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1.
Keller W  Heneberry JH  Dixit SS 《Ambio》2003,32(3):183-189
Lakes in Killarney Park near Sudbury, Ontario, Canada, have shown dramatic water quality changes including general increases in pH and alkalinity, and decreases in SO4(2-), base cations and metals. While some lakes have recovered to pH > 6.0, many are still highly acidic despite decades of improvement. Very high historical S deposition related to emissions from the Sudbury metal smelters dominated the acidification process in this region. However, since the implementation of substantial S emission controls (90%) at the smelters, the Sudbury emissions are no longer the major source of S deposition in the Sudbury area. Wet deposition of SO4(2-) and SO4(2-) concentrations in lakewaters at Killarney now approach values in the Dorset, Ontario, area, about 200 km from Sudbury. This suggests that the S deposition to the Killarney area is now primarily from long-range transport, not from local sources. Studies of Killarney lakes are revealing the complex nature of the chemical recovery process. As lake acidity decreases, other changes including decreased Ca2+ concentrations, increased transparency, and altered thermal regimes may potentially affect some of these ecosystems. It is clear that continuing assessments of the recovery of Killarney lakes, within a multiple-stressor framework, are needed.  相似文献   

2.
Reductions in North American sulfur dioxide (SO2) emissions promoted expectations that aquatic ecosystems in southeastern Canada would soon recover from acidification. Only lakes located near smelters that have dramatically reduced emissions approach this expectation. Lakes in the Atlantic provinces, Quebec and Ontario affected only by long-range sources show a general decline in sulfate (SO4(2-)) concentrations, but with a relatively smaller compensating increase in pH or alkalinity. Several factors may contribute to the constrained (or most likely delayed) acidity response: declining base cation concentrations, drought-induced mobilization of SO4(2-), damaged internal alkalinity generation mechanisms, and perhaps increasing nitrate or organic anion levels. Monitoring to detect biological recovery in southeastern Canada is extremely limited, but where it occurs, there is little evidence of recovery outside of the Sudbury/Killarney area. Both the occurrence of Atlantic salmon in Nova Scotia rivers and the breeding success of Common Loons in Ontario lakes are in fact declining although factors beyond acidification also play a role. Chemical and biological models predict that much greater SO2 emission reductions than those presently required by legislation will be needed to promote widespread chemical and latterly, biological recovery. It may be unrealistic to expect that pre-industrial chemical and biological conditions can ever be reestablished in many lakes of southeastern Canada.  相似文献   

3.
In Europe, secondary particulate matter (PM) comprises 50% or more of PM 2.5. To reduce PM concentrations requires lowering precursor emissions. Since the 1980s, SO(2) emissions have decreased by more than 60%, while particle concentrations have decreased less. NO(x) and NH(3) emissions have decreased slightly. The role of ammonia in particle formation is addressed here. It is shown that secondary PM concentrations can only be effectively reduced if ammonia emissions are decreased in much the same way as those of SO(2) and NO(x).  相似文献   

4.
Twenty-five MiniVol samplers were operated throughout the Mexico City metropolitan region from February 22 through March 22, 1997, to evaluate the variability of PM10 concentrations and composition. The highest PM10 concentrations were found in neighborhoods with unpaved or dirty roads, and elements related to crustal material were the main cause of differences from nearby (<200 m) monitors that were not adjacent to the roadbed. SO4(2-) concentrations were homogeneous across the city. SO4(2-) measured at the city boundaries was about two-thirds of the concentrations measured within the urbanized area, indicating that most SO4(2-) is of regional origin. Elemental carbon (EC) and organic carbon (OC) concentrations were highly variable, with higher concentrations in areas that had high diesel traffic and older vehicles. Spatial correlations among PM10 concentrations were high, even though absolute concentrations were variable, indicating a common effect of meteorology on the concentration or dispersion of local emissions.  相似文献   

5.
Ozone (O(3)) pollution episodes take place in Catalonia (NE of the Iberian Peninsula), mainly during summertime. The complex O(3) behaviour could be understood by using a Chemical Transport Model (CTM). Emission inventories provide the spatial and temporal emissions distribution of the O(3) precursors and other pollutants required by this approach. We developed the EMICAT2000 model with high spatial (cells of 1 km(2)) and temporal (1h) resolutions, to estimate the emissions during the year 2000 from Catalonia. Total annual emissions were 107 kt yr(-1) of NO(x), 137 kt yr(-1) of NMVOC, 267 kt yr(-1) of CO, 65 kt yr(-1) of SO(2), 24 kt yr(-1) of TSP and 32,175 kt yr(-1) of equivalent CO(2). Main NO(x) sources are on-road traffic (58%) and industries (38%). Main NMVOC sources are on-road traffic (36%), vegetation (34%) and use of solvents (13%). Speciation was established according to the Carbon Bond IV mechanism. EMICAT2000 generates directly the data files required for the third generation CTM Models-3/CMAQ.  相似文献   

6.
A three-dimensional chemical transport model (PMCAMx) was used to investigate changes in fine particle (PM2.5) concentrations in response to changes in sulfur dioxide (SO2) and ammonia (NH3) emissions during July 2001 and January 2002 in the eastern United States. A uniform 50% reduction in SO2 emissions was predicted to produce an average decrease of PM2.5 concentrations by 26% during July but only 6% during January. A 50% reduction of NH3 emissions leads to an average 4 and 9% decrease in PM2.5 in July and January, respectively. During the summer, the highest concentration of sulfate is in South Indiana (12.8 microg x m(-3)), and the 50% reduction of SO2 emissions results in a 5.7 microg x m(-3) (44%) sulfate decrease over this area. During winter, the SO2 emissions reduction results in a 1.5 microg x m(-3) (29%) decrease of the peak sulfate levels (5.2 microg x m(-3)) over Southeast Georgia. The maximum nitrate and ammonium concentrations are predicted to be over the Midwest (1.9 (-3)g x m(-3) in Ohio and 5.3 microg x m(-3) in South Indiana, respectively) in the summer whereas in the winter these concentrations are higher over the Northeast (3 microg x m(-3) of nitrate in Connecticut and 2.7 microg x m(-3) of ammonium in New York). The 50% NH3 emissions reduction is more effective for controlling nitrate, compared with SO2 reductions, producing a 1.1 microg x m(-3) nitrate decrease over Ohio in July and a 1.2 microg x m(-3) decrease over Connecticut in January. Ammonium decreases significantly when either SO2 or NH3 emissions are decreased. However, the SO2 control strategy has better results in July when ammonium decreases, up to 2 microg x m(-3) (37%), are predicted in South Indiana. The NH3 control strategy has better results in January (ammonium decreases up to 0.4 microg x m(-3) in New York). The spatial and temporal characteristics of the effectiveness of these emission control strategies during the summer and winter seasons are discussed.  相似文献   

7.
A survey of monthly average concentrations of sulfur dioxide (SO2) and hydrogen sulfide (H2S) at rural locations in western Canada (provinces of Alberta, British Columbia, and Saskatchewan) was conducted in 2001-2002, as part of an epidemiological study of the effects of oil and gas industry emissions on the health of cattle. Repeated measurements were obtained at some months and locations. We aimed to develop statistical models of the effect of oil and gas infrastructure on air concentrations. The regulatory authorities supplied the information on location of the different oil and gas facilities during the study period and, for Alberta, provided data on H2S content of wells and flaring volumes. Linear mixed effects models were used to relate observed concentrations to proximity and type of oil and gas infrastructure. Low concentrations were recorded; the monthly geometric mean was 0.1-0.2 ppb for H2S, and 0.3-1.3 ppb for SO2. Substantial variability between repeated measurements was observed. The precision of the measurement method was 0.005 ppb for both contaminants. There were seasonal trends in the concentrations, but the spatial variability was greater. This was explained, in part, by proximity to oil/gas/bitumen wells and (for SO2) gas plants. Wells within 2 km of monitoring stations had the greatest impact on measured concentrations. For H2S, 8% of between-location variability was explained by proximity to industrial sources of emissions; for SO2 this proportion was 18%. In Alberta, proximity to sour gas wells and flares was associated with elevated H2S concentrations; however, the estimate of the effect of sour gas wells in the immediate vicinity of monitoring stations was unstable. Our study was unable to control for all possible sources of the contaminants. However, the results suggest that oil and gas extraction activities contribute to air pollution in rural areas of western Canada.  相似文献   

8.
Ambient aerosols adversely affect human health and visibility and impact climate. Identification of sources of particulate matter and its precursors is necessary for developing control strategies. The goal of this research is to utilize long-term speciated particulate matter data and back-trajectory cluster analyses to determine trends and sources of particulate matter in the Superstition Wilderness, a rural area east of Phoenix, Arizona. Twenty-four hour back-trajectories were calculated for every hour of every 24-h particulate matter sample obtained by IMPROVE from 1991 to 2004. Days that included back-trajectories with considerable spatial variance were excluded from further analyses. To minimize uncertainties inherent in single trajectories, all calculated trajectories for each sampling day were averaged to represent the air mass sampled during that day. Cluster analysis of trajectories identified four unique regions, including a region with Phoenix, a region with copper smelters, and one with coal-fired power plants. Yearly averages of sulfate, nitrate, soil, and carbon concentrations were calculated for each region. Statistically significant trends in species concentrations by region and independent of region and differences in concentrations between regions were examined.Sulfate concentrations from the region with smelters were higher than other regions but decreased during the study period. Emissions data from the smelters indicate that much of the sulfate from the region was due to the smelters. The overall 2.2% year−1 decrease in sulfate concentrations at TNM is likely due to decreased emissions from the copper smelters. A 3.6% year−1 increase in nitrate concentrations was driven largely by increasing NOx concentrations from Phoenix and to a lesser extent the region southwest of the site which includes Tucson and suburban/urban areas between Phoenix and Tucson. Soil concentrations were higher from regions with deserts than the region without desert. This method could not identify trends or source regions of carbonaceous aerosols at this site.  相似文献   

9.
Estimates of emissions of SO2, NOx, HCl and NH3 have been made for a densely populated region of the UK, the North-West of England, using data on power generation, incinerator plant capacity, fuel usage and animal and human population statistics. The spatial distributions of SO2 and NOx emissions are quite different, reflecting their different source strengths. The emissions from motor vehicles make up 52% of the NOx emissions from the North-West of England, whilst those from fossil-fuel-fired power stations make up 20%. The emissions of fossil-fuel-fired power stations make up 58% of SO2 emissions from the North-West. A large fossil-fuel-fired power station is the largest known point source for emissions of SO2, NOx and HCl. The largest contribution to NH3 emissions in the North-West is from cattle. Humans may contribute some NH3 to overall emissions but there is considerable uncertainty as to how much is emitted and what fraction of this is deposited within buildings. The uncertainties in the methodologies used are high-lighted and, where possible, recommendations are made as to how future emissions estimates might be improved. Potential reductions in emissions of SO2, NOx and HCl are discussed under basic scenarios of planned power station closures in the area and the compliance of the electricity generation industry with the European Community Directive on Large Combustion Plants.  相似文献   

10.
Ammonium (NH(4)(+)) concentrations in air and precipitation at the Institute of Ecosystem Studies (IES) in southeastern New York, USA declined over an 11-year period from 1988 to 1999, but increased from 1999 to 2001. These trends in particulate NH(4)(+) correlated well with trends in particulate SO(4)(2-) over the 1988-2001 period. The NH(4)(+) trends were not as well correlated with local cattle and milk production, which declined continuously throughout the period. This suggests that regional transport of SO(4)(2-) may have a greater impact on concentrations of NH(4)(+) and subsequent deposition than local agricultural emissions of NH(3). Ammonium concentrations in precipitation correlated significantly with precipitation SO(4)(2-) concentrations for the 1984-2001 period although NH(4)(+) in precipitation increased after 1999 and SO(4)(2-) in precipitation continued to decline after 1999. The correlation between NH(4)(+) and SO(4)(2-) was stronger for particulates than for precipitation. Particulate NH(4)(+) concentrations were also correlated with particulate SO(4)(2-) concentrations at 31 of 35 eastern U.S. CASTNet sites that had at least 10 years of data. Air concentrations of NH(4)(+) and SO(4)(2-) were more strongly correlated at the sites that were located within an agricultural landscape than in forested sites. At most of the sites there was either no trend or a decrease in NH(4)(+) dry deposition during the 1988-2001 period. The sites that showed an increasing trend in NH(4)(+) dry deposition were generally located in the southeastern U.S. The results of this study suggest that, in the northeastern U.S., air concentrations of NH(4)(+) and subsequent deposition may be more closely linked to SO(4)(2-) and thus SO(2) emissions than with NH(3) emissions. These results also suggest that reductions in S emissions have reduced NH(4)(+) transport to and NH(4)(+)-N deposition in the Northeast.  相似文献   

11.
To gain an understanding of the characteristics of the needle surfaces of naturally regenerated Scots pine (Pinus sylvestris L.) and their geographical distribution, eight physicochemical variables were investigated within the north boreal forest area. The visibly undamaged needles were collected in autumn 1990 from 114 plots (3-5 pines per plot) along radial transects from the Monchegorsk and Nikel smelters, emitting SO2 and heavy metals, on the Kola Peninsula, Russia, to Finnish Lapland. The needles were examined by scanning electron microscopy (SEM) and measured for surface wettability using the droplet contact angle (DCA) method. Significant geographical south-north and west-east patterns could be observed in needle surface characteristics, correlating with emissions from the smelters and to climate. Despite the slightly higher initial DCAs (61.4-87.6 degrees) towards the north, the pine needle surfaces of the northernmost transects exhibited higher annual needle wettability change (ANWC) and wax erosion rate (AWER), expressed as the reduction in DCAs and epistomatal wax tube distribution (WTD) during one year, respectively, but a lower occurrence of particles and fungal hyphae than those of more southern transects. The higher ANWC was related to higher atmospheric SO2 concentration, and to the lower long-term temperature sum, but not clearly to annual precipitation. In the Monchegorsk smelter area, the current needles exhibited, on average, a 15% higher WTD and seven degree larger DCA, resulting in more hydrophobic needle surfaces than in Finnish Lapland, but during their first year, both the AWER and ANWC, were greatly increased. In Finnish Lapland, 30%, of all the epistomatal wax tubes disappeared from the needle surface during the first year, the value being 70% for the pines located 8 km from the smelter. The mineral composition of the particles deposited on the needle surfaces mirrored that of the minerals being produced by the smelters (e.g. FexSx, CuFeS2, NixSx, FexOx). Stomatal densities were in the range of 71.1-141.7 stomata mm(-2). The lower densities of stomata on needles close to the smelters correlated with reduced number of needle age classes of the pines, higher dry weights, higher pollutant accumulation and lower Mn and Zn concentrations in the needles. The AWER and ANWC were able to indicate the most seriously deteriorated needle surfaces on a regional scale, e.g. including the surroundings of both smelters, although the plot-specific relationships between 'needle surface variables' and 'pollution variables' were generally weak. The present study showed that the exposure of pine needles to the combined effects of ambient pollutants and harsh climate led to a deterioration in the physicochemical characteristics of the epicuticular wax, which may have serious ecophysiological consequences in the long term.  相似文献   

12.
Gold smelters near Yellowknife in Canada's Northwest Territories have emitted large quantities of sulfur dioxide and arsenic since inception of roasting in 1941. Although particulate wastes are well contained by baghouse fitters in the one remaining operating smelter, significant gaseous emissions continue. Soil and vegetation were sampled at 52 sites over an area of about 40 km radius from the source. Plant ecology was studied at 43 of those sites. After preliminary multi-element screening that indicated only arsenic was a serious persistent contaminant, x-ray fluorescence was used to measure arsenic content in sampled materials. The plant ecology data were synthesized into an Index of Vitality with numerical ratings of pertinent factors. In the marginal forests and rocky outcrops of the area, indicator species of vegetation permitted a division into zones of severe, moderate, mild, or no impact in order of increasing distance from the current center of emissions. Severe impact, including killing of trees, is local only. Analyses of foliage indicate little uptake of arsenic which, together with the presence of S02 symptoms, point to S02 as the main factor causing decline of vegetation. A separate study, abstracted here, supports this view by providing data that show a frequency of at least 2 significant fumigation episodes per growing season. Soil analyses indicate extremely high arsenic contamination near the stack. A monotonie pattern of dispersion yielded a function explainable in terms of rapid condensation of gaseous emissions. The relationship of arsenic in surface soil and vegetation to distance is approximately an inverse square.  相似文献   

13.
Reductions in the emissions of SO2 and trace metals from the Sudbury smelters have resulted in substantial improvements in water quality in many surrounding lakes. Significant biological changes have accompanied the chemical improvements. Evidence of relatively rapid recovery was found for benthic filamentous algae, phytoplankton, zooplankton, mobile species of benthic invertebrates, and some fish populations. Organisms with low dispersal ability (e.g. Hyalella azteca) have not yet recolonized these lakes. The partial recovery observed to date shows movement toward re-establishment of biological communities typical of natural Precambrian Shield lakes in this area. These findings offer strong support for further efforts to reduce industrial emissions of pollutants to the atmosphere.  相似文献   

14.
Recently, we measured the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) in soil and herbage samples collected in the vicinity of a municipal solid waste incinerator (MSWI) from Tarragona (Catalonia, Spain). Since these concentrations could be increased by the presence of other emission sources of PCDD/Fs in the same area in which the MSWI is placed, the main goal of the present study was to determine the PCDD/F congener profiles in the soil and vegetation samples collected in 1996 and again in 1997 near to the facility and to compare with those from samples collected in a close area outside of direct emissions of the plant. From an accurate inspection of the PCDD/F congener profiles, it was concluded that PCDD/F emissions from the MSWI here examined are neither the only nor the main responsible for the presence of PCDD/Fs in the samples of environmental matrices collected in the area under direct influence of the plant.  相似文献   

15.
Site and regional trends in seasonally averaged particle SO4(2-) concentrations were examined for a large portion of the United States using data collected by the CASTNet air monitoring network. Trends were analyzed for overlapping periods of 1988-1999 and 1992-1999. The largest absolute SO4(2-) decreases--approximately -0.4 microg/m3/yr--between 1988 and 1999 occurred in summer for sites in the Ohio River Valley and areas to the east. Generally, the largest SO4(2-) reductions were found for summer, but larger relative reductions often occurred for spring and autumn. Sulfate changes during 1992-1999 were quite different from those found for 1988-1999 and were not entirely consistent with changes in SO2 emissions. In some locations, the 1992-1999 period saw smaller declines in SO4(2-), while in other places seasonal SO4(2-) actually increased. Increases were mostly confined to summer and autumn across the southern and southwestern states. Multivariate analysis of ambient sulfur levels, by region, versus SO2 emissions reveals that annual emissions are associated with more than 80% of the variance in seasonal sulfur (SO2 and SO4(2-)) in more than three-quarters of the cases examined. The weakest associations were found for the southeastern United States.  相似文献   

16.
S-concentrations were determined in 9 different sample materials (precipitation (rain and snow), vegetation, O-, E-, B- and C- horizon pf podzols, streams water and ground water) collected in eight small catchments (10-30 km2) at different distances from major SO2 point-source emitters on the Kola Peninsula, Russia. Comparison of the results from these materials, representing different compartments of the ecosystems under varying natural conditions leads to a better understanding of sources, cycling and fate of S in the Arctic environment. More than 300,000 t of SO2 emitted annually from the Kola smelters affect the air quality over a large area. Arctic climatic conditions (cold and dry) and the remote location of the emitters results in considerably lower S-deposition values than those observed in central Europe. The pathways of atmospheric S-deposition in the terrestrial environment vary significantly from summer to winter because different compartments of the ecosystems, with a different capability to accumulate S, are active. The actual S-flux is altered by every component of the ecosystem. When estimating the total S-deposition this effect must be considered.  相似文献   

17.
Abstract

Chemical composition and particle size data for particulate emissions from stationary sources are required for environmental health effect assessments, air chemistry studies and for air quality modeling investigations such as source apportionment. The Information presented In this paper is directed to those individuals concerned with these environmental Investigations. In this study, particulate emissions from a group of non-ferrous smelters have been physically and chemically characterized. Emission samples were collected at the baghouse outlets from smelter furnaces and at smelter acid plant stacks at three locations; a zinc, a lead, and a copper smelter.

Mass emission rate determinations were made by EPA reference methods. Cascade impactors were used to collect in-stack samples for particle size distribution measurements. Particulate samples for chemical characterization were collected on membrane filters for analysis by X-ray fluorescence spectroscopy. Development of measurement techniques required to determine the elemental composition of the total mass and sized fractions of the emission are discussed. Results of the tests at the three smelters include total mass and elemental emission rates, particle size distribution, and the elemental composition of the total particulate mass and of sized fractions from both the smelter furnaces and acid plants. The results obtained at the copper smelter may not be representative of the emissions at the many copper smelters where reverbatory furnaces have been replaced.  相似文献   

18.
Blood samples were obtained from 284 deer mice (Peromyscus maniculatus) live-trapped near two base metal smelters in northern Manitoba, Canada. Hemoglobin and hematocrit values were significantly higher in mice trapped within 40-70 km of the smelters compared to those in control areas 185 to 190 km from the smelter. These increases appear to be normal physiological responses to a mild respiratory stress, as in a true secondary polycythemia of anoxic tupe. The mice are sensitive bioindicators of sulphur dioxide emissions that apparently induce the higher blood values.  相似文献   

19.
The geochemical model MAGIC was applied to estimate streamwater and soil chemistry between 1851 and 2030 at the Lysina catchment, an acid-sensitive granitic catchment covered by planted Norway spruce monoculture in the western Czech Republic. The total deposition of sulfur to the catchment was 164 meq m(-2) in 1991, but had declined to 52 meq m(-2) by 2000. Although SO2 emissions in the region declined by 90% compared to the 1980s, acidification recovery was small within the period 1990-2000. Stream pH increased only slightly (from 3.92 to 4.07), although SO4 concentration declined sharply from 568 microeq l(-1) (1990) to 232 microeq l(-1) (2000). Organic acids played an important role in streamwater buffering. According to the MAGIC prediction using deposition measured in 1999-2000, streamwater pH will increase to 4.3 and soil base saturation will increase to 6.2% by 2030 (from 5.7% in 2002). Pre-industrial pH was estimated to be 5.5 and soil base saturation 24.7%. The loss of base cations (Ca, Mg, Na, K) was caused predominantly by atmospheric acidity, but intensive forestry was responsible for approximately one third of the net base cation loss via accumulation in harvested biomass. Severely damaged sites, under continued pressure from forestry, will not return to a good environmental status in the near future (if ever) when the acid deposition input is only partially reduced.  相似文献   

20.
This paper describes remote monitoring of air pollutant emissions by a mobile lidar (light detection and ranging)/ sodar (sound detection and ranging) system. First, measurements are carried out in the flue gas plume of a public power plant. The investigations focus mainly on quantifying SO2 emissions, but the uncertainties of such measurements are also emphasized. Furthermore, an example providing valuable data sets for the development and validation of plume dispersion models is outlined with measurements of the dilution of SO2 along the plume axis. Series of repeated determinations of SO2 emissions show a large variation in the obtained flux values, with moderate margins of error. Incomplete recording of the plume within the individual lidar scans, induced by strong looping movements of the flue gas plume, predominantly causes the variations of flux values. Therefore, the highest flux values determined are considered to be the most exact. This is verified by a comparison of measured fluxes with in situ measurements made by the plant operators. The results further indicate that lidar measurements illustrate the location and dimension of aerosol plumes better than the location and dimension of the plumes of gaseous compounds. The wind direction affecting the plume at any moment can be determined faster by lidar than by sodar because the latter requires much longer time intervals of signal averaging. Measurements show higher concentrations of SO2 compared with results from a Gaussian plume model for periods of less than 5 min after dispersion. The findings emphasize the suitability of remote sensing for detecting emissions and for investigating the propagation and dilution of air pollutant plumes.  相似文献   

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