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1.
Abstract

A computer model called the Ozone Risk Assessment Model (ORAM) was developed to evaluate the health effects caused by ground-level ozone (O3) exposure. ORAM was coupled with the U.S. Environmental Protection Agency’s (EPA) Third-Generation Community Multiscale Air Quality model (Models-3/CMAQ), the state-of-the-art air quality model that predicts O3 concentration and allows the examination of various scenarios in which emission rates of O3 precursors (basically, oxides of nitrogen [NOx] and volatile organic compounds) are varied. The principal analyses in ORAM are exposure model performance evaluation, health-effects calculations (expected number of respiratory hospital admissions), economic valuation, and sensitivity and uncertainty analysis through a Monte Carlo simulation. As a demonstration of the system, ORAM was applied to the eastern Tennessee region, and the entire O3 season was simulated for a base case (typical emissions) and three different emission scenarios. The results indicated that a synergism occurs when reductions in NOx emissions from mobile and point sources were applied simultaneously. A 12.9% reduction in asthma hospital admissions is expected when both mobile and point source NOx emissions are reduced (50 and 70%, respectively) versus a 5.8% reduction caused by mobile source and a 3.5% reduction caused by point sources when these emission sources are reduced individually.  相似文献   

2.
Ambient O3 concentrations in California's South Coast Air Basin (SoCAB) can be as much as 55% higher on weekends than on weekdays under comparable meteorological conditions. This is paradoxical because emissions of O3 precursors (hydrocarbons, CO, and nitrogen oxides [NOx]) are lower on weekends. Day-of-week emissions activity data were collected and analyzed to investigate the hypothesized causes of the "weekend O3 effect." Emission activity data were collected for various mobile, area, and point sources throughout the SoCAB, including on-road vehicles, lawn and garden equipment, barbecues, fireplaces, solvent use, and point sources with continuous emission monitoring data. The results of this study indicate significant differences between weekday and weekend emission activity patterns and emissions. Their combined effect results in a 12-18% decrease in reactive organic gases (ROGs) and a 35-41% decrease in NOx emissions on Saturdays and Sundays, respectively, relative to weekdays in summer 2000. These changes in emissions result in an increase of more than 30% in the ROG/NOx ratio on weekends compared with weekdays, which, along with lower NOx emissions, leads to increased O3 production on weekends.  相似文献   

3.
The location of the northeastern Iberian Peninsula (NEIP) in the northwestern Mediterranean basin, the presence of the Pyrenees mountain range (with altitudes > 3000 m), and the influence of the Mediterranean Sea and the large valley canalization of Ebro river induce an extremely complicated structure for the dispersion of photochemical pollutants. Air pollution studies in very complex terrains such as the NEIP require high-resolution modeling for resolving the very complex dynamics of flows. To deal with the influence of larger-scale transport, however, high-resolution models have to be nested in larger models to generate appropriate initial and boundary conditions for the finer resolution domains. This article shows the results obtained through the utilization of the MM5-EMICAT2000-CMAQ multiscale-nested air quality model relating the sensitivity regimes for ozone (O3)-nitrogen oxides (NOx)-volatile organic compounds (VOCs) in an area of high geographical complexity, like the industrial area of Tarragona, located in the NEIP. The model was applied with fine temporal (one-hour) and spatial resolution (cells of 24 km, 2 km, and 1 km) to represent the chemistry and transport of tropospheric O3 and other photochemical species with respect to different hypothetical scenarios of emission controls and to quantify the influence of different emission sources in the area. Results indicate that O3 chemistry in the industrial domain of Tarragona is strongly sensitive to VOCs; the higher percentages of reduction for ground-level O3 are achieved when reducing by 25% the emissions of industrial VOCs. On the contrary, reductions in the industrial emissions of NOx contribute to a strong increase in hourly peak levels of O3. At the same time, the contribution of on-road traffic and biogenic emissions to ground-level O3 concentrations in the area is negligible with respect to the pervasive weight of industrial sources. This analysis provides an assessment of the effectiveness of different policies for the control of emission of precursors by comparing the modeled results for different scenarios.  相似文献   

4.
A photochemical smog model system, the Variable-Grid Urban Airshed Model/Systems Applications International Mesoscale Model (UAM-V/SAIMM), was used to investigate photochemical pollution in the Bangkok Metropolitan Region (BMR). The model system was first applied to simulate a historical photochemical smog episode of two days (January 13-14, 1997) using the 1997 anthropogenic emission database available at the Pollution Control Department and an estimated biogenic emission. The output 1-hr ozone (O3) for BMR, however, did not meet the U.S. Environmental Protection Agency suggested performance criteria. The simulated minimum and maximum O3 values in the domain were much higher than the observations. Multiple model runs with different precursor emission reduction scenarios showed that the best model performance with the simulated 1-hr O3 meeting all the criteria was obtained when the volatile organic compound (VOC) and oxides of nitrogen (NOx) emission from mobile source reduced by 50% and carbon monoxide by 20% from the original database. Various combinations of anthropogenic and biogenic emissions in Bangkok and surrounding provinces were simulated to assess the contribution of different sources to O3 pollution in the city. O3 formation in Bangkok was found to be more VOC-sensitive than NOx-sensitive. To attain the Thailand ambient air quality standard for 1-hr O3 of 100 ppb, VOC emission in BMR should be reduced by 50-60%. Management strategies considered in the scenario study consist of Stage I, Stage II vapor control, replacement of two-stroke by four-stroke motorcycles, 100% compressed natural gas bus, 100% natural gas-fired power plants, and replacement of methyltertiarybutylether by ethanol as an additive for gasoline.  相似文献   

5.
The purpose of this investigation was to quantify the potential of natural gas to reduce emissions from stationary combustion sources by analyzing the case study of the metropolitan region of Santiago, Chile. For such purposes, referential base scenarios have been defined that represent with and without natural gas settings. The method to be applied is an emission estimate based on emission factors. The results for this case study reveal that stationary combustion sources that replaced their fuel reduced particulate matter (PM) emissions by 61%, sulfur oxides (SOx) by 91%, nitrogen oxides (NOx) by 40%, and volatile organic compounds (VOC) by 10%. Carbon monoxide (CO) emissions were reduced by 1%. As a result of this emission reduction, in addition to reductions caused by other factors, such as a shift to cleaner fuels other than natural gas, technological improvements, and sources which are not operative, emission reduction goals set forth by the environmental authorities were broadly exceeded.  相似文献   

6.
In this paper, we examine the changes in ambient ozone concentrations simulated by the Community Multiscale Air Quality (CMAQ) model for summer 2002 under three different nitrogen oxides (NOx) emission scenarios. Two emission scenarios represent best estimates of 2002 and 2004 emissions; they allow assessment of the impact of the NOx emissions reductions imposed on the utility sector by the NOx State Implementation Plan (SIP) Call. The third scenario represents a hypothetical rendering of what NOx emissions would have been in 2002 if no emission controls had been imposed on the utility sector. Examination of the modeled median and 95th percentile daily maximum 8-hr average ozone concentrations reveals that median ozone levels estimated for the 2004 emission scenario were less than those modeled for 2002 in the region most affected by the NOx SIP Call. Comparison of the "no-control" with the "2002" scenario revealed that ozone concentrations would have been much higher in much of the eastern United States if the utility sector had not implemented NOx emission controls; exceptions occurred in the immediate vicinity of major point sources where increased NO titration tends to lower ozone levels.  相似文献   

7.
Two photochemical smog modeling systems, UAM-V/ SAIMM (the Variable-Grid UAM/Systems Applications International Mesoscale Model) and CHIMERE/ECMWF (European Center for Medium Range Weather Forecast), are applied to the same tropical domain (Bangkok Metropolitan Region) and the same episode (January 13-14, 1997) to evaluate their relative performance using the same anthropogenic emission database (emission database available at the Pollution Control Department [PCD] 1997). Ozone (O3) produced by both models meets U.S. Environment Protection Agency (EPA) suggested prediction criteria of mean normalized bias error and mean normalized gross error on January 14 but none on January 13. Both models are tested with various modified databases of precursors emissions from the PCD original database. Performance of UAM-V is the best when using the modified emission data with volatile organic compound (VOC), NOx, and CO mobile source emission reduced by 50%, 50%, and 20% from the original database. CHIMERE suggests a similar emission database except for the VOC emission, which is a reduction by 40% from the original PCD mobile source emission. Spatial and temporal variations of O3, CO, NOy (total reactive nitrogen), and Ox (NO2+O3) predicted by both model systems using the modified  相似文献   

8.
The spatial distributions of sulphur dioxide (SO2) and nitrogen oxides (NOx) emissions are essential inputs to models of atmospheric transport and deposition. Information of this type is required for international negotiations on emission reduction through the critical load approach. High-resolution emission maps for the Republic of Ireland have been created using emission totals and a geographical information system, supported by surrogate statistics and landcover information. Data have been subsequently allocated to the EMEP 50 x 50-km grid, used in long-range transport models for the investigation of transboundary air pollution. Approximately two-thirds of SO2 emissions in Ireland emanate from two grid-squares. Over 50% of total SO2 emissions originate from one grid-square in the west of Ireland, where the largest point sources of SO2 are located. Approximately 15% of the total SO2 emissions originate from the grid-square containing Dublin. SO2 emission densities for the remaining areas are very low, < 1 t km-2 year-1 for most grid-squares. NOx emissions show a very similar distribution pattern. However, NOx emissions are more evenly spread over the country, as about 40% of total NOx emissions originate from road transport.  相似文献   

9.
The recorded exceedances of the 24-hr PM10 National Ambient Air Quality Standard (NAAQS) in Treasure Valley, Idaho, have been associated with prolonged stagnation periods during the winter. A comprehensive modeling study of PM10 impact in Treasure Valley was performed to support the State Implementation Plan (SIP). The study included base-year and short-term episodic conditions. The ISCST3 (Industrial Source Complex Short Term 3) model, using the base-year meteorology and gridded emissions of mobile sources, point sources, and wood burning as input, generally agreed well with measurements in both temporal patterns and annual averages. The WYNDvalley model was evaluated using monitoring data and was used to simulate the PM10 impact for episodic exceedances during stagnant winter conditions. An emission inventory was prepared for a base year (1995) and then extrapolated to the years 2000, 2005, 2010, and 2015 in order to determine air quality planning requirements. According to the simulations using base-year emissions and meteorology, exceedances are not expected. However, exceedances at some stations could be expected using projected emissions and episodic meteorology. Results from emission control strategies we developed indicate that mobile-source emissions have the most significant impact; reduction of 25% would be needed to eliminate the simulated exceedances in all projected years.  相似文献   

10.
Numerous studies of ambient ozone (O3) in the Los Angeles (LA) area have found both increases and decreases in elevated O3 levels on weekends, depending on location and year. Since the mid-1990s, average daily maximum O3 levels have been higher on weekends than on weekdays throughout most of the area. We used the Comprehensive Air-Quality Model with extensions to investigate causes of weekday/weekend O3 differences in the LA area for August 3-7, 1997, from the Southern California Ozone Study. Weekday/weekend emission changes were estimated, because explicit weekend inventories are not yet available from regulatory agencies. Changes to on-road motor vehicle (MV) emissions were derived from observed weekday/weekend traffic differences. The estimated changes in MV emissions of nitrogen oxides (NOx) were a 5% increase on Friday, a 27% decrease on Saturday, and a 37% decrease on Sunday, relative to Monday-Thursday levels. The corresponding changes in MV volatile organic carbon (VOC) emissions were an 8% increase on Friday, an 8% decrease on Saturday, and a 15% decrease on Sunday. Modeling these MV emissions changes explained the observed weekend O3 effect very well. Furthermore, changes to the mass of MV NOx emissions were the main contributor to O3 differences rather than changes to the timing of MV emissions. Ozone increases on weekends were caused by NOx emission decreases, because O3 formation is strongly VOC-limited throughout most of the LA area.  相似文献   

11.
In this paper, the NOx emission scaling factors applied over the 2001 National Emissions Inventory (NEI) are estimated through a four-dimensional variational (4D-Var) approach using SCIAMACHY (Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY) tropospheric NO2 columns measured during summer 2004. In the “top-down” approach, two-month average NO2 columns are assimilated into a regional chemical transport model (CTM), STEM, using different assimilation setups. In a basic setup, NOx emissions are adjusted by assimilating the NO2 columns. A more general setup of emission inversion allows the initial O3 concentrations be adjusted along with the NOx emissions. A final case is set up to assimilate both the NO2 columns and O3 measurement from various platforms while allowing adjustments of both the NOx emissions and the initial O3 concentrations. It is found that the addition of O3 measurements did not improve the NOx emission inversion. With the NOx emission at surface and upper levels being adjusted separately, results from four cases show that the elevated NOx emission reduction ranges from 8.9% to 11.4%, and the surface NOx emission reduction is up to 6.6%. All the cases show NOx emission reduction in Ohio valley and Washington, District of Columbia areas.  相似文献   

12.
Emission trading is a market-based approach designed to improve the efficiency and economic viability of emission control programs; emission trading has typically been confined to trades among single pollutants. Interpollutant trading (IPT), as described in this work, allows for trades among emissions of different compounds that affect the same air quality end point, in this work, ambient ozone (O3) concentrations. Because emissions of different compounds impact air quality end points differently, weighting factors or trading ratios (tons of emissions of nitrogen oxides (NO(x)) equivalent to a ton of emissions of volatile organic compounds [VOCs]) must be developed to allow for IPT. In this work, IPT indices based on reductions in O3 concentrations and based on reductions in population exposures to O3 were developed and evaluated using a three-dimensional gridded photochemical model for Austin, TX, a city currently on the cusp of nonattainment with the National Ambient Air Quality Standards for O3 concentrations averaged over 8 hr. Emissions of VOC and NO(x) from area and mobile sources in Austin are larger than emissions from point sources. The analysis indicated that mobile and area sources exhibited similar impacts. Trading ratios based on maximum O3 concentration or population exposure were similar. In contrast, the trading ratios did exhibit significant (more than a factor of two) day-to-day variability. Analysis of the air quality modeling indicated that the daily variability in trading ratios could be attributed to daily variations in both emissions and meteorology.  相似文献   

13.
ABSTRACT

The recorded exceedances of the 24-hr PM10 National Ambient Air Quality Standard (NAAQS) in Treasure Valley, Idaho, have been associated with prolonged stagnation periods during the winter. A comprehensive modeling study of PM10 impact in Treasure Valley was performed to support the State Implementation Plan (SIP). The study included base-year and short-term episodic conditions. The ISCST3 (Industrial Source Complex Short Term 3) model, using the base-year meteorology and gridded emissions of mobile sources, point sources, and wood burning as input, generally agreed well with measurements in both temporal patterns and annual averages. The WYNDvalley model was evaluated using monitoring data and was used to simulate the PM10 impact for episodic exceedances during stagnant winter conditions. An emission inventory was prepared for a base year (1995) and then extrapolated to the years 2000, 2005, 2010, and 2015 in order to determine air quality planning requirements. According to the simulations using base-year emissions and meteorology, exceedances are not expected. However, exceedances at some stations could be expected using projected emissions and episodic meteorology. Results from emission control strategies we developed indicate that mobile-source emissions have the most significant impact; reduction of 25% would be needed to eliminate the simulated exceedances in all projected years.  相似文献   

14.
Regional estimates of both anthropogenic and biogenic emissions are important inputs for models of atmospheric chemistry. A disaggregated emissions inventory of all relevant pollutants for an area of 100 x 100 km2 centered in Burriana (Castellon, Spain) has been worked out. Time and spatial resolutions were hourly and 1 x 1 km2, respectively. Estimates were made for all relevant sources of anthropogenic emissions. The pollutants considered were SO2, NOx, NMVOCs (nonmethane volatile organic compounds), CH4, CO, CO2, N2O, and NH3. Thus, the emissions inventory includes up to 18 different NMVOCs. Emissions were computed for a typical sunny workday in June when strong photochemical activity could be expected. A "top-down" methodology was applied, taking as a starting point official annual and provincial estimates based on CORINAIR emission factors. This procedure is a very useful tool, particularly for those cases where a lack of sufficient local detailed information about the main emission-generating activities, such as road traffic, makes the use of a "bottom-up" approximation inadvisable. Moreover, updating these emission inventories is easier and they could be used to evaluate the impact of possible abatement strategies.  相似文献   

15.
For at least 30 years, ozone (O3) levels on weekends in parts of California's South Coast (Los Angeles) Air Basin (SoCAB) have been as high as or higher than on weekdays, even though ambient levels of O3 precursors are lower on weekends than on weekdays. A field study was conducted in the Los Angeles area during fall 2000 to test whether proposed relationships between emission sources and ambient nonmethane hydrocarbon (NMHC) and oxides of nitrogen (NOx) levels can account for observed diurnal and day-of-week variations in the concentration and proportions of precursor pollutants that may affect the efficiency and rate of O3 formation. The contributions to ambient NMHC by motor vehicle exhaust and evaporative emissions, estimated using chemical mass balance (CMB) receptor modeling, ranged from 65 to 85% with minimal day-of-week variation. Ratios of ambient NOx associated with black carbon (BC) to NOx associated with carbon monoxide (CO) were approximately 1.25 +/- 0.22 during weekdays and 0.76 +/- 0.07 and 0.52 +/- 0.07 on Saturday and Sunday, respectively. These results demonstrate that lower NOx emissions from diesel exhaust can be a major factor causing lower NOx mixing ratios and higher NMHC/NOx ratios on weekends. Nonmobile sources showed no significant day-of-week variations in their contributions to NMHC. Greater amounts of gasoline emissions are carried over on Friday and Saturday evenings but are, at most, a minor factor contributing to higher NMHC/NOx ratios on weekend mornings.  相似文献   

16.
A fuel-based assessment of off-road diesel engine emissions   总被引:1,自引:0,他引:1  
The use of diesel engines in off-road applications is a significant source of nitrogen oxides (NOx) and particulate matter (PM10). Such off-road applications include railroad locomotives, marine vessels, and equipment used for agriculture, construction, logging, and mining. Emissions from these sources are only beginning to be controlled. Due to the large number of these engines and their wide range of applications, total activity and emissions from these sources are uncertain. A method for estimating the emissions from off-road diesel engines based on the quantity of diesel fuel consumed is presented. Emission factors are normalized by fuel consumption, and total activity is estimated by the total fuel consumed. Total exhaust emissions from off-road diesel equipment (excluding locomotives and marine vessels) in the United States during 1996 have been estimated to be 1.2 x 10(9) kg NOx and 1.2 x 10(8) kg PM10. Emissions estimates published by the U.S. Environmental Protection Agency are 2.3 times higher for both NOx and exhaust PM10 emissions than estimates based directly on fuel consumption. These emissions estimates disagree mainly due to differences in activity estimates, rather than to differences in the emission factors. All current emission inventories for off-road engines are uncertain because of the limited in-use emissions testing that has been performed on these engines. Regional- and state-level breakdowns in diesel fuel consumption by off-road mobile sources are also presented. Taken together with on-road measurements of diesel engine emissions, results of this study suggest that in 1996, off-road diesel equipment (including agriculture, construction, logging, and mining equipment, but not locomotives or marine vessels) was responsible for 10% of mobile source NOx emissions nationally, whereas on-road diesel vehicles contributed 33%.  相似文献   

17.
Numerous emission and air quality modeling studies have suggested the need to accurately characterize the spatial and temporal variations in on-road vehicle emissions. The purpose of this study was to quantify the impact that using detailed traffic activity data has on emission estimates used to model air quality impacts. The on-road vehicle emissions are estimated by multiplying the vehicle miles traveled (VMT) by the fleet-average emission factors determined by road link and hour of day. Changes in the fraction of VMT from heavy-duty diesel vehicles (HDDVs) can have a significant impact on estimated fleet-average emissions because the emission factors for HDDV nitrogen oxides (NOx) and particulate matter (PM) are much higher than those for light-duty gas vehicles (LDGVs). Through detailed road link-level on-road vehicle emission modeling, this work investigated two scenarios for better characterizing mobile source emissions: (1) improved spatial and temporal variation of vehicle type fractions, and (2) use of Motor Vehicle Emission Simulator (MOVES2010) instead of MOBILE6 exhaust emission factors. Emissions were estimated for the Detroit and Atlanta metropolitan areas for summer and winter episodes. The VMT mix scenario demonstrated the importance of better characterizing HDDV activity by time of day, day of week, and road type. More HDDV activity occurs on restricted access road types on weekdays and at nonpeak times, compared to light-duty vehicles, resulting in 5-15% higher NOx and PM emission rates during the weekdays and 15-40% lower rates on weekend days. Use of MOVES2010 exhaust emission factors resulted in increases of more than 50% in NOx and PM for both HDDVs and LDGVs, relative to MOBILE6. Because LDGV PM emissions have been shown to increase with lower temperatures, the most dramatic increase from MOBILE6 to MOVES2010 emission rates occurred for PM2.5 from LDGVs that increased 500% during colder wintertime conditions found in Detroit, the northernmost city modeled.  相似文献   

18.
Large auxiliary engines operated on ocean-going vessels in transit and at berth impact the air quality of populated areas near ports. This paper presents new information on the comparison of emission ranges from three similar engines and the effectiveness of three control technologies: switching to cleaner burning fuels, operating in the low oxides of nitrogen (NOx) mode, and selective catalytic reduction (SCR). In-use measurements of gaseous (NOx, carbon monoxide [CO], carbon dioxide [CO2]) and fine particulate matter (PM2.5; total and speciated) emissions were made on three auxiliary engines on post-PanaMax class container vessels following the International Organization for Standardization-8178-1 protocol. The in-use NOx emissions for the MAN B&W 7L32/40 engine family vary from 15 to 21.1 g/kW-hr for heavy fuel oil and 8.9 to 19.6 g/kW-hr for marine distillate oil. Use of cleaner burning fuels resulted in NOx reductions ranging from 7 to 41% across different engines and a PM2.5 reduction of up to 83%. The NOx reductions are a consequence of fuel nitrogen content and engine operation; the PM2.5 reduction is attributed to the large reductions in the hydrated sulfate and organic carbon (OC) fractions. As expected, operating in the low-NOx mode reduced NOx emissions by approximately 32% and nearly doubled elemental carbon (EC) emissions. However, PM2.5 emission factors were nearly unchanged because the EC emission factor is only approximately 5% of the total PM2.5 mass. SCR reduced the NOx emission factor to less than 2.4 g/kW-hr, but it increased the PM2.5 emissions by a factor of 1.5-3.8. This increase was a direct consequence of the conversion of sulfur dioxide to sulfate emissions on the SCR catalyst. The EC and OC fractions of PM2.5 reduced across the SCR unit.  相似文献   

19.
Abstract

The purpose of this investigation was to quantify the potential of natural gas to reduce emissions from stationary combustion sources by analyzing the case study of the metropolitan region of Santiago, Chile. For such purposes, referential base scenarios have been defined that represent with and without natural gas settings. The method to be applied is an emission estimate based on emission factors. The results for this case study reveal that stationary combustion sources that replaced their fuel reduced particulate matter (PM) emissions by 61%, sulfur oxides (SOx) by 91%, nitrogen oxides (NOx) by 40%, and volatile organic compounds (VOC) by 10%. Carbon mon-oxide (CO) emissions were reduced by 1%. As a result of this emission reduction, in addition to reductions caused by other factors, such as a shift to cleaner fuels other than natural gas, technological improvements, and sources which are not operative, emission reduction goals set forth by the environmental authorities were broadly exceeded.  相似文献   

20.
Hong Kong is a densely populated city situated in the fast developing Pearl River Delta of southern China. In this study, the recent data on ozone (O3) and related air pollutants obtained at three sites in Hong Kong are analyzed to show the variations of O3 in urban, sub-urban and rural areas and the possible regional influences. Highest monthly averaged O3 was found at a northeastern rural site and lowest O3 level was observed at an urban site. The levels of NOx, CO, SO2 and PM10 showed a different spatial pattern with the highest level in the urban site and lowest at the rural site. Analysis of chemical species ratios such as SO2/NOx and CO/NOx indicated that the sites were under the influences of local and regional emissions to varying extents reflecting the characteristics of emission sources surround the respective sites. Seasonal pattern of O3 is examined. Low O3 level was found in summer and elevated levels occurred in autumn and spring. The latter appears different from the previous result obtained in 1996 indicating a single maximum occurring in autumn. Principal component analysis was used to further elucidate the relationships of air pollutants at each site. As expected, the O3 variation in the northeastern rural area was largely determined by regional chemical and transport processes, while the O3 variability at the southwestern suburban and urban sites were more influenced by local emissions. Despite the large difference in O3 levels across the sites, total potential ozone (O3+NO2) showed little variability. Cases of high O3 episodes were presented and elevated O3 levels were formed under the influence of tropical cyclone bringing in conditions of intense sunlight, high temperature and light winds. Elevated O3 levels were also found to correlate with enhanced ratio of SO2 to NOx, suggesting influence of regional emissions from the adjacent Pearl River Delta region.  相似文献   

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