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1.
The characteristics of carbonyl compounds (carbonyls) including concentrations, major sources, and personal exposure were investigated for 29 vehicles including taxi, bus and subway in Beijing. It was found that the taxis (Xiali, TA) and buses (Huanghe, BA) fueled by gasoline with longer service years had the higher indoor carbonyl levels (178±42.7 and 188±31.6 μg m−3) while subways energized by electricity without exhaust and the jingwa buses (BB) driven in the suburb had the lower levels with total concentrations of 98.5±26.3 and 92.1±20.3 μg m−3, respectively. Outdoor carbonyls of taxi cars and buses were nearly at the same level with their total concentrations varying from 80 to 110 μg m−3. The level of outdoor subways carbonyls was equal with the ambient air levels. Exhaust leakage, indoor material emissions, photochemical formation, and infiltration of outdoor air were considered to be the major sources to in-vehicle carbonyls. Personal exposures and cancer risk to formaldehyde and acetaldehyde were calculated for professional bus and taxi drivers, respectively. Taxi drivers had the highest cancer risk with personal exposure to formaldehyde and acetaldehyde of 212 and 243 μg day−1, respectively. The public concern should pay considerable attention to professional drivers’ health.  相似文献   

2.
The concentrations of C1–C8 carbonyl compounds were measured at two urban sites in Hong Kong from October 1997 to September 2000. The daily total carbonyl concentrations were found to range from 2.4 to 37 μg m−3. Formaldehyde was the most abundant species, which comprised from 36 to 43% of the total detected carbonyls, followed by acetaldehyde (18–21%) and acetone (8–20%). The highest 24-hour average concentrations measured were 10 and 7.7 μg m−3 for formaldehyde and acetaldehyde, respectively. Seasonal and temporal variations in the concentrations of formaldehyde and acetaldehyde were not obvious, but lowest concentrations often occurred from June to August. The mean formaldehyde/acetaldehyde molar ratios at the two sites in summer (2.8±1.1 and 2.5±1.2) were significantly higher (p⩽0.01) than those in winter periods (1.9±0.6 and 2.0±0.6). The phenomena were explained by influences of both photochemical reactions and local meteorological conditions. Better correlations between formaldehyde and acetaldehyde, and between NOx and each of the two major carbonyls were obtained in winter periods indicating direct vehicular emissions were the principal sources. The ambient formaldehyde and acetaldehyde concentrations in the urban atmosphere of Hong Kong were within the normal ranges reported in the literature for other urban sites world-wide.  相似文献   

3.
Indoor and outdoor carbonyl concentrations were measured simultaneously in 12 urban dwellings in Beijing, Shanghai, Guangzhou, and Xi’an, China in summer (from July to September in 2004) and winter (from December 2004 to February 2005). Formaldehyde was the most abundant indoor carbonyls species, while formaldehyde, acetaldehyde and acetone were found to be the most abundant outdoor carbonyls species. The average formaldehyde concentrations in summer indoor air varied widely between cities, ranging from a low of 19.3 μg m−3 in Xi’an to a high of 92.8 μg m−3 in Beijing. The results showed that the dwellings with tobacco smoke, incense burning or poor ventilation had significantly higher indoor concentrations of certain carbonyls. It was noticed that although one half of the dwellings in this study installed with low emission building materials or furniture, the carbonyls levels were still significantly high. It was also noted that in winter both the indoor and outdoor acetone concentrations in two dwellings in Guangzhou were significantly high, which were mainly caused by the usage of acetone as industrial solvent in many paint manufacturing and other industries located around Guangzhou and relatively longer lifetime of acetone for removal by photolysis and OH reaction than other carbonyls species. The indoor carbonyls levels in Chinese dwellings were higher than that in dwellings in the other countries. The levels of indoor and ambient carbonyls showed great seasonal differences. Six carbonyls species were carried out the estimation of indoor source strengths. Formaldehyde had the largest indoor source strength, with an average of 5.25 mg h−1 in summer and 1.98 mg h−1 in winter, respectively. However, propionaldehyde, crotonaldehyde and benzaldehyde had the weakest indoor sources.  相似文献   

4.
The fuel matrix used in Brazil is unique around the world. The intensive use of hydrated ethanol, gasohol (gasoline with 25% v/v of ethanol), compressed natural gas (CNG), and biodiesel leads to a peculiar composition of the urban atmosphere. From 1998 to 2002 an increase in formaldehyde levels was observed and since then, a reduction. This work presents a monitoring campaign that was executed from March 2004 to February 2009 by sampling at early morning on every sunny Wednesday for a total of 183 samples. The results indicate a strong reduction in formaldehyde levels from 2004 (average of 135.8 μg m?3 with SD 28.4 μg m?3) to 2009 (average of 49.3 μg m?3 with SD 27.4 μg m?3). The levels of acetaldehyde showed a slight reduction from 2004 (average of 34.9 μg m?3 with SD 8.0 μg m?3) to 2009 (average of 26.8 μg m?3 with SD 11.5 μg m?3). Comparing the results with the concurrent evolution of the fleet and of fuel composition indicates that the observed formaldehyde levels could be associated with the increase in ethanol use and in CNG use by engines with improved technology over the first converted CNG engines. Modelling studies using the OZIPR trajectory model and the SAPRC chemical mechanism indicate that formaldehyde is the main ozone precursor in Rio de Janeiro and acetaldehyde is the forth one.  相似文献   

5.
A preliminary study of ambient carbonyls was performed in Xalapa City to measure carbonyls in the atmosphere of this City, because it has an explosive increase in population and traffic density, but few industries. The city is located at the eastern flanks of the Sierra Madre Oriental, between 1350 and 1550 m above sea level. Acetone was the most abundant carbonyl in June, followed by formaldehyde and acetaldehyde, whereas acetaldehyde was the most abundant one in November. Higher concentrations were observed in autumn than in spring, probably due to stagnation conditions in autumn and heavy rains from late spring to early autumn. The very high concentrations of acetaldehyde found in November could have been caused by an accidental leak or spill from a truck, since no stationary sources were identified and acetaldehyde concentrations steeply rose and constantly decreased after few days. Moreover, a highly transited highway traverses Xalapa. The most important ozone and carbon monoxide concentrations were below the Mexican Air Quality Standards; 216 μg m−3 (0.11 ppm) for 1 h average and 12.6 mg m−3 (11 ppm) for 8 h moving average, respectively. The low concentrations of the main carbonyls, compared with the values reported for other urban areas, and of carbon monoxide, seem to indicate that air quality is still satisfactory in Xalapa City.  相似文献   

6.
Behavioral and environmental determinants of PM2.5 personal exposures were analyzed for 201 randomly selected adult participants (25–55 years old) of the EXPOLIS study in Helsinki, Finland. Personal exposure concentrations were higher than respective residential outdoor, residential indoor and workplace indoor concentrations for both smokers and non-smokers. Mean personal exposure concentrations of active smokers (31.0±31.4 μg m−3) were almost double those of participants exposed to environmental tobacco smoke (ETS) (16.6±11.8 μg m−3) and three times those of participants not exposed to tobacco smoke (9.9±6.2 μg m−3). Mean indoor concentrations of PM2.5 when a member of the household smoked indoors (20.8±23.9 μg m−3) were approximately 2.5 times the concentrations of PM2.5 when no smoking was reported (8.2±5.2 μg m−3). Interestingly, however, both mean (8.2 μg m−3) and median (6.9 μg m−3) residential indoor concentrations for non-ETS exposed participants were lower than residential outdoor concentrations (9.5 and 7.3 μg m−3, respectively). In simple linear regression models residential indoor concentrations were the best predictors of personal exposure concentrations. Correlations (r2) between PM2.5 personal exposure concentrations of all participants, both smoking and non-smoking, and residential indoor, workplace indoor, residential outdoor and ambient fixed site concentrations were 0.53, 0.38, 0.17 and 0.16, respectively. Predictors for personal exposure concentrations of non-ETS exposed participants identified in multiple regression were residential indoor concentrations, workplace concentrations and traffic density in the nearest street from home, which accounted for 77% of the variance. Subsequently, step-wise regression not including residential and workplace indoor concentrations as input (as these are frequently not available), identified ambient PM2.5 concentration and home location, as predictors of personal exposure, accounting for 47% of the variance. Ambient fixed site PM2.5 concentrations were closely related to residential outdoor concentrations (r2=0.9, p=0.000) and PM2.5 personal exposure concentrations were higher in summer than during other seasons. Personal exposure concentrations were significantly (p=0.040) higher for individuals living downtown compared with individuals in suburban family homes. Further analysis will focus on comparisons of determinants between Helsinki and other EXPOLIS centers.  相似文献   

7.
Personal exposures, residential indoor, outdoor and workplace levels of nitrogen dioxide (NO2) were measured for 262 urban adult (25–55 years) participants in three EXPOLIS centres (Basel; Switzerland, Helsinki; Finland, and Prague; Czech Republic) using passive samplers for 48-h sampling periods during 1996–1997. The average residential outdoor and indoor NO2 levels were lowest in Helsinki (24±12 and 18±11 μg m−3, respectively), highest in Prague (61±20 and 43±23 μg m−3), with Basel in between (36±13 and 27±13 μg m−3). Average workplace NO2 levels, however, were highest in Basel (36±24 μg m−3), lowest in Helsinki (27±15 μg m−3), with Prague in between (30±18 μg m−3). A time-weighted microenvironmental exposure model explained 74% of the personal NO2 exposure variation in all centres and in average 88% of the exposures. Log-linear regression models, using residential outdoor measurements (fixed site monitoring) combined with residential and work characteristics (i.e. work location, using gas appliances and keeping windows open), explained 48% (37%) of the personal NO2 exposure variation. Regression models based on ambient fixed site concentrations alone explained only 11–19% of personal NO2 exposure variation. Thus, ambient fixed site monitoring alone was a poor predictor for personal NO2 exposure variation, but adding personal questionnaire information can significantly improve the predicting power.  相似文献   

8.
The aerosol scattering properties were investigated at two continental sites in northern China in 2004. Aerosol light scattering coefficient (σsp) at 525 nm, PM10, and aerosol mass scattering efficiencies (α) at Dunhuang had a mean value of 165.1±148.8 M m−1, 157.6±270.0 μg m−3, and 2.30±3.41 m2 g−1, respectively, while these values at Dongsheng were, respectively, 180.2±151.9 M m−1, 119.0±112.9 μg m−3, and 1.87±1.41 m2 g−1. There existed a seasonal variability of aerosol scattering properties. In spring, at Dunhuang PM10, σsp, and α were 184.1±211.548 μg m−3, 126.3±89.6 M m−1, and 1.05±0.97 m2 g−1, respectively, and these values at Dongsheng were 146.4±142.1 μg m−3, 183.4±81.7 M m−1, and 1.98±1.52 m2 g−1, respectively. However, in winter at Dunhuang PM10, σsp, and α were 158.1±261.4 μg m−3, 303.3±165.2 M m−1, and 3.17±1.93 m2 g−1, respectively, and these values at Dongsheng were 155.7±170.1 μg m−3, 304.4±158.1 M m−1, and 2.90±1.72 m2 g−1, respectively. σsp and α in winter were higher than that in spring at both the sites, which coincides with the characteristics of dust aerosol and pollution aerosol. Overall, the dominant aerosol types in spring and winter at both sites in northern China are dust aerosol and pollution aerosol, respectively.  相似文献   

9.
The estimated annual throughfall deposition flux of Hg in a northern mixed-hardwood forest in the Lake Huron Watershed was 10.5±1.0 μg m−2 compared to an annual precipitation Hg flux of 8.7±0.5 μg m−2 (June 1996–June 1997). The source of this additional Hg in throughfall is often attributed to wash-off of dry deposition, but foliar leaching of Hg may also be important. To determine the influence of both dry deposition and foliar leaching of Hg and other elements in throughfall, we measured a suite of trace elements (Hg, Al, Mg, V, Mn, Cu, Zn, As, Rb, Sr, Cd, Ba, La, Ce, and Pb) in throughfall, precipitation, and ambient air samples from a northern mixed-hardwood forest. Based on a multiple linear regression model, dry deposition had the most important influence on Hg, Al, La, Ce, V, As, Cu, Zn, Cd, and Pb fluxes while foliar leaching strongly influenced Mg, Mn, Rb, Sr, and Ba fluxes in net throughfall. The Hg dry deposition flux was estimated using gaseous and aerosol Hg measurements and modeled deposition velocities. The calculated dry deposition flux (∼12–14 μg m−2) of Hg to the canopy indicated that atmospheric deposition of Hg could easily account for all of the Hg deposited in net throughfall (1.9±0.1 μg m−2). Although there is a large uncertainty associated with these techniques, the modeling estimates indicate that atmospheric Hg may account for all of the Hg deposited in litterfall (11.4±2.8 μg m−2).  相似文献   

10.
Air–water exchange fluxes of polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in air and water samples from two sites on the Kenting coast, located at the southern tip of Taiwan, from January to December 2010. There was no significant difference in the total PAH (t-PAH) concentrations in both gas and dissolved phases between these two sites due to the less local input which also coincided to the low levels of t-PAH concentration; the gas and dissolved phases averaged 1.29 ± 0.59 ng m?3 and 2.17 ± 1.19 ng L?1 respectively. The direction and magnitude of the daily flux of PAHs were significantly influenced by wind speed and dissolved PAH concentrations. Individual PAH flux ranged from 627 ng m?2 d?1 volatilization of phenanthrene during the rainy season with storm–water discharges raising dissolved phase concentration, to 67 ng m?2 d?1 absorption of fluoranthene during high wind speed periods. Due to PAH annual fluxes through air–water exchange, Kenting seawater is a source of low molecular weight PAHs and a reservoir of high molecular weight PAHs. Estimated annual volatilization fluxes ranged from 7.3 μg m?2 yr?1 for pyrene to 50 μg m?2 yr?1 for phenanthrene and the absorption fluxes ranged from ?2.6 μg m?2 yr?1 for chrysene to ?3.5 μg m?2 yr?1 for fluoranthene.  相似文献   

11.
Children’s exposures to ambient and non-ambient fine particulate matter (PM2.5) were determined using the sulphate and elemental carbon components of the PM2.5 mixture as tracers of the ambient contribution during a 6-week winter period in Prince George, British Columbia, Canada. Personal exposures to PM2.5 were measured in children at 5 elementary schools located throughout the city and ambient samples were collected on school rooftops. Average ambient levels and personal exposures during this time period were 13.8 μg m?3 and 16.4 μg m?3 respectively. From the data pooled across individuals, use of the two different tracers indicated identical estimates of median exposure to ambient PM2.5 (7.5 μg m?3) and similar estimates of non-ambient generated exposure (6.4 and 5.0 μg m?3) and infiltration (0.49 and 0.52) for the sulphate and elemental carbon approach, respectively. The median fraction of the ambient concentration resulting in exposure or exposure factors were 0.54 and 0.55 respectively, however lower values of 0.46 and 0.42 were determined from regression analysis. A strong association was found between exposure to ambient PM2.5 and measured ambient concentrations at both the closest school monitor (median r = 0.92) and a central site (median r = 0.88) demonstrating that the central site monitor was suitable for assessing longitudinal ambient generated exposure throughout the city. These results support the use of elemental carbon as a tracer of ambient generated exposure and the use of ambient data as estimates of longitudinal changes in children’s exposure in this setting. The importance of both ambient and non-ambient sources of PM2.5 is emphasized by their almost equal contribution to total personal exposures. Comparison with other studies suggests a limited influence of climate and the cold season in Prince George on exposure levels and found similar mean non-ambient generated exposures despite large variability across and within subjects in any given location.  相似文献   

12.
The effects of natural compounds on reducing formaldehyde emission from plywood were investigated. Urea, catechin and vanillin were examined as the natural formaldehyde reducers. The microemission cell, with an internal volume of 35 ml, the maximum exposed test surface area of 177 cm2 and an air purge flow rate of 50 ml min−1, was used to measure specific emission rate (SER). In the case of no reducer treatment, formaldehyde emission from plywood was fast and SERs were 4.4 mg m−2 h−1 at 30 °C and 15 mg m−2 h−1 at 60 °C. When this plywood was treated with the natural compounds, the SERs of formaldehyde were decreased at all temperatures. In the case of urea treatment, the SERs of formaldehyde decreased to 0.30 mg m−2 h−1 at 30 °C and 0.65 mg m−2 h−1 at 60 °C. When the urea treatment was applied to the inside of kitchen cabinet (made from plywood; 270 cm wide, 60 cm deep, 250 cm high), the concentration of formaldehyde was reduced substantially from 1600 to 130 μg m−3. The reducing effect of formaldehyde continued during the observation period (6 months), with a mean concentration of 100 μg m−3. Reducers in the plywood would react with released formaldehyde. Application of natural compounds such as urea, catechin and vanillin could provide a simple and effective approach for suppressing formaldehyde emission from plywood.  相似文献   

13.
The present study has been conducted in the frame of BUMA (Prioritization of Building Materials Emissions as indoor pollution sources), a European funded project, aiming at assessing the exposure to emitted compounds in indoor air. Field campaigns in five (5) European cities (Milan, Copenhagen, Dublin, Athens and Nicosia) were carried out. These campaigns covered weekly winter and summer concentration measurements in two (2) public buildings and two (2) private houses in each city. BTEX, terpenes, and carbonyls were measured using passive sampling in two sites inside the building and one outside. VOC emission measurements on selected building material have also been performed using Field and Laboratory Emission Cell (FLEC). The results on indoor concentrations for compounds such as formaldehyde (1.2–62.6 μg m?3), acetaldehyde (0.7–41.6 μg m?3), toluene (0.9–163.5 μg m?3), xylenes (0.2–177.5 μg m?3) and acetone (2.8–308.8 μg m?3) have shown diversity and relatively significant indoor sources depending on the building type, age etc. Indoor concentrations of these substances are varied depending on the building age and type. The percentage of approximately 40% of the indoor air quality levels originated from building materials.  相似文献   

14.
Carbonaceous aerosol particles were observed in a residential area with wood combustion during wintertime in Northern Sweden. Filter samples were analyzed for elemental carbon (EC) and organic carbon (OC) content by using a thermo-optical transmittance method. The light-absorbing carbon (LAC) content was determined by employing a commercial Aethalometer and a custom-built particle soot absorption photometer. Filter samples were used to convert the optical signals to LAC mass concentrations. Additional total PM10 mass concentrations and meteorological parameters were measured. The mean and standard deviation mass concentrations were 4.4±3.6 μg m−3 for OC, and 1.4±1.2 μg m−3 for EC. On average, EC accounted for 10.7% of the total PM10 and the contribution of OC to the total PM10 was 35.4%. Aethalometer and custom-built PSAP measurements were highly correlated (R2=0.92). The hourly mean value of LAC mass concentration was 1.76 μg m−3 (median 0.88 μg m−3) for the winter 2005–2006. This study shows that the custom-built PSAP is a reliable alternative for the commercial Aethalometer with the advantage of being a low-cost instrument.  相似文献   

15.
Atmospheric deposition of Hg and selected trace elements was reconstructed over the past 150 years using sediment cores collected from nine remote, high-elevation lakes in Rocky Mountain National Park in Colorado and Glacier National Park in Montana. Cores were age dated by 210Pb, and sedimentation rates were determined using the constant rate of supply model. Hg concentrations in most of the cores began to increase around 1900, reaching a peak sometime after 1980. Other trace elements, particularly Pb and Cd, showed similar post-industrial increases in lake sediments, confirming that anthropogenic contaminants are reaching remote areas of the Rocky Mountains via atmospheric transport and deposition. Preindustrial (pre-1875) Hg fluxes in the sediment ranged from 5.7 to 42 μg m?2 yr?1 and modern (post-1985) fluxes ranged from 17.7 to 141 μg m?2 yr?1. The average ratio of modern to preindustrial fluxes was 3.2, which is similar to remote lakes elsewhere in North America. Estimates of net atmospheric deposition based on the cores were 3.1 μg m?2 yr?1 for preindustrial and 11.7 μg m?2 yr?1 for modern times. Current-day measurements of wet deposition range from 5.0 to 8.6 μg m?2 yr?1, which are lower than the modern sediment-based estimate of 11.7 μg m?2 yr?1, perhaps owing to inputs of dry-deposited Hg to the lakes.  相似文献   

16.
Regional estimates of fluxes of volatile organic compounds (VOCs) are required to improve our understanding of their role in the chemistry of the atmosphere. Flux measurements on such a scale can best be obtained using aircraft-based systems. These systems usually rely on the eddy covariance technique, which requires fast response gas sensors for flux measurement, but such sensors are not available for most organic compounds, therefore, the relaxed eddy-accumulation (REA) technique was selected. An aircraft-based REA sampling system was developed and used to measure isoprene emission over the boreal forest during the 1996 summer. Over a short period in July at the Boreal Ecosystem/Atmosphere Study (BOREAS) southern study area (SSA), the isoprene fluxes ranged from −0.06 to 1.79 μg m-2 s-1, with a mean of 0.59±0.34 μg m-2 s-1, while in August at the BOREAS northern study area (NSA) the isoprene fluxes ranged from 0.00 to 0.26 μg m-2 s-1, with a mean of 0.14±0.09 μg m-2 s-1. In the SSA, the isoprene fluxes over aspen ranged from 0.44 to 1.79 μg m-2 s-1, with a mean of 0.92±0.33 μg m-2 s-1, whereas over black spruce, isoprene fluxes ranged from −0.06 to 0.54 μg m-2 s-1, with a mean of 0.36±0.21 μg m-2 s-1. The isoprene fluxes were exponentially correlated with solar radiation and radiative surface temperature. High correlations between isoprene fluxes and the fluxes of CO2 and latent heat were also observed. Carbon lost through isoprene emissions was about 0.7 and 0.8% of the CO2 assimilation rate for aspen and black spruce, respectively. The results demonstrate that the aircraft-based relaxed eddy-accumulation technique is a promising approach for quantifying the atmosphere–surface exchange of VOCs on a regional scale.  相似文献   

17.
The long-range transported smokes emitted by biomass burning had a strong impact on the PM2.5 mass concentrations in Helsinki over the 12 days period in April and May 2006. To characterize aerosols during this period, the real-time measurements were done for PM2.5, PM2.5–10, common ions and black carbon. Moreover, the 24-h PM1 filter samples were analysed for organic and elemental carbon (OC and EC), water-soluble organic carbon (WSOC), ions and levoglucosan. The Finnish emergency and air quality modelling system SILAM was used for the forecast of the PM2.5 concentration generated by biomass burning. According to the real-time PM2.5 data, the investigated period was divided into four types of PM situations: episode 1 (EPI-1; 25–29 April), episode 2 (EPI-2; 1–5 May), episode 3 (EPI-3; 5–6 May) and a reference period (REF; 24 March–24 April). EPI-3 included a local warehouse fire and therefore it is discussed separately. The PM1 mass concentrations of biomass burning tracers—levoglucosan, potassium and oxalate—increased during the two long-range transport episodes (EPI-1 and EPI-2). The most substantial difference between the episodes was exhibited by the sulphate concentration, which was 4.9 (±1.4) μg m−3 in EPI-2 but only 2.4 (±0.31) μg m−3 in EPI-1 being close to that of REF (1.8±0.54 μg m−3). The concentration of particulate organic matter in PM1 was clearly higher during EPI-1 (11±3.3 μg m−3) and EPI-2 (9.7±4.0 μg m−3) than REF (1.3±0.45 μg m−3). The long-range transported smoke had only a minor impact on the WSOC-to-OC ratio. According to the model simulations, MODIS detected the fires that caused the first set of concentration peaks (EPI-1) and the local warehouse fire (EPI-3), but missed the second one (EPI-2) probably due to dense frontal clouds.  相似文献   

18.
Hourly concentrations of benzene, toluene, ethylbenzene, m,p-xylenes, and o-xylene (BTEX) plus CO, NOx, SO2 were monitored at roadsides simultaneously with the traffic volume during the dry season of 2004, in Hanoi, Vietnam. The selected three streets included Truong Chinh (TC) with high traffic volume, Dien Bien Phu (DBP) with low traffic volume, and Nguyen Trai (NT) with high traffic volume running through an industrial estate. BTEX were sampled by SKC charcoal tubes and analyzed by GC–FID. Geometric means of hourly benzene, toluene, ethylbenzene, m,p-xylenes and o-xylene are, respectively, 65, 62, 15, 43, and 22 μg m−3 in TC street; 30, 38, 9, 26, and 13 μg m−3 in DBP street; and 123, 87, 24, 56, and 30 μg m−3 in NT street. Levels of other gaseous pollutants including CO, NOx, and SO2, measured by automatic instruments, were low and not exceeding the Vietnam national ambient air quality standards. BTEX levels were comparatively analyzed for different downwind distances (3–50 m) from the street, between peak hours and off-peak hours, as well as between weekdays and weekend. Results of principal component analysis suggest that the gaseous pollutants are associated with different vehicle types.  相似文献   

19.
We use a global 3-D atmospheric chemistry model (GEOS-Chem) to simulate surface and aircraft measurements of organic carbon (OC) aerosol over eastern North America during summer 2004 (ICARTT aircraft campaign), with the goal of evaluating the potential importance of a new secondary organic aerosol (SOA) formation pathway via irreversible uptake of dicarbonyl gases (glyoxal and methylglyoxal) by aqueous particles. Both dicarbonyls are predominantly produced in the atmosphere by isoprene, with minor contributions from other biogenic and anthropogenic precursors. Dicarbonyl SOA formation is represented by a reactive uptake coefficient γ = 2.9 × 10?3 and takes place mainly in clouds. Surface measurements of OC aerosol at the IMPROVE network in the eastern U.S. average 2.2 ± 0.7 μg C m?3 for July–August 2004 with little regional structure. The corresponding model concentration is 2.8 ± 0.8 μg C m?3, also with little regional structure due to compensating spatial patterns of biogenic, anthropogenic, and fire contributions. Aircraft measurements of water-soluble organic carbon (WSOC) aerosol average 2.2 ± 1.2 μg C m?3 in the boundary layer (<2 km) and 0.9 ± 0.8 μg C m?3 in the free troposphere (2–6 km), consistent with the model (2.0 ± 1.2 μg C m?3 in the boundary layer and 1.1 ± 1.0 μg C m?3 in the free troposphere). Source attribution for the WSOC aerosol in the model boundary layer is 27% anthropogenic, 18% fire, 28% semi-volatile SOA, and 27% dicarbonyl SOA. In the free troposphere it is 13% anthropogenic, 37% fire, 23% semi-volatile SOA, and 27% dicarbonyl SOA. Inclusion of dicarbonyl SOA doubles the SOA contribution to WSOC aerosol at all altitudes. Observed and simulated correlations of WSOC aerosol with other chemical variables measured aboard the aircraft suggest a major SOA source in the free troposphere compatible with the dicarbonyl mechanism.  相似文献   

20.
Sources of carbonaceous aerosols collected from three sites of Chattanooga, TN (CH), Muscle Shoals, AL (MS), and Look Rock, TN (LR) in the Tennessee Valley Region (TVR) were apportioned using both organic tracer-based chemical mass balance (CMB) modeling and radiocarbon (14C) measurement and the results were compared. Eight sources were resolved by CMB, among which wood combustion (averaging 0.92 μg m−3) was the largest contributor to primary organic carbon (OC) concentrations, followed by gasoline exhaust (0.35 μg m−3), and diesel exhaust (0.18 μg m−3). The identified primary sources accounted for 43%, 71%, and 14% of measured OC at CH, MS, and LR, respectively. Contributions from the eight primary sources resolved by CMB could explain 107±10% of ambient elemental carbon (EC) concentrations, with diesel exhaust (66±32%) and wood combustion (37±33%) as the most important contributors. The fossil fractions in total carbon determined by 14C measurements were in reasonably good agreement with that in primary (OC+EC) carbon apportioned by CMB in the MS winter samples. The comparison between the 14C and CMB results revealed that contemporary sources dominated other OC in the TVR, especially in summertime (84% contemporary).  相似文献   

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