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1.
Foliage on spruce trees (Picea rubens Sarg.) growing on dry SO(2) deposition zones (dry SO(2) deposition ranging from 0.5 and 8.5 S kg ha(-1) year(-1)) downwind from a SO(2) emission source was analyzed to assess chronic effects of long-term low-grade SO(2) deposition on net photosynthesis, stomatal conductance, dark respiration, stomatal antechamber wax structures, elemental concentrations in and on foliage (bulk and surficial concentrations), and types of epiphytic fungi that reside in the phylloplane. Elemental distributions on stomatal antechambers, on fungal colonies, and on smooth surfaces between stomates and fungus colonies were determined with a scanning electronic microscope (SEM) by way of X-ray scanning. It was found that net photosynthesis of newly developed spruce foliage (current-year, and 1-year-old) was not significantly affected by the local SO(2) deposition rates. Sulfur dioxide deposition, however, may have contributed to the gradual decrease in net photosynthesis with increasing needle age. Dark respiration rates were significantly higher on foliage taken from high SO(2) deposition zones. Stomatal rod-web structures deteriorated to flakes with increasing needle age and increasing SO(2) deposition. Further inspection of the needle surfaces revealed an increasing abundance of fungal colonies with increasing needle age. Many fungal taxa were isolated and identified. It was found that black yeasts responded positively, and Xylohypha pinicola responded negatively to high rates of SO(2) deposition. Surficial concentrations of elements such as P, S, K, Cl, Ca were about 10 times higher on fungal colonies than on smooth needle surfaces. Surficial Ca contents on 4 or 5-year-old needles decreased with increasing SO(2) deposition, but surficial S concentrations remained the same. In contrast, bulk foliar Ca and S concentrations increased with increasing SO(2) deposition.  相似文献   

2.
Nighttime measurements of aerosol surface area, O3, NOy and moisture were made downwind of Portland, Oregon, as part of a study to characterize the chemistry in a nocturnal urban plume. Air parcels sampled within the urban plume soon after sunset had positive correlations between O3, relative humidity, NOy and aerosol number density. However, the air parcels sampled within the urban plume just before dawn had O3 mixing ratios that were highly anti-correlated with aerosol number density, NOy and relative humidity. Back-trajectories from a mesoscale model show that both the post-sunset and pre-dawn parcels came from a common maritime source to the northwest of Portland. The pre-dawn parcels with strong anti-correlations passed directly over Portland in contrast to the other parcels that were found to pass west of Portland. Several gas-phase mechanisms and a heterogeneous mechanism involving the loss of O3 to the aerosol surface, are examined to explain the observed depletion in O3 within the pre-dawn parcels that had passed over Portland.  相似文献   

3.
To understand the influence of the reduction of SO2 emissions from a single source in the S and N deposition around its local environment, the application of the Sulphur Transport Eulerian Model 2 (STEM-II) was introduced in this paper. Observed local deposition patterns were analysed and explained in terms of the main processes involved in the pollutants deposition. It was necessary to take into account the limited availability of H2O2 because of its influence on both S(IV) and oxidized nitrogen deposition. In order to estimate the quantitative relationship between the SO2 emissions reduction and the observed S and N deposition patterns, these processes were simulated for different meteorological conditions. Simulation results were in agreement with both observed deposition patterns and limited availability of H2O2, specially if significant changes in the S deposition patterns were considered. Both observed and estimated S deposition patterns changed their top value location from the Southwest (1990) to the Northwest (1997) of the domain, because of the reduction of dry deposition. The global reduction of total S depositions, estimated and observed, were in good agreement too. Model simulations could explain the higher S dry deposition reduction, considering the emissions reduction strategy applied.  相似文献   

4.
Ek AS  Löfgren S  Bergholm J  Qvarfort U 《Ambio》2001,30(2):96-103
Copper production in Falun, central Sweden, has emitted sulfur dioxide (SO2) and metals to the air during at least 1000 years. Emissions peaked in the 17th century when Falun produced 2/3 of the world's copper supply. This area offers unique opportunities to study long-term effects of acid deposition and metal pollution, including recovery following the three centuries of decreasing SO2 and metal deposition. Here we present a 1000-yr perspective on local emissions of SO2, estimated air concentrations and dry deposition of SO2, as well as results on acidification and metal pollution of soils and lakes. Despite a long period when deposition of SO2 exceeded the critical load, soil acidification is limited to the most heavily polluted area 12 km NW and SE from the mine. According to diatom analyses of take sediments, only 8 of 14 lakes have become acidified (0.4-0.8 pH units). None of these lakes show recovery from acidification, probably due to large amounts of sulfate still accumulated in the soils and changes in land use.  相似文献   

5.
BACKGROUND, AIM, AND SCOPE: Asymmetrical convective non-local scheme (CON) with varying upward mixing rates is developed for simulation of vertical turbulent mixing in the convective boundary layer in air quality and chemical transport models. MATERIALS AND METHODS: The upward mixing rate form the surface layer is parameterized using the sensible heat flux and the friction and convective velocities. Upward mixing rates varying with height are scaled with an amount of turbulent kinetic energy in layer, while the downward mixing rates are derived from mass conservation. RESULTS: This scheme provides a less rapid mass transport out of surface layer into other layers than other asymmetrical convective mixing schemes. DISCUSSION: In this paper, we studied the performance of a nonlocal convective mixing scheme with varying upward mixing in the atmospheric boundary layer and its impact on the concentration of pollutants calculated with chemical and air-quality models. This scheme was additionally compared versus a local eddy-diffusivity scheme (KSC). Simulated concentrations of NO(2) and the nitrate wet deposition by the CON scheme are closer to the observations when compared to those obtained from using the KSC scheme. CONCLUSIONS: Concentrations calculated with the CON scheme are in general higher and closer to the observations than those obtained by the KSC scheme (of the order of 15-20%). Nitrate wet deposition calculated with the CON scheme are in general higher and closer to the observations than those obtained by the KSC scheme. RECOMMENDATIONS AND PERSPECTIVES: To examine the performance of the scheme, simulated and measured concentrations of a pollutant (NO(2)) and nitrate wet deposition was compared for the year 2002. The comparison was made for the whole domain used in simulations performed by the chemical European Monitoring and Evaluation Programme Unified model (version UNI-ACID, rv2.0) where schemes were incorporated.  相似文献   

6.
The rate of conversion of SO2 to SO4(2-) was re-estimated from measurements made in the plume of the Cumberland power plant, located on the Cumberland River in north-central Tennessee, after installation of flue gas desulfurization (FGD) scrubbers for SO2 removal in 1994. The ratio of SO2 to NOy emissions into the plume has been reduced to approximately 0.1, compared with a prescrubber value of approximately 2. To determine whether the SO2 emissions reduction has correspondingly reduced plume-generated particulate SO4(2-) production, we have compared the rates of conversion before and after scrubber installation. The prescrubber estimates were developed from measurements made during the Tennessee Plume Study conducted in the late 1970s. The postscrubber estimates are based upon two series of research flights in the summers of 1998 and 1999. During two of these flights, the Cumberland plume did not mix with adjacent power plant plumes, enabling rate constants for conversion to be estimated from samples taken in the plume at three downwind distances. Dry deposition losses and the fact the fact that SO2 is no longer in large excess compared with SO4(2-) have been taken into account, and an upper limit for the conversion rate constant was re-estimated based on plume excess aerosol volume. The estimated upper limit values are 0.069 hr(-1) and 0.034 hr(-1) for the 1998 and 1999 data, respectively. The 1999 rate is comparable with earlier values for nonscrubbed plumes, and although the 1998 upper limit value is higher than expected, these estimates do not provide strong evidence for deviation from a linear relationship between SO2 emissions and SO4(2-) formation.  相似文献   

7.
Agricultural meteorological modeling techniques are used to investigate the relative and absolute dry deposition fluxes of SO2 (as sulfur), HNO3 (as nitrogen) and O3 to large fields of maize, soybeans, and alfalfa exposed in conditions as measured in northern Illinois, central Pennsylvania, and eastern Tennessee. For HNO3, the differences in seasonal deposition rates among the three types of plant species are small. Within the same environment, the soybean canopy has the potential to receive substantially more gaseous dry deposition of SO2 and O3 than the maize and alfalfa (which are about the same), as a result of lower stomatal resistance and consequently higher deposition velocities. Deposition differences among the sites are small except for the case of SO2, for which deposition rates estimated for northern Illinois are nearly double those at the other locations. The high SO2 deposition at the northern Illinois location is a consequence of the higher air concentrations observed there.  相似文献   

8.
Production and transport of urban air pollution were studied at São Paulo, Brazil, due to the importance of the megacity as source of pollutants and the flow pattern and topography of the region. An Eulerian air quality model was applied. An improved method for calculating vertical diffusivities was introduced in the model and the impact on the behavior of pollutants was analyzed. The approach includes both shear generated and buoyancy-driven turbulence in a continuous formulation that adequately represents turbulence evolution in the atmospheric boundary layer. Dispersion and transformation processes are well described by model simulations. The application of the proposed parameterization leads to increased predicted concentrations. Relative changes range from 1.2 to 2. Uncertainties in the emissions result in some disagreement between measured and simulated concentrations.  相似文献   

9.
The Fugitive Dust Model (FDM) and Industrial Source Complex (ISC), widely used coarse particulate dispersion models, have been shown inaccurate due to the neglect of vertical variations in atmospheric wind speed and turbulent diffusivity (Vesovic et al., 2001), omission of the gravitational advection velocity, and an underestimation of the ground deposition velocity (Kim and Larson, 2001). A simple, transient two-dimensional convection-diffusion-sedimentation model is proposed to simulate the evolution in particle size distribution of an aerosol ‘puff’ containing coarse particulate in the atmospheric surface layer. Monin-Okhubov similarity theory, accompanied by empirical observations made by Businger et al. (1971), is adopted to characterize the surface layer wind speed and turbulent diffusivity profiles over a wide range of atmospheric conditions. A first order analysis of the crossing trajectories effect suggests simulation data presented here are not significantly affected by particle inertia. The model is validated against Suffield experimental data in which coarse particulate deposition was measured out to a distance of 800 m from the source (Walker, 1965). Good agreement is found for the decay in ground deposits with distance from the source for stable atmospheres. Deposition data was also simulated for unstable atmospheric stratification and the current model was determined to modestly underestimate the peak concentration with increasing accuracy further downwind of the release. The current model's effective deposition velocity was compared to that suggested by Kim et al. (2000) and shows improvement with respect to FDM. Lastly, the model was used to simulate the dispersion of nine lognormal aerosol puffs in the lowest 50 m of the atmospheric surface layer for four classes of atmospheric stability. The simulated mass median aerodynamic diameters (MMAD) at multiple downwind sampling locations were calculated and plotted with distance from the source. The first 50 m from the source was found to have a substantial impact on the evolution of MMAD for stable atmospheric conditions. Away from the source, it was observed that particle size distributions were truncated by removal of all particles larger than about 60 μm. A particle Peclet number was also defined to quantify the relative importance of turbulent dispersion and sedimentation on particle motion in the vertical direction.  相似文献   

10.
Clear and through-fall bulk depositions were collected in the downwind of a highly industrialized region in Sonbhadra district of India to estimate the influence of anthropogenic activities on chemical composition of depositions. Significant spatial and temporal variations in depositions of cations and anions were observed. Depositions were higher near the thermal power stations and coal mines as compared to distantly situated site. Seasonally summer samples showed maximum cation and anion depositions followed by winter and minimum in rainy season. The mean pH of the depositions indicates that rainfall in the area is alkaline. Among the anions, maximum deposition was recorded for SO4(2-) followed by NO3- and minimum for Cl-. Among the cations, Ca2+ deposition was maximum followed by NH4+. Na+, K+ and Mg2+ deposition rates showed more or less similar values. The depositions of cations and anions as well as pH were higher in through-fall than clear-fall samples. Results of the present study suggest that atmospheric depositions are strongly modified due to thermal power stations and coal mines in the area.  相似文献   

11.
The experimental and numerical study considers the concentration of airborne particulate contaminants, such as spores of spoilage fungi, and their deposition on a surface, in a Petri dish, and on a warm box-shaped product placed in a food-processing environment. Field measurements by standard, active and passive samplers provide typical values of airborne concentrations and specific deposition fluxes. Velocity and turbulence data from field studies are used as input in large eddy simulations of the process, and estimates of deposition fluxes are of the same order of magnitude as those deduced from field measurements. Particle deposition is shown to be associated with near-wall coherent structures. Flow reversal, simulated by impulsive start, is shown to give higher deposition rates than steady mean flows.  相似文献   

12.
This study used pollution roses to assess sulfur dioxide (SO2) pollution in a township downwind of a large petrochemical complex based on data collected from a single air quality monitoring station. The pollution roses summarized hourly SO2 concentrations at the Taishi air quality monitoring station, located approximately 7.8–13.0 km south of the No. 6 Naphtha Cracking Complex in Taiwan, according to 36 sectors of wind direction during the preoperational period (1995–1999) and two postoperational periods (2000–2004 and 2005–2009). The 99th percentile of hourly SO2 concentrations 350? downwind from the complex increased from 28.9 ppb in the preoperational period to 86.2–324.2 ppb in the two postoperational periods. Downwind SO2 concentrations were particularly high during 2005–2009 at wind speeds of 6–8 m/sec. Hourly SO2 levels exceeded the U.S. Environmental Protection Agency (EPA) health-based standard of 75 ppb only in the postoperational periods, with 65 exceedances from 0–10? and 330–350? downwind directions during 2001–2009. This study concluded that pollution roses based on a single monitoring station can be used to investigate source contributions to air pollution surrounding industrial complexes, and that it is useful to combine such directional methods with analyses of how pollution varies between different wind speeds, times of day, and periods of industrial development.

Implications: The pollution roses summarize SO2 concentrations by wind direction and to investigate source contribution to air quality. Percentile statistics can catch pollution episodes occurring in a very short time at specific wind directions and speeds. The downwind areas have already exceeded regulated 1-hr SO2 standard since the operation of the complex.  相似文献   

13.
This work focuses on bulk deposition in a rural area located around a large coal-fired power station in northeast Spain. Deposition chemistry was characterised by high concentrations of SO(4)(2-), Ca(2+) and NH(4)(+), which were relatively high when compared with other rural areas. Monthly bulk deposition evolution of major ions was the result of two superimposed patterns: one pattern related to the volume of precipitation and the other showed the seasonal influence of the major ionic sources. A major local origin was attributed to bulk deposition of SO(4)(2-), NH(4)(+), and Ca(2+), whereas a relatively higher contribution of an external source was deduced for NO(3)(-), Na(+) and Cl(-). The SO(4)(2-) concentrations showed a significant correlation with the local SO(2) emissions. High levels of Ca(2+) were due to the high alkalinity of soils in the study area, although an external origin was attributed to the frequent air mass intrusions from the Sahara. Sources of NH(4)(+) were related to intensive livestock farming in the area. Total suspended particles exert a marked influence over bulk deposition and neutralisation. Thus, despite the high emissions of SO(2) in the area, neutral pH values have always been attained given that the concentrations of Ca(2+) and NH(4)(+) account for the total neutralisation of NO(3)(-) and SO(4)(2-).  相似文献   

14.
The effect of three-dimensional, axisymmetric hills on the mean flow and turbulence structure of a boundary layer is investigated through experiments conducted in a large meteorological wind tunnel Two conical hills having slopes of 26.5° and 17.5° and height (H) about one-quarter of the simulated boundary layer thickness were considered. Measurements of mean and turbulent flow and diffusion on the lee sides of the hills are presented and compared with the observations made without the hills. Velocity measurements behind the steeper hill (26.5°) showed a well defined recirculating zone and the presence of weak trailing vortices in the lower region (z = 0.3H), whereas no such features could be detected behind the gentler hill.Perturbations in mean velocity, Reynolds stress and variances of velocity fluctuations in the far wake (beyond 4H) are found to decay with the downwind distance from the center of the hill according to some power laws. The decay rates of mean velocity deficit and turbulence pertubations in the far wake are compared with the theoretical predictions of Hunt (1971, Central Electricity Research Lab. Rep. 1974, ARC, Rep. 35601, Atmos. 229) and Lemberg (1973, PhD Dissertation, Rep. No. BLWT-3-73, Univ. of W Ontario) as well as with the results of other experiments.Comparisons of diffusion measurements at various distances from a point source with and without the hill bring out several interesting aspects of dispersion in the wake of the gentler hill. A 40–65% reduction in maximum ground-level concentration (glc) was observed when the source was placed at the top of the hill, whereas a marked increase (up to six times) in the glc was noticed when the source was moved to the downwind base of the hill. Enhanced vertical and lateral dispersion was also evident in the wake region.  相似文献   

15.
Air quality model simulations constitute an effective approach to developing source-receptor relationships (so-called transfer coefficients in the risk analysis framework) because a significant fraction of particulate matter (particularly PM2.5) is secondary (i.e., formed in the atmosphere) and, therefore, depends on the atmospheric chemistry of the airshed. In this study, we have used a comprehensive three-dimensional air quality model for PM2.5 (SAQM-AERO) to compare three approaches to generating episodic transfer coefficients for several source regions in the Los Angeles Basin. First, transfer coefficients were developed by conducting PM2.5 SAQM-AERO simulations with reduced emissions of one of four precursors (i.e., primary PM, sulfur dioxide (SO2), oxides of nitrogen (NOx), and volatile organic compounds) from each source region. Next, we calculated transfer coefficients using two other methods: (1) a simplified chemistry for PM2.5 formation, and (2) simplifying assumptions on transport using information limited to basin-wide emission reductions. Transfer coefficients obtained with the simplified chemistry were similar to those obtained with the comprehensive model for VOC emission changes but differed for NOx and SOz emission changes. The differences were due to the parameterization of the rates of secondary PM formation in the simplified chemistry. In 90% of the cases, transfer coefficients estimated using only basin-wide information were within a factor of two of those obtained with the explicit source-receptor simulations conducted with the comprehensive model. The best agreement was obtained for VOC emission changes; poor agreement was obtained for primary PM2.5.  相似文献   

16.
A new method was developed for determining the contribution of one pollutant source to the air quality in an industrialized region. Although the method is general, it is presented in reference to a 130,000 bbl/day petroleum refinery and its effect on ambient SO2 concentrations in Sarnia, Ontario. The plumes from SO2 emitters located upwind of the refinery were represented by a single hypothetical plume which influences monitoring stations located upwind as well as downwind from the refinery. However, the refinery emissions affect only the downwind stations. A simple equation was derived by means of which the concentration at the downwind station could be calculated from the concentration at the upwind station and the refinery emission. This equation contains two coefficients A and B which were evaluated such that the difference between the cumulative frequency distributions of the measured and calculated SO2 concentrations at the downwind station was minimized. For the meteorological conditions and monitoring stations considered, it was found that the refinery contributed less than 4.5 pphm to ambient SO2 concentrations over 1 hr periods. This result and the validity of the method are discussed.  相似文献   

17.
This paper presents a new approach to quantify emissions from fugitive gaseous air pollution sources. The authors combine Computed Tomography (CT) with Path-Integrated Optical Remote Sensing (PI-ORS) concentration data in a new field beam geometry. Path-integrated concentrations are sampled in a vertical plane downwind from the source along several radial beam paths. An innovative CT technique, which applies the Smooth Basis Function Minimization method to the beam data in conjunction with measured wind data, is used to estimate the total flux from the fugitive source. The authors conducted a synthetic data study to evaluate the proposed methodology under different meteorological conditions, beam geometry configurations, and simulated measurement errors. The measurement errors were simulated based on data collected with an Open-Path Fourier Transform Infra-Red system. This approach was found to be robust for the simulated errors and for a wide range of fluctuating wind directions. In the very sparse beam geometry examined (eight beam paths), successful emission rates were retrieved over a 70 degrees range of wind directions under extremely large measurement error conditions.  相似文献   

18.
The particle size distributions (PSDs) of particulate matter (PM) in the downwind plume from simulated sources of a cotton gin were analyzed to determine the impact of PM settling on PM monitoring. The PSD of PM in a plume varies as a function of gravitational settling. Gravitational settling has a greater impact on the downwind PSD from sources with PSDs having larger mass median diameters (MMDs). The change in PSD is a function of the source PSD of emitted PM, wind speed, and downwind distance. Both MMD and geometric standard deviation (GSD) in the downwind plume decrease with an increase in downwind distance and source MMD. The larger the source MMD, the greater the change in the downwind MMD and GSD. Also, the greater the distance from the source to the sampler, the greater the change in the downwind MMD and GSD. Variations of the PSD in the downwind plume significantly impact PM10 sampling errors associated with the U.S. Environmental Protection Agency (EPA) PM10 samplers. For the emission sources with MMD > 10 microm, the PM10 oversampling rate increases with an increase in downwind distance caused by the decrease of GSD of the PSD in the downwind plume. Gravitational settling of particles does not help reduce the oversampling problems associated with the EPA PM10 sampler. Furthermore, oversampling rates decrease with an increase of the wind speed.  相似文献   

19.
Contributions of the emissions from a U.K. regulated fossil-fuel power station to regional air pollution and deposition are estimated using four air quality modeling systems for the year 2003. The modeling systems vary in complexity and emphasis in the way they treat atmospheric and chemical processes, and include the Community Multiscale Air Quality (CMAQ) modeling system in its versions 4.6 and 4.7, a nested modeling system that combines long- and short-range impacts (referred to as TRACK-ADMS [Trajectory Model with Atmospheric Chemical Kinetics-Atmospheric Dispersion Modelling System]), and the Fine Resolution Atmospheric Multi-pollutant Exchange (FRAME) model. An evaluation of the baseline calculations against U.K. monitoring network data is performed. The CMAQ modeling system version 4.6 data set is selected as the reference data set for the model footprint comparison. The annual mean air concentration and total deposition footprints are summarized for each modeling system. The footprints of the power station emissions can account for a significant fraction of the local impacts for some species (e.g., more than 50% for SO2 air concentration and non-sea-salt sulfur deposition close to the source) for 2003. The spatial correlation and the coefficient of variation of the root mean square error (CVRMSE) are calculated between each model footprint and that calculated by the CMAQ modeling system version 4.6. The correlation coefficient quantifies model agreement in terms of spatial patterns, and the CVRMSE measures the magnitude of the difference between model footprints. Possible reasons for the differences between model results are discussed. Finally, implications and recommendations for the regulatory assessment of the impact of major industrial sources using regional air quality modeling systems are discussed in the light of results from this case study.  相似文献   

20.
Land use data are among the inputs used to determine dry deposition velocities for photochemical grid models such as the Comprehensive Air Quality Model with extensions (CAMx) that is currently used for attainment demonstrations and air quality planning by the state of Texas. The sensitivity of dry deposition and O3 mixing ratios to land use classification was investigated by comparing predictions based on default U.S. Geological Survey (USGS) land use data to predictions based on recently compiled land use data that were collected to improve biogenic emissions estimates. Dry deposition of O3 decreased throughout much of eastern Texas, especially in urban areas, with the new land use data. Predicted 1-hr averaged O3 mixing ratios with the new land use data were as much as 11 ppbv greater and 6 ppbv less than predictions based on USGS land use data during the late afternoon. In addition, the area with peak O3 mixing ratios in excess of 100 ppbv increased significantly in urban areas when deposition velocities were calculated based on the new land use data. Finally, more detailed data on land use within urban areas resulted in peak changes in O3 mixing ratios of approximately 2 ppbv. These results indicate the importance of establishing accurate, internally consistent land use data for photochemical modeling in urban areas in Texas. They also indicate the need for field validation of deposition rates in areas experiencing changing land use patterns, such as during urban reforestation programs or residential and commercial development.  相似文献   

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