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1.
O3 concentrations were simulated over the Seoul metropolitan area in Korea using a simple semi-empirical reaction (SEGRS) model which consists of generic reaction set (GRS), photochemical reaction set, and the diagnostic wind field generation model. The aggregated VOC emission strength was empirically scaled by the comparison of the simulated slope of (O3–2NO–NO2) concentration as a function of cumulative actinic light flux against measurements on high surface ozone concentration days with the relatively weak easterly geostrophic winds at the 850 hPa level in summer when the effect of horizontal advection was fairly small. The results indicated that the spatial distribution patterns and temporal variations of spatially averaged ground-level ozone concentrations were quite well simulated compared with those of observations with the modified volatile organic compound (VOC) emission strength. The diurnal trend of the surface ozone concentration and the maximum concentration compared observations were also quite reasonably simulated. However, the maximum ozone concentration occurring time at Seoul lagged about 2 h and the ozone concentration in the suburban area was slightly overestimated in the afternoon due to the influx of high ozone concentration from the urban area. It was found that the SEGRS model could be effectively used to simulate or predict the ground-level ozone concentration reasonably well without heavy computational cost provided the emission of ozone precursors are given.  相似文献   

2.
Abstract

Ground‐level ozone (O3) time series are characterized by the sum of several distinct temporal scales: long‐term, seasonal, synoptic, diurnal (daily), and intraday variation. In this study, the authors use a Kolmorogov‐Zurbenko filter to separate the 1981–2001 O3 time‐series from many sites in and around Georgia into these various components. The authors compare the temporal components to examine differences between small and large metropolitan areas and between urban and rural areas. They then focus on the synoptic component to define a predominant transport region or airshed for each site.  相似文献   

3.
A spatially and temporally resolved biogenic hydrocarbon and nitrogen oxides (NOx) emissions inventory has been developed for a region along the Mexico-U.S. border area. Average daily biogenic non-methane organic gases (NMOG) emissions for the 1700 x 1000 km2 domain were estimated at 23,800 metric tons/day (62% from Mexico and 38% from the United States), and biogenic NOx was estimated at 1230 metric tons/day (54% from Mexico and 46% from the United States) for the July 18-20, 1993, ozone episode. The biogenic NMOG represented 74% of the total NMOG emissions, and biogenic NOx was 14% of the total NOx. The CIT photochemical airshed model was used to assess how biogenic emissions impact air quality. Predicted ground-level ozone increased by 5-10 ppb in most rural areas, 10-20 ppb near urban centers, and 20-30 ppb immediately downwind of the urban centers compared to simulations in which only anthropogenic emissions were used. A sensitivity analysis of predicted ozone concentration to emissions was performed using the decoupled direct method for three dimensional air quality models (DDM-3D). The highest positive sensitivity of ground-level ozone concentration to biogenic volatile organic compound (VOC) emissions (i.e., increasing biogenic VOC emissions results in increasing ozone concentrations) was predicted to be in locations with high NOx levels, (i.e., the urban areas). One urban center--Houston--was predicted to have a slight negative sensitivity to biogenic NO emissions (i.e., increasing biogenic NO emissions results in decreasing local ozone concentrations). The highest sensitivities of ozone concentrations to on-road mobile source VOC emissions, all positive, were mainly in the urban areas. The highest sensitivities of ozone concentrations to on-road mobile source NOx emissions were predicted in both urban (either positive or negative sensitivities) and rural (positive sensitivities) locations.  相似文献   

4.
Because of climatic reasons and of reduced concentrations of SO2, ground-level ozone (O3) is one of the main air pollutants in Southern Europe. Ozone levels are very high both in rural and urban locations. In the cities, O3 can affect human health and materials. Regarding materials, most relevant is the exposure to pollutants of cultural heritage buildings. In particular, monuments registered on UNESCO's list of the world heritage require special monitoring. In Italy 34% and 97% of the territory is exposed to corrosion risk higher than the tolerable level for limestone and copper, respectively. The tolerable corrosion level for limestone and copper was also exceeded in the central area of Milan. In this area the tolerable O3 concentration for copper was calculated. These concentrations (ranging between 30 and 40 μg/m3) cannot be exceeded at unchanged concentration of other pollutants to maintain corrosion levels below the tolerable ones.  相似文献   

5.
This paper presents the temporal variation in surface-level ozone (O3) measured at Gummidipoondi near Chennai, Tamilnadu. The site chosen for the present study has high potential for ozone generation sources, such as vehicular traffic and industrial activities. The site is also located near a hazardous waste management facility. The key sources of nitrogen oxides (NOx), which are considered to be an important precursor of O3, include hazardous waste incineration, trucks bringing the hazardous wastes, and vehicles plying on the nearby National Highway 16 (NH 16). The measurements clearly showed diurnal variation, with maximum values observed during the noon hours and minimum values observed when solar radiation was less. The data showed a marked seasonal variation in O3, with the highest hourly average O3 concentration (497.2 µg/m3) in the summer season. Consequently, in order to identify the long-range transport sources adding to the increased O3 levels, backward trajectories were computed using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. It was found that the polluted air mass originated from the Southeast Asian region and the Indo-Gangetic Plain. The polluted air mass, which advected large amounts of carbon monoxide (CO) plumes, was analyzed using the Measurement of Pollution in the Troposphere (MOPITT) retrievals. The correlations of O3 with temperature (r = 0.746; P < 0.01) and solar radiation (r = 0.751; P < 0.01) were strongly positive, and that with NOx was found to be negative. Stronger correlation of O3 with NOx was observed during pre-monsoon months (r = 0.627; P < 0.01) and following hours of photochemical reactions. There were substantial differences in concentrations between weekdays and weekends, with higher nitric oxide (NO) and nitrogen dioxide (NO2), but lower O3, concentrations on weekdays. A substantial weekday-weekend difference in O3, which was higher on weekends, appears to be attributable to lower daytime traffic activity and hence reduced emissions of NOx to a “NOx-saturated” atmosphere.

Implications: The assessment of ground-level ozone in an industrial area with hazardous waste management facility is very important, as there is high possibility for more generation of tropospheric ozone. Since the location of the study area is coastal, wind plays a major role in O3 transportation; hence, the effects of wind speed and wind direction have been studied in different seasons. When compared with the other studies carried out in different places across India, the present study area has recorded much greater O3 mixing ratio. This study can be useful for setting up control strategies in such industrial areas.  相似文献   

6.
Ozone measurements made from 5 sites in Hong Kong have been analyzed, including those from one upwind, one downwind, and three urban locales. The data are analyzed in terms of the seasonal and diurnal trends. A subset of data in autumn is further analyzed to study the relationship between the ozone spatial pattern and wind flow as well as other meteorological parameters. The results show that averaged ozone levels at most sites exhibit maxima in autumn, which appears to be a unique feature for eastern Asia. On average the daily maximum 1-h concentrations are found to be higher in the western (normally downwind) site than those on the eastern side and in urban areas. Examination of surface wind patterns and other meteorological parameters suggest that elevated ozone concentrations on the western side occur during the days with intense solar radiation, light winds, and in the presence of a unique wind circulation. The wind reversal in the western parts under the “convergence” flow is believed to be an important cause of the high-ozone events observed there. Such wind flow may re-circulate/transport nearby urban plumes (in this case the Hong Kong–Shenzhen urban complex). Examination of chemical data from the western site has shown that averaged afternoon SO2 to NOx ratios on days with wind reversal are larger than those of typical urban Hong Kong and that a significant SO2 enhancement was clearly indicated on several occasions. The SO2 enhancement may be interpreted as being the evidence to suggest the contribution of regional sources and/or Hong Kong’s power plants (both containing high SO2). A case study has shown that when moderately strong northwesterly wind prevails, elevated ozone and SO2 can be transported to western Hong Kong from the inner Pearl Delta region. This study has also indicated that under the impact of ENE winds the eastern side of Hong Kong is not frequently affected by the re-circulating ozone plumes present in the western side.  相似文献   

7.
The combined action of urbanization (change in land use) and increase in vehicular emissions intensifies the urban heat island (UHI) effect in many cities in the developed countries. The urban warming (UHI) enhances heat-stress-related diseases and ozone (O3) levels due to a photochemical reaction. Even though UHI intensity depends on wind speed, wind direction, and solar flux, the thermodynamic properties of surface materials can accelerate the temperature profiles at the local scale. This mechanism modifies the atmospheric boundary layer (ABL) structure and mixing height in urban regions. These changes further deteriorate the local air quality. In this work, an attempt has been made to understand the interrelationship between air pollution and UHI intensity at selected urban areas located at tropical environment. The characteristics of ambient temperature profiles associated with land use changes in the different microenvironments of Chennai city were simulated using the Envi-Met model. The simulated surface 24-hr average air temperatures (11 m above the ground) for urban background and commercial and residential sites were found to be 30.81 ± 2.06, 31.51 ± 1.87, and 31.33 ± 2.1ºC, respectively. The diurnal variation of UHI intensity was determined by comparing the daytime average air temperatures to the diurnal air temperature for different wind velocity conditions. From the model simulations, we found that wind speed of 0.2 to 5 m/sec aggravates the UHI intensity. Further, the diurnal variation of mixing height was also estimated at the study locations. The estimated lowest mixing height at the residential area was found to be 60 m in the middle of night. During the same period, highest ozone (O3) concentrations were also recorded at the continuous ambient air quality monitoring station (CAAQMS) located at the residential area.

Implications: An attempt has made to study the diurnal variation of secondary pollution levels in different study regions. This paper focuses mainly on the UHI intensity variations with respect to percentage of land use pattern change in Chennai city, India. The study simulated the area-based land use pattern with local mixing height variations. The relationship between UHI intensity and mixing height provides variations on local air quality.  相似文献   


8.
Abstract

Meteorologically adjusted ozone (O3) concentrations during five recent O3 seasons (1998-2002) were computed for six Kentucky metro areas using a nonlinear regression model originally developed for forecasting ground-level O3 concentrations. The meteorological adjustment procedure was based on modifying actual measured O3 concentrations according to model-predicted responses to climate departures with respect to a reference year. For all six Kentucky metro areas, meteorologically adjusted O3 concentrations declined over the five-year period. The linear best-fit rate of decline in mean adjusted O3 concentrations ranged from 0.9 to 2.6 ppb/yr for these metro areas; the average rate of decline was 1.6 ppb/yr. The rates of decline in meteorologically adjusted extreme value (e.g., 95th percentile) concentrations were approximately the same, but there is greater statistical uncertainty concerning the extreme value trends.  相似文献   

9.
Possible effects of climate change on air quality are studied for two urban sites in the UK, London and Glasgow. Hourly meteorological data were obtained from climate simulations for two periods representing the current climate and a plausible late 21st century climate. Of the meteorological quantities relevant to air quality, significant changes were found in temperature, specific humidity, wind speed, wind direction, cloud cover, solar radiation, surface sensible heat flux and precipitation. Using these data, dispersion estimates were made for a variety of single sources and some significant changes in environmental impact were found in the future climate. In addition, estimates for future background concentrations of NOx, NO2, ozone and PM10 upwind of London and Glasgow were made using the meteorological data in a statistical model. These showed falls in NOx and increases in ozone for London, while a fall in NO2 was the largest percentage change for Glasgow. Other changes were small. With these background estimates, annual-average concentrations of NOx, NO2, ozone and PM10 were estimated within the two urban areas. For London, results averaged over a number of sites showed a fall in NOx and a rise in ozone, but only small changes in NO2 and PM10. For Glasgow, the changes in all four chemical species were small. Large-scale background ozone values from a global chemical transport model are also presented. These show a decrease in background ozone due to climate change. To assess the net impact of both large scale and local processes will require models which treat all relevant scales.  相似文献   

10.
Combustion emissions and strong Santa Ana winds had pronounced effects on patterns and levels of ambient ozone (O3) in southern California during the extensive wildland fires of October 2007. These changes are described in detail for a rural receptor site, the Santa Margarita Ecological Reserve, located among large fires in San Diego and Orange counties. In addition, O3 changes are also described for several other air quality monitoring sites in the general area of the fires. During the first phase of the fires, strong, dry and hot northeasterly Santa Ana winds brought into the area clean continental air masses, which resulted in minimal diurnal O3 fluctuations and a 72-h average concentration of 36.8 ppb. During the second phase of the fires, without Santa Ana winds present and air filled with smoke, daytime O3 concentrations steadily increased and reached 95.2 ppb while the lowest nighttime levels returned to ~0 ppb. During that period the 8-h daytime average O3 concentration reached 78.3 ppb, which exceeded the federal standard of 75 ppb. After six days of fires, O3 diurnal concentrations returned to pre-fire patterns and levels.  相似文献   

11.
Ozone Transport     
Elevated concentrations of ozone, often above the national ambient air quality standard for photochemical oxidants, have been measured in both urban and rural areas of Connecticut. One such episode took place on June 10, 1974. Ozone levels, after stabilizing at values slightly above the standard (i.e., 80 to 110 ppb; Connecticut generated ozone concentrations), rose sharply late in the afternoon reaching concentrations as high as 310 ppb (almost 4 times the standard) in Hartford. The trajectory of the air mass, which arrived in Hartford at the time of maximum O3 occurence, had its origin in the metropolitan New York area during the early morning rush hour on the episode day. This illustrates that the advective transport of O3 and O3 precursors into Connecticut from New York are probably responsible for a significant portion (approximately two-thirds) of the elevated O3 concentrations measured throughout Connecticut on days when winds are from the south-southwest direction. The fact that peak O3 levels occur late in the afternoon, several hours after maximum sunlight intensity, reinforces the conclusion that excessive O3 concentrations developed as O3 and ozone precursors were generated in the vicinity of New York City and then drifted inland into Connecticut on the afternoon sea breeze.

It appears to be unrealistic to develop a hydrocarbon control strategy for Connecticut in order to meet the photochemical oxidant ambient air quality standard when O3 and/or ozone precursors ad-vectively transported into the State cause oxidant levels to exceed the standard. The complete cessation of all anthropogenic hydrocarbon emissions in Connecticut would not necessarily assure that the standard would be attained here. The implication is that a regional (i.e., the eastern part of the United States) hydrocarbon control strategy is needed to reduce adequately ozone formation and transport so as to allow Connecticut to meet the current oxidant standard.  相似文献   

12.
The aim of this study was to identify areas of potential relevant exposure to pollutants within Rome's urban core. To meet this goal, intensive field campaigns were conducted and simulations were performed, using the flexible air quality regional model (FARM), to study winter and summer pollution episodes. The simulations were performed using a complete emission inventory that included traffic flow model results of the Roman street network to better describe, with respect to the available diffuse national emission inventory, the hourly variation of traffic emissions in the city. The meteorological reconstruction was performed by means of both prognostic and diagnostic models by using experimental data collected during the field campaigns. To evaluate the capability of the FARM model to capture the main features of the selected episodes, a comparison of modelled results against observed air quality data for different pollutants was performed at urban and rural sites. FARM performed well in predicting ozone (O3) and nitrogen dioxide (NO2) concentrations, showing a good reproduction of both daily peaks and their diurnal variations. The model also showed a good capability to reproduce the magnitude of volatile alkane, aromatic and carbonyl compound concentrations. PM10 model results revealed the tendency to under-predict the observed values. PM composition model results were compared with observed data, evidencing good results for elemental carbon (EC), nitrate (NO3) and ammonium (NH4+), underestimation for sulphate (SO42−) and poor performance for organic matter (OM). The soil components of PM were found to be significantly under-predicted by the model, especially during Saharan dust episodes. Overall, the study results show large areas of high O3 and PM10 concentrations where levels of pollutants should be carefully monitored and population exposure evaluated.  相似文献   

13.
Land use and pollutant emission changes can have significant impacts on air quality, regional climate, and human health. Here we describe a modeling study aimed at quantifying the potential effects of extensive changes in urban land cover in the New York City (NYC), USA metropolitan region on surface meteorology and ozone (O3) concentrations. The SLEUTH land-use change model was used to extrapolate urban land cover over this region from “present-day” (ca. 1990) conditions to a future year (ca. 2050), and these projections were subsequently integrated into meteorological and air quality simulations. The development of the future-year land-use scenario followed the narrative of the “A2” scenario described by the Intergovernmental Panel on Climate Change (IPCC), but was restricted to the greater NYC area. The modeling system consists of the Penn State/NCAR MM5 mesoscale meteorological model; the Sparse Matrix Operator Kernal Emissions processing system; and the US EPA Community Multiscale Air Quality model, and simulations were performed for two 18-day episodes, one near-past and one future. Our results suggest that extensive urban growth in the NYC metropolitan area has the potential to increase afternoon near-surface temperatures by more than 0.6 °C and planetary boundary layer (PBL) heights by more than 150 m, as well as decrease water vapor mixing ratio by more than 0.6 g kg−1, across the NYC metropolitan area, with the areal extent of all of these changes generally coinciding with the area of increased urbanization. On the other hand, the impacts of these land use changes on ozone concentrations are more complex. Simulation results indicate that future changes in urbanization, with emissions held constant, may lead to increases in episode-average O3 levels by about 1–5 ppb, and episode-maximum 8 h O3 levels by more than 6 ppb across much of the NYC area. However, spatial patterns of ozone changes are heterogeneous and also indicate the presence of areas with decreasing ozone concentrations. When anthropogenic emissions were increased to be consistent with the extensive urbanization in the greater NYC area, the O3 levels increased in outer counties of the metropolitan region but decreased in others, including coastal Connecticut and the Long Island Sound area.  相似文献   

14.
Air quality impacts of volatile organic compound (VOC) and nitrogen oxide (NOx) emissions from major sources over the northwestern United States are simulated. The comprehensive nested modeling system comprises three models: Community Multiscale Air Quality (CMAQ), Weather Research and Forecasting (WRF), and Sparse Matrix Operator Kernel Emissions (SMOKE). In addition, the decoupled direct method in three dimensions (DDM-3D) is used to determine the sensitivities of pollutant concentrations to changes in precursor emissions during a severe smog episode in July of 2006. The average simulated 8-hr daily maximum O3 concentration is 48.9 ppb, with 1-hr O3 maxima up to 106 ppb (40 km southeast of Seattle). The average simulated PM2.5 (particulate matter with an aerodynamic diameter <2.5 μm) concentration at the measurement sites is 9.06 μg m?3, which is in good agreement with the observed concentration (8.06 μg m?3). In urban areas (i.e., Seattle, Vancouver, etc.), the model predicts that, on average, a reduction of NOx emissions is simulated to lead to an increase in average 8-hr daily maximum O3 concentrations, and will be most prominent in Seattle (where the greatest sensitivity is??0.2 ppb per % change of mobile sources). On the other hand, decreasing NOx emissions is simulated to decrease the 8-hr maximum O3 concentrations in remote and forested areas. Decreased NOx emissions are simulated to slightly increase PM2.5 in major urban areas. In urban areas, a decrease in VOC emissions will result in a decrease of 8-hr maximum O3 concentrations. The impact of decreased VOC emissions from biogenic, mobile, nonroad, and area sources on average 8-hr daily maximum O3 concentrations is up to 0.05 ppb decrease per % of emission change, each. Decreased emissions of VOCs decrease average PM2.5 concentrations in the entire modeling domain. In major cities, PM2.5 concentrations are more sensitive to emissions of VOCs from biogenic sources than other sources of VOCs. These results can be used to interpret the effectiveness of VOC or NOx controls over pollutant concentrations, especially for localities that may exceed National Ambient Air Quality Standards (NAAQS).

Implications: The effect of NOx and VOC controls on ozone and PM2.5 concentrations in the northwestern United States is examined using the decoupled direct method in three dimensions (DDM-3D) in a state-of-the-art three-dimensional chemical transport model (CMAQ). NOx controls are predicted to increase PM2.5 and ozone in major urban areas and decrease ozone in more remote and forested areas. VOC reductions are helpful in reducing ozone and PM2.5 concentrations in urban areas. Biogenic VOC sources have the largest impact on O3 and PM2.5 concentrations.  相似文献   

15.
An experimental study on the formation and transport of ozone in ambient air was performed in Tenerife (Canary Islands) in order to investigate the processes affecting ozone levels and air quality. The special features of Tenerife (prevalence of the trade wind pattern (NE), orography and the specific location of the local ozone sources) permit to quantify the role of the ‘long-range transport from northern latitudes' versus the ‘formation and transport of ozone downwind of the main urban areas' of Tenerife. Levels of O3, NO2 and OX were monitored in different types of environments to achieve this purpose. The results showed that: (1) upwind of the urban areas ozone is mainly transported from the ocean by trade winds, (2) local ozone titration (by NO) and ozone replenishment from the ocean are the main causes of ozone variations in urban and suburban areas, and (3) photochemical ozone production occurs downwind of the urban areas. Photochemical production causes daylight O3 and OX levels downwind of urban areas to be frequently (60% and 35% days/year, respectively) higher than upwind of the urban sites (O3 and OX excess frequently in the range 5–20 ppbv). Due to the above processes, different daily ozone cycles occur in short distances (<30 km), with maximum O3 levels during daylight or night depending on the site. Ozone phytotoxicity was assessed by calculating the AOT40 index upwind and downwind of the main urban areas. The critical value for the 5-day-AOT40 index was simultaneously exceeded at the two sites (few times/year) during long-range transport events. During the additional exceedances of the critical value downwind of the urban area, relatively high 5-day-AOT40 values were recorded upwind of the urban site. Thus, long-range transport from northern latitudes may produce relatively high 5-days-AOT40 levels in the oceanic boundary layer. These results are important for the protection of the large number of endemic plants in the Canaries. The conceptual model discussed in this study may be qualitatively applied to other islands which possess features similar to those of Tenerife.  相似文献   

16.
This paper summarizes the results of a yearlong continuous measurements of gaseous pollutants, NO, NO2, NOx and O3 in the ambient air at Kathmandu valley. Measured concentration of the pollutants in study area is a function of time. NO, NO2 and O3 peak occurred in succession in presence of sunlight. At the time of maximum O3 concentration most of the NOx are utilized. The diurnal cycle of ground level ozone concentrations, revealed mid-day peak with lower nocturnal concentrations and inverse relationship exists between O3 and NOx, which are evidences of photochemical O3 formation. The observed ground level ozone during monsoon is slight lower than the pre-monsoon value. Further, lack of rainfall and higher temperature, solar radiation in the pre-monsoon have given rise to the gradual build up of ozone and it is lowest during winter. Ground level ozone concentrations measured during bandha (general strike) and weekend are 19% and 13% higher than those measured during weekdays. The most effective ozone abatement strategy for Kathmandu Valley may be control of NOx emissions.  相似文献   

17.
In the frame of a European research project on air quality in urban agglomerations, data on ozone concentrations from 23 automated urban and suburban monitoring stations in 11 cities from seven countries were analysed and evaluated. Daily and summer mean and maximum concentrations were computed based on hourly mean values, and cumulative ozone exposure indices (Accumulated exposure Over a Threshold of 40 ppb (AOT40), AOT20) were calculated. The diurnal profiles showed a characteristic pattern in most city centres, with minimum values in the early morning hours, a strong rise during the morning, peak concentrations in the afternoon, and a decline during the night. The widest amplitudes between minimum and maximum values were found in central and southern European cities such as Düsseldorf, Verona, Klagenfurt, Lyon or Barcelona. In the northern European cities of Edinburgh and Copenhagen, by contrast, maximum values were lower and diurnal variation was much smaller. Based on ozone concentrations as well as on cumulative exposure indices, a clear north–south gradient in ozone pollution, with increasing levels from northern and northwestern sites to central and southern European sites, was observed. Only the Spanish cities did not fit this pattern; there, ozone levels were again lower than in central European cities, probably due to the direct influence of strong car traffic emissions. In general, ozone concentrations and cumulative exposure were significantly higher at suburban sites than at urban and traffic-exposed sites. When applying the newly established European Union (EU) Directive on ozone pollution in ambient air, it was demonstrated that the target value for the protection of human health was regularly surpassed at urban as well as suburban sites, particularly in cities in Austria, France, northern Italy and southern Germany. European target values and long-term objectives for the protection of vegetation expressed as AOT40 were also exceeded at many monitoring sites.  相似文献   

18.
During the summer of 1976, a comparison was made between ozone measurements for a coastal industrial concentration area (Norfolk/Virginia Beach, Virginia) and an offshore station (Chesapeake Light Station, 15 miles out to sea). The anticipated dominance of high offshore ozone readings with offshore flow was not observed. A surprising number of high O3 concentrations were observed at both the offshore and land sites with northeasterly and easterly winds. This suggests that the phenomenon of long range transport of contaminants from highly urbanized centers in the northeast to the mid-Atlantic states via an offshore sea route must be given careful consideration. The body of information presented in this paper points out the need for a clearer understanding of the complex urban/rural O3 problem coupled with transport effects before costly control strategies are to be implemented.  相似文献   

19.
Reduced sulfur compounds (RSCs) such as carbonyl sulfide (OCS), dimethyl sulfide (DMS) and carbon disulfide (CS2) impact radiative forcing, ozone depletion, and acid rain. Although Asia is a large source of these compounds, until now a long-term study of their emission patterns has not been carried out. Here we analyze 16 months of RSC data measured at a polluted rural/coastal site in the greater Pearl River Delta (PRD) of southern China. A total of 188 canister air samples were collected from August 2001 to December 2002. The OCS and CS2 mixing ratios within these samples were higher in autumn/winter and lower in summer due to the influence of Asian monsoon circulations. Comparatively low DMS values observed in this coastal region suggest a relatively low biological productivity during summer months. The springtime OCS levels in the study region (574 ± 40 pptv) were 25% higher than those on other East Asia coasts such Japan, whereas the springtime CS2 and DMS mixing ratios in the PRD (47 ± 38 pptv and 22 ± 5 pptv, respectively) were 3–30 times lower than elevated values that have been measured elsewhere in East Asia (Japan and Korea) at this time of year. Poor correlations were found among the three RSCs in the whole group of 188 samples, suggesting their complex and variable sources in the region. By means of backward Lagrangian particle release simulations, air samples originating from the inner PRD, urban Hong Kong and South China Sea were identified. The mean mixing ratio of OCS in the inner PRD was significantly higher than that in Hong Kong urban air and South China Sea marine air (p < 0.001), whereas no statistical differences were found for DMS and CS2 among the three regions (p > 0.05). Using a linear regression method based on correlations with the urban tracer CO, the estimated OCS emission in inner PRD (49.6 ± 4.7 Gg yr?1) was much higher than that in Hong Kong (0.32 ± 0.05 Gg yr?1), whereas the estimated CS2 and DMS emissions in the study region accounted for a very few percentage of the total CS2 and DMS emission in China. These findings lay the foundation for better understanding sulfur chemistry in the greater PRD region of southern China.  相似文献   

20.
Tropospheric ozone concentrations regarded as harmful for human health are frequently encountered in Central Europe in summertime. Although ozone formation generally results from precursors transported over long distances, in urban areas local effects, such as reactions due to nearby emission sources, play a major role in determining ozone concentrations. Europe-wide mapping and modeling of population exposure to high ozone concentrations is subject to many uncertainties, because small-scale phenomena in urban areas can significantly change ozone levels from those of the surroundings. Currently the integrated assessment modeling of European ozone control strategies is done utilizing the results of large-scale models intended for estimating the rural background ozone levels. This paper presents an initial study on how much local nitrogen oxide (NOx) concentrations can explain variations between large-scale ozone model results and urban ozone measurements, on one hand, and between urban and nearby rural measurements, on the other. The impact of urban NOx concentrations on ozone levels was derived from chemical equations describing the ozone balance. The study investigated the applicability of the method for improving the accuracy of modeled population exposure, which is needed for efficient control strategy development. The method was tested with NOx and ozone measurements from both urban and rural areas in Switzerland and with the ozone predictions of the large-scale photochemical model currently used in designing Europe-wide control strategies for ground-level ozone. The results suggest that urban NOx levels are a significant explanatory factor in differences between urban and nearby rural ozone concentrations and that the phenomenon could be satisfactorily represented with this kind of method. Further research efforts should comprise testing of the method in more locations and analyzing the performance of more widely applicable ways of deriving the initial parameters.  相似文献   

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