (PbS) detectors. The completed instrument was tested to determine its performance characteristics. Through these tests it was found that the photometer output offset is sensitive to ambient temperature fluctuations. An analysis of the instrument noise was done in an attempt to explain this sensitivity. The output noise performance was characterized and is presented together with the absolute brightness and wavelength calibrations. Data was collected with the instrument in Saskatoon, SK and Eureka, NU. After an initial observation campaign in the high arctic (Eureka, NU) modifications were made to the environmental housing of the instrument in order to improve the scientific value of the data collected. The collected data was processed and a simple analysis performed to demonstrate the capability of the photometer to measure the infrared atmospheric airglow. The collected data can be used to determine the mesospheric ozone height profile. The required data analysis to do so is beyond the scope of this presentation. However, the presented data does demonstrate that the designed and constructed two channel photometer can make the necessary measurements.

Measurements by OSIRIS, an infrared imaging system that measures emission from excited-state molecular oxygen, are used to retrieve mesospheric ozone through a photochemical model. The design of the model and the spectral data used in the calculation of pho- tochemical production coe±cients are presented. The model has been run in a variety of modes to provide comparisons with measurements of excited-state molec- ular oxygen; it has been found that the model results are in excellent agreement with measurements. The model is used in conjunction with a retrieval scheme to estimate the con- centrations of mesospheric ozone from measurements made on a satellite platform. An analysis of the sensitivity of retrieved ozone to key model parameters is done, and it is shown that uncertainty in several kinetic reaction rates can signi¯cantly change the retrieved results. Comparisons are made for the ozone retrieved in this work and that from several other instruments that make similar measurements. The retrieved concentrations are shown to be in excellent agreement with results from other instruments. The present work provides a climatological database of mesospheric ozone and will provide useful comparisons with concurrent measurements of mesospheric ozone. The new data obtained in this work are in good agreement with expected results, and it is shown that the unprecedented high-spatial resolution of OSIRIS reveals interesting features that should be further investigated.

<p>In many spatio-temporal applications a vector of covariates is measured alongside a spatio-temporal response. In such cases, the purpose of the statistical model is to quantify the change, in expectation or otherwise, in the response due to a change in the predictors while adequately accounting for the spatio-temporal structure of the response, the predictors, or both. The most common approach for building such a model is to confine the relationship between the response and the predictors to a single spatio-temporal coordinate. For spatio-temporal problems, however, the relationship between the response and predictors may not be so confined. For example, spatial models are often used to quantify the effect of pollution exposure on mortality. Yet, an unknown lag exists between time of exposure to pollutants and mortality. Furthermore, due to mobility and atmospheric movement, a spatial lag between pollution concentration and mortality may also exist (e.g. subjects may live in the suburbs where pollution levels are low but work in the city where pollution levels are high).</p><p>The contribution of this thesis is to propose a hierarchical modeling framework which captures complex spatio-temporal relationships between responses and covariates. Specifically, the models proposed here use kernels to capture spatial and/or temporal lagged effects. Several forms of kernels are proposed with varying degrees of complexity. In each case, however, the kernels are assumed to be parametric with parameters that are easily interpretable and estimable from the data. Full distributional results are given for the Gaussian setting along with consequences of model misspecification. The methods are shown to be effective in understanding the complex relationship between responses and covariates through various simulated examples and analyses of physical data sets.</p> / Dissertation

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Fumes emitted from coffee bean roasters contain various chemicals such as aldehydes, pyridine, volatile fatty acids, and ketones. These chemicals have high odor intensities and are sensitive to human breathing organs and eyes. In Taiwan, most of these fumes are not well controlled before venting to the atmosphere. This research attempted to eliminate these odorous and offensive chemicals by chemical scrubbing methods. Sodium hypochlorite oxidation followed by hydrogen peroxide reduction (hypochlorite-peroxide) was investigated first. After that, ozone oxidation followed by hydrogen peroxide reduction (ozone-peroxide) was also tried. In both methods, hydrogen peroxide acted as a reducing agent for the elimination of either residual chlorine or ozone emitted from the oxidation reaction. Experimental results indicated that both methods were effective. An oxidative scrubbing liquid with an initial effective chlorine content of 200 mg/L and a pH of 12, and an reducing scrubbing liquid with an initial hydrogen peroxide concentration of 1% and a pH of 12 could remove an average of 85% of total hydrogen carbons (THC) in the fume gas from a coffee bean roaster. With a dose of 10 ppm ozone in the fume gas to the oxidative scrubbing liquid (water only) followed by an reducing scrubbing liquid with an initial hydrogen peroxide concentration of 0.3% and a pH of 12, an average removal of 80% of the THC could be removed. An odor intensity (expressed by the dilution to threshold ratio) of 9,772 in the original fume could be reduced to as low as 31 by both methods. As indicated by the data from GC/MS (gas chromatography-mass spectrometry) analysis for the hypochlorite-peroxide method, acrolein, vinyl acetate, 2-butanone, and acetone in the roaster fume could almost completely be eliminated. Traces of chlorinated hydrocarbons as potential secondary pollutants were detected in the treated gases from the hypochlorite-peroxide scrubbing system. While by the ozone-peroxide one, satisfactory results were also obtained with no chlorinated hydrocarbons emitted. An economical analysis shows that the ozone-peroxide approach is a practical one for actual control applications.

In this research, used dimethyl ether as second fuel blended with diesel (mixed quantity with 10 L/min to 60 L/min, interval 10L/min), which test behavior of diesel engine and carbonyls emission investigated. The engine operated at steady-state condition of 1600 rpm, 145 Nm torque , eight kinds of carbonyls were sampling and analysis, and discuss the performance of the ozone formation potential (OFP). The results of regulated pollutant emissions, CO, THC and PM emission could increasing with the addition of DME, NOX emissions, along with the mixed rate of per minute from 10 L, 20 L, 30 L, 40 L, 50 L and 60 L of its reduction rate was 6.8%¡B8.3%¡B10.0%¡B10.6%¡B13.1% and 15.4%, shows that the DME can reduce NOX emissions. Add a various amount of dimethyl ether , which carbonyl compounds emission from the gas flow 0 L(with neat diesel), 10 L, 20 L, 30 L, 40 L, 50 L and 60 L concentrations were 2507.44 g/m3, 2665.27 g/m3, 2726.67 g/m3, 2958.07 g/m3, 4645.87 g/m3, 5470.20 g/m3 and 7279.91 g/m3; the emission factor of 143.58 mg/bhp-hr, 152.65 mg/bhp-hr, 156.62 mg/bhp-hr, 168.69 mg/bhp-hr, 266.22 mg/bhp-hr, 312.38 mg/bhp-hr and 416.36 mg/bhp-hr, shows the addition of DME will rising the carbonyl compound emissions of diesel engine. Gas of dimethyl ether (10,20,30,40,50 and 60 L/min) into the neat diesel fuel (0 L/min) as a mixture fuel additives, the effect of ozone formation potential as increase in the total ozone formation potential, 21945.93 g-O3/m3, 23698.40 g-O3/m3, 24427.46 g-O3/m3, 26672.98 g-O3/m3, 42683.69 g-O3/m3, 50519.26 g-O3/m3 and 67710.60 g-O3/m3 respectively, and ozone manufacturability will 0 L/min of 8.75 increased to 60 L/min of 9.30.

With the increases of environmental awareness and attention by the government and audiences, people begin to prosecute the pollution makers instead of tolerance. This study tried to control an air pollution source from a wallpaper plant for the purpose of attenuating odor prosecutes by residents near the plant. This study investigated chemical scrubbing, ozonation followed by GAC (Granular Activated Carbon) adsorption and biotrickling filtration techniques as control methods for eliminating odorous compounds from a waste gas stream emitted from the wallpaper plant. Scrubbing test results indicate that with an oxidative solution of 800 mg/L residual chlorine at pH 7.0 and a reductive solution of 0.2% hydrogen peroxide at pH = 12, around 90% of the VOCs (volatile organic compounds) in the tested gas could be removed. Odor intensities could be reduced from 2,317 (expressed as dilutions to threshold) to 130. Results also indicate that around 85 % of the carbonyl compounds, 41% of the alkenes and 22% of the alkanes in the waste gas could be eliminated. No removal of aromatic and halo-hydrocarbons was observed. It requires around NT$70 for chemicals to treat 1000 m3 of the gas. Ozonation-GAC adsorption tests indicate that with an ozone dosage of 5 ppm in the waste gas and a gas-ozone contact time of 12 s followed by GAC adsorption, around 95% of the VOCs in the tested gas could be removed. Odor intensities were reduced from 2,317 to <55. Around 94 % of the carbonyl compounds, 79% of the alkanes, 76% of halo-hydrocarbons, 41% of the alkenes and 20% of aromatics in the waste gas could be removed. Around NT$ 15,700 for ozone and GAC is required to treat 1000m3 of the gas. Results from biotrickling filtration tests indicate that with the supplementations of nitrogen and phosphorous nutrients to biofilms attached to wood-chip packings, around 83% of the influent VOCs could be biodegraded. Odor intensities could be reduced from 1,737 to <55. Around 61 % of the carbonyl compounds, 67% of the alkanes, 18% of halo-hydrocarbons and 33% of aromatics in the waste gas could be removed. Around NT$ 13 is required to treat 1000m3 of the gas. For an actual application, it is suggested that a process that a combination of chemical scrubbing and ozonation-GAC adsorption may be a proper solution to the control of the odorous emission from the plant. Biotrickling filtration can be best after verifying the performances of the technique by a pilot test.