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Robert R. Arnts Robert L. Seila Joseph J. Bufalini 《Journal of the Air & Waste Management Association (1995)》2013,63(4):453-460
A relative rate procedure was used to measure hydroxyl rate constants at room temperature in the presence of oxygen. The photolysis of methyl nitrite in the presence of nitric oxide was used to generate OH radicals. The rate of loss of the test compounds was measured relative to that of ethane (kOH = 2.74 × 10-13 cm3 molec-1 s-1). The rates obtained at 297 ± 2 K are: acetylene = (7.8 ± 1.6) × 10-13 cm3 molec-1 s-1,1,2-dichloroethane (2.8 ± Q.6) × 10-13 cm3 molec-1 s-1, 1,2-dibromoethane (2.4 ± 0.5) × 10-13 cm3 molec-1 s-1, p-dichlorobenzene (4.3 ± 0.9) × 10-13 cm3 molec-1 s-1 and carbon disulfide (29 ± 6) × 10-13 cm3 molec-1 s-1. Under a proposed EPA rule, this OH rate determination procedure could be used to determine if a given volatile organic will be subject to control for reduction of photochemical ozone. 相似文献
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Teri L. Conner William A. Lonneman Robert L. Seila 《Journal of the Air & Waste Management Association (1995)》2013,63(5):383-394
Abstract Samples representative of transportation-related hydrocarbon emissions were collected as part of the 1990 Atlanta Ozone Precursor Monitoring Study. Motor vehicle emissions were sampled in canisters beside a roadway in a tunnel-like underpass during periods of heavy traffic. Airport and aircraft emissions were approximated by canister samples obtained at a major airport facility. Three octane grades of gasoline were purchased from six major vendors in Atlanta. Canister samples were prepared using these fuels to approximate the whole gasoline and gasoline vapor composition of the fuels in use during the study. All samples were analyzed by gas chromatography/flame ionization detection (GC/FID) for their hydrocarbon content. Detailed speciated hydrocarbon profiles were developed from this source sampling and analysis program for use in the Chemical Mass Balance (CMB) model. Profiles presented and discussed here represent the hydrocarbon composition of emissions from a roadway, composite headspace gasoline at two temperatures, composite whole gasoline, whole gasoline at three octane grades, and an airport. The roadway profile is compared with similar profiles in the literature, and recommendations are made regarding its use in the CMB model. The roadway and fuel profiles are discussed in the context of the MOBILE5 model outputs. The headspace gasoline vapor profile presented here is compared with a headspace gasoline vapor profile calculated from the whole gasoline profile by means of Raoult’s law. Agreement between the measured and calculated headspace profiles is excellent. The airport profile demonstrates the importance of high molecular weight volatile hydrocarbons in airport and aircraft emissions. 相似文献
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Spatial gradients and source apportionment of volatile organic compounds near roadways 总被引:1,自引:0,他引:1
David A. Olson Davyda M. Hammond Robert L. Seila Janet M. Burke Gary A. Norris 《Atmospheric environment (Oxford, England : 1994)》2009,43(35):5647-5653
Concentrations of 55 volatile organic compounds (VOCs) (C2–C12) are reported near a highway in Raleigh, NC. Thirty-minute samples were collected at eight locations, ranging from approximately 10–100 m perpendicular from the roadway. The highest concentrations of VOCs were generally measured closest to the roadway, and concentrations decreased exponentially with increasing distance from the roadway. The highest mean concentration for individual VOCs were for ethylene (3.10 ppbv) (mean concentration at x = 13 m), propane (2.27 ppbv), ethane (1.91 ppbv), isopentane (1.54 ppbv), toluene (0.95 ppbv), and n-butane (0.89 ppbv). Concentrations at the nearest roadway location (x = 13 m) were generally between 2.0 and 1.5 times those from the farthest roadway location (x = 92 m). The data were apportioned into four source categories using the EPA Chemical Mass Balance Model (CMB8.2): motor vehicle exhaust, compressed natural gas, propane gas, and evaporative gasoline. The majority of the VOCs resulted from motor vehicle exhaust (67 ± 12%) (% of total VOC at x = 13 m ± S.D.). Compressed natural gas, propane gas, and evaporative gasoline accounted for approximately 15%, 7% and 1% of the total VOC emissions, respectively, at x = 13 m. 相似文献
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Traffic and meteorological impacts on near-road air quality: summary of methods and trends from the Raleigh Near-Road Study 总被引:2,自引:0,他引:2
Baldauf R Thoma E Hays M Shores R Kinsey J Gullett B Kimbrough S Isakov V Long T Snow R Khlystov A Weinstein J Chen FL Seila R Olson D Gilmour I Cho SH Watkins N Rowley P Bang J 《Journal of the Air & Waste Management Association (1995)》2008,58(7):865-878
A growing number of epidemiological studies conducted worldwide suggest an increase in the occurrence of adverse health effects in populations living, working, or going to school near major roadways. A study was designed to assess traffic emissions impacts on air quality and particle toxicity near a heavily traveled highway. In an attempt to describe the complex mixture of pollutants and atmospheric transport mechanisms affecting pollutant dispersion in this near-highway environment, several real-time and time-integrated sampling devices measured air quality concentrations at multiple distances and heights from the road. Pollutants analyzed included U.S. Environmental Protection Agency (EPA)-regulated gases, particulate matter (coarse, fine, and ultrafine), and air toxics. Pollutant measurements were synchronized with real-time traffic and meteorological monitoring devices to provide continuous and integrated assessments of the variation of near-road air pollutant concentrations and particle toxicity with changing traffic and environmental conditions, as well as distance from the road. Measurement results demonstrated the temporal and spatial impact of traffic emissions on near-road air quality. The distribution of mobile source emitted gas and particulate pollutants under all wind and traffic conditions indicated a higher proportion of elevated concentrations near the road, suggesting elevated exposures for populations spending significant amounts of time in this microenvironment. Diurnal variations in pollutant concentrations also demonstrated the impact of traffic activity and meteorology on near-road air quality. Time-resolved measurements of multiple pollutants demonstrated that traffic emissions produced a complex mixture of criteria and air toxic pollutants in this microenvironment. These results provide a foundation for future assessments of these data to identify the relationship of traffic activity and meteorology on air quality concentrations and population exposures. 相似文献
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Near-road multipollutant profiles: associations between volatile organic compounds and a tracer gas surrogate near a busy highway 总被引:1,自引:0,他引:1
Barzyk TM Ciesielski A Shores RC Thoma ED Seila RL Isakov V Baldauf RW 《Journal of the Air & Waste Management Association (1995)》2012,62(5):594-603
This research characterizes associations between multiple pollutants in the near-road environment attributed to a roadway line source. It also examines the use of a tracer gas as a surrogate of mobile source pollutants. Air samples were collected in summa canisters along a 300 m transect normal to a highway in Raleigh, North Carolina for five sampling periods spanning four days. Samples were subsequently measured for volatile organic compounds (VOCs) using an electron capture gas chromatograph. Sulfur hexafluoride (SF6) was released from a finite line source adjacent to the roadway for two of the sampling periods, collected in the canisters and measured with the VOCs. Associations between each VOC, and between VOCs and the tracer, were quantified with Pearson correlation coefficients to assess the consistency of the multi-pollutant dispersion profiles, and assess the tracer as a potential surrogate for mobile source pollutants. As expected, benzene, toluene, ethylbenzene, and m,p- and o-xylenes (collectively, BTEX) show strong correlations between each other; further BTEX shows a strong correlation to SF6. Between 26 VOCs, correlation coefficients were greater than 0.8, and 14 VOCs had coefficients greater than 0.6 with the tracer gas. Even under non-downwind conditions, chemical concentrations had significant correlations with distance. Results indicate that certain VOCs are representative of a larger multi-pollutant mixture, and many VOCs are well-correlated with the tracer gas. 相似文献
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Basil Dimitriades Bruce W. Gay Jr. Robert R. Arnts Robert L. Seila 《Journal of the Air & Waste Management Association (1995)》2013,63(6):575-587
Perchloroethylene (PCE), a solvent used in dry cleaning, has been suspected of contributing significantly to photochemical ozone/oxidant (O3/Ox) problems in urban atmospheres. Past evidence, however, was neither complete nor consistent. To interpret more conclusively the past evidence, and further understand PCE's role in the O3Ox problem, a smog chamber testing program was conducted. The program's objectives were: (a) to explain the mechanism of the PCE reaction in smog chamber atmospheres, and (b) to extrapolate the smog chamber findings regarding PCE reactivity to the real atmosphere. Results showed that in smog chambers, PCE reacts and forms O3/Ox following what appears to be a Cl instigated photooxidation mechanism rather than the OH initiated mechanism accepted in current smog chemistry. The evidence, collectively, strongly supported this conclusion even though the source of Cl atoms could not be identified with confidence. It was further concluded that in the real atmosphere neither the Cl instigated nor the OH instigated photooxidations of PCE can generate substantial concentrations of O3/Ox. In fact, PCE contributes less to the ambient O3/Ox problem than equal concentrations of ethane. 相似文献
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Akula Venkatram Vlad Isakov Robert Seila Richard Baldauf 《Atmospheric environment (Oxford, England : 1994)》2009,43(20):3191-3199
The dispersion formulation incorporated in the U.S. Environmental Protection Agency's AERMOD regulatory dispersion model is used to estimate the contribution of traffic-generated emissions of select VOCs – benzene, 1,3-butadiene, toluene – to ambient air concentrations at downwind receptors ranging from 10-m to 100-m from the edge of a major highway in Raleigh, North Carolina. The contributions are computed using the following steps: 1) Evaluate dispersion model estimates with 10-min averaged NO data measured at 7 m and 17 m from the edge of the road during a field study conducted in August, 2006; this step determines the uncertainty in model estimates. 2) Use dispersion model estimates and their uncertainties, determined in step 1, to construct pseudo-observations. 3) Fit pseudo-observations to actual observations of VOC concentrations measured during five periods of the field study. This provides estimates of the contributions of traffic emissions to the VOC concentrations at the receptors located from 10 m to 100 m from the road. In addition, it provides estimates of emission factors and background concentrations of the VOCs, which are supported by independent estimates from motor vehicle emissions models and regional air quality measurements. The results presented in the paper demonstrate the suitability of the formulation in AERMOD for estimating concentrations associated with mobile source emissions near roadways. This paper also presents an evaluation of the key emissions and dispersion modeling inputs necessary for conducting assessments of local-scale impacts from traffic emissions. 相似文献
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S. L. Kopczynski W. A. Lonneman T. Winfield R. Seila 《Journal of the Air & Waste Management Association (1995)》2013,63(3):251-255
During the fall of 1972, a study was undertaken to characterize gaseous air pollutants in the St. Louis metropolitan area. Information obtained in this study will be used in planning air pollution modeling studies to be carried out over the next 4 or 5 years under the Regional Air Pollution Study (RAPS) of the Environmental Protection Agency. From analyses of roadway samples, it was found that certain compounds in automotive emissions such as acetylene, carbon monoxide, o-xylene, ethylene, and 2-methylpentane occur in consistent proportions to other compounds. The concentrations of these indicator compounds in atmospheric samples were used to estimate the amounts of other hydrocarbons present that are attributable to automotive related emissions. Methane, ethane, and propane were found to originate principally from nonautomotive sources, both at St. Louis University and the St. Louis CAMP station. Similar concentrations were found in urban and non-urban areas. A comparison of ethylene-CO and propyl-ene-CO ratios in urban and non-urban areas indicates that CO can serve as an indicator of transport of urban pollutants. Sunlight irradiations of captured air samples showed increasing ozone production with increasing initial concentrations of hydrocarbons and nitrogen oxides. Substantial ozone and peroxyacetyl nitrate were formed from a total non-methane hydrocarbon concentration of only 1/4 ppm C. 相似文献
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