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1.
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   

2.
The visual impact of primary particles emitted from stacks is regulated according to stack opacity criteria. In-stack monitoring of the flue gas opacity allows plant operators to ensure that the plant meets U.S. Environmental Protection Agency opacity regulations. However, the emission of condensable gases such as SO3 (that hydrolyzes to H2SO4), HCl, and NH3, which may lead to particle formation after their release from the stack, makes the prediction of stack plume opacity more difficult. We present here a computer simulation model that calculates the opacity due to both primary particles emitted from the stack and secondary particles formed in the atmosphere after the release of condensable gases from the stack. A comprehensive treatment of the plume rise due to buoyancy and momentum is used to calculate the location at which the condensed water plume has evaporated (i.e., where opacity regulations apply). Conversion of H2SO4 to particulate sulfate occurs through nucleation and condensation on primary particles. A thermodynamic aerosol equilibrium model is used to calculate the amount of ammonium, chloride, and water present in the particulate phase with the condensed sulfate. The model calculates the stack plume opacity due to both primary and secondary particles. Examples of model simulations are presented for three scenarios that differ by the emission control equipment installed at the power plant: (1) electrostatic precipitators (ESP), (2) ESP and flue gas desulfurization, and (3) ESP and selective catalytic reduction. The calculated opacity is most sensitive to the primary particulate emissions. For the conditions considered here, SO3 emissions showed only a small effect, except if one assumes that most H2SO4 condenses on primary particles. Condensation of NH4Cl occurs only at high NH3 emission rates (about 25 ppm stack concentration).  相似文献   

3.
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   

4.
In this paper the relative importance of NO3- and SO4(2-) as anions in oligotrophic surface waters and evidence that NO3 concentrations have been increasing in recent decades in reviewed. The relationship between NO3- and the concentrations of cations (H+ and Al3+) known to be harmful to aquatic biota is also discussed. It is generally concluded that although direct proof of an association is lacking, circumstantial evidence suggests that atmospheric input of nitrogen to soils on certain 'sensitive' geologies may be having consequences for surface waters and the biota living in them, especially at certain times of the year, e.g. snowmelt.  相似文献   

5.
Visibility: science and regulation   总被引:50,自引:0,他引:50  
The 1999 Regional Haze Rule provides a context for this review of visibility, the science that describes it, and the use of that science in regulatory guidance. The scientific basis for the 1999 regulation is adequate. The deciview metric that tracks progress is an imperfect but objective measure of what people see near the prevailing visual range. The definition of natural visibility conditions is adequate for current planning, but it will need to be refined as visibility improves. Emissions from other countries will set achievable levels above those produced by natural sources. Some natural events, notably dust storms and wildfires, are episodic and cannot be represented by annual average background values or emission estimates. Sulfur dioxide (SO2) emission reductions correspond with lower sulfate (SO4(2-)) concentrations and visibility improvements in the regions where these have occurred. Non-road emissions have been growing more rapidly than emissions from other sources, which have remained stable or decreased since 1970. Simpler models representing transport, limiting precursor pollutants, and gas-to-particle equilibrium should be used to understand where and when emission reductions will be effective, rather than large complex models that have insufficient input and validation measurements. Examples of model-based source attribution show large differences among estimates from various modeling systems and with ambient measurements.  相似文献   

6.
This study evaluates chemical trends of seven acidified reservoirs and 22 tributaries in the Erzgebirge from 1993 to 2003. About 85% of these waters showed significantly (p < 0.05) declining concentrations of protons (-69%), nitrate (-41%), sulfate (-27%), and reactive aluminum (-50% on average). This reversal is attributed to the intense reduction of industrial SO2 and NOx emissions from formerly high levels, which declined by 99% and 82% in the German-Czech border region between 1993 and 1999. The deposition rates of protons and sulfur decreased by 70-90%. Since 1993, the dry deposition of total inorganic nitrogen diminished to a minor degree, but the wet deposition remained unchanged. The surface waters reflect a substantial decrease in Al exchange processes, a release of sulfur previously stored in soils, and an uptake of nitrate by forest vegetation. The latter effect may be supported by soil protection liming which contributed to the chemical reversal in almost 20% of the study waters.  相似文献   

7.
浙江省酸雨的空间分布格局及其未来变化趋势预测   总被引:13,自引:3,他引:10  
利用浙江省1992、2002年的酸雨监测数据,并利用RAINS-ASIA模型模拟了1990-2030年浙江省酸雨前体物(SO2)的排放量,以及酸沉降超临界负荷面积占研究区域面积比例的变化情况.结果表明,浙江省的酸雨分布范围不断扩大、危害程度不断加重;未来一个时期内,SO2排放量都会维持在较高的水平;酸沉降超临界负荷面积所占比例在经历较快的增长阶段之后,会维持在较为恒定的水平,并呈现出明显的时滞性.  相似文献   

8.
Air pollution and forest health: toward new monitoring concepts   总被引:4,自引:0,他引:4  
It is estimated that 49% of forests (17 million km(2)) will be exposed to damaging concentrations of tropospheric O(3) by 2100. Global forest area at risk from S deposition may reach 5.9 million km(2) by 2050, despite SO(2) emission reductions of 48% in North America and 25% in Europe. Although SO(2) levels have decreased, emissions of NO(x) are little changed, or have increased slightly. In some regions, the molar SO(4)/NO(3) ratio in precipitation has switched from 2/1 to near 1/1 during the past two decades. Coincidentally, pattern shifts in precipitation and temperature are evident. A number of reports suggest that forests are being affected by air pollution. Yet, the extent to which such effects occur is uncertain, despite the efforts dedicated to monitoring forests. Routine monitoring programmes provide a huge amount of data. Yet in many cases, these data do not fit the conceptual and statistical requirements for detecting status and trends of forest health, nor for cause-effect research. There is a clear need for a re-thinking of monitoring strategies.  相似文献   

9.
This paper analyzes the air quality impacts of coal-fired power plants in the northern passageway of the West-East Power Transmission Project in China. A three-layer Lagrangian model called ATMOS, was used to simulate the spatial distribution of incremental sulfur dioxide (SO2) and coarse particulate matter (PM10) concentrations under different emission control scenarios. In the year 2005, the emissions from planned power plants mainly affected the air quality of Shanxi, Shaanxi, the common boundary of Inner Mongolia and Shanxi, and the area around the boundary between Inner Mongolia and Ningxia. In these areas, the annually averaged incremental SO2 and PM10 concentrations exceed 2 and 2.5 microg/m3, respectively. The maximum increases of the annually averaged SO2 and PM10 concentrations are 8.3 and 7.2 microg/m3, respectively, which occur around Hancheng city, near the boundary of the Shaanxi and Shanxi provinces. After integrated control measures are considered, the maximum increases of annually averaged SO2 and PM10 concentrations fall to 4.9 and 4 microg/m3, respectively. In the year 2010, the areas affected by planned power plants are mainly North Shaanxi, North Ningxia, and Northwest Shanxi. The maximum increases of the annually averaged SO2 and PM10, concentrations are, respectively, 6.3 and 5.6 microg/m3, occurring in Northwest Shanxi, which decline to 4.4 and 4.1 microg/m3 after the control measures are implemented. The results showed that the proposed power plants mainly affect the air quality of the region where the power plants are built, with little impact on East China where the electricity will be used. The influences of planned power plants on air quality will be decreased greatly by implementing integrated control measures.  相似文献   

10.
Natural attenuation of contaminants in groundwater depends on an adequate supply of electron acceptors to stimulate biodegradation. In an alluvial aquifer contaminated with leachate from an unlined municipal landfill, the mechanism of recharge infiltration was investigated as a source of electron acceptors. Water samples were collected monthly at closely spaced intervals in the top 2 m of the saturated zone from a leachate-contaminated well and an uncontaminated well, and analyzed for delta(18)O, delta(2)H, non-volatile dissolved organic carbon (NVDOC), SO(4)(2-), NO(3)(-) and Cl(-). Monthly recharge amounts were quantified using the offset of the delta(18)O or delta(2)H from the local meteoric water line as a parameter to distinguish water types, as evaporation and methanogenesis caused isotopic enrichment in waters from different sources. Presence of dissolved SO(4)(2-) in the top 1 to 2 m of the saturated zone was associated with recharge; SO(4)(2-) averaged 2.2 mM, with maximum concentrations of 15 mM. Nitrate was observed near the water table at the contaminated site at concentrations up to 4.6 mM. Temporal monitoring of delta(2)H and SO(4)(2-) showed that vertical transport of recharge carried SO(4)(2-) to depths up to 1.75 m below the water table, supplying an additional electron acceptor to the predominantly methanogenic leachate plume. Measurements of delta(34)S in SO(4)(2-) indicated both SO(4)(2-) reduction and sulfide oxidation were occurring in the aquifer. Depth-integrated net SO(4)(2-) reduction rates, calculated using the natural Cl(-) gradient as a conservative tracer, ranged from 7.5x10(-3) to 0.61 mM.d(-1) (over various depth intervals from 0.45 to 1.75 m). Sulfate reduction occurred at both the contaminated and uncontaminated sites; however, median SO(4)(2-) reduction rates were higher at the contaminated site. Although estimated SO(4)(2-) reduction rates are relatively high, significant decreases in NVDOC were not observed at the contaminated site. Organic compounds more labile than the leachate NVDOC may be present in the root zone, and SO(4)(2-) reduction may be coupled to methane oxidation. The results show that sulfur (and possibly nitrogen) redox processes within the top 2 m of the aquifer are directly related to recharge timing and seasonal water level changes in the aquifer. The results suggest that SO(4)(2-) reduction associated with the infiltration of recharge may be a significant factor affecting natural attenuation of contaminants in alluvial aquifers.  相似文献   

11.
The sulphur content and sulphur isotopic composition of Sphagnum as well as anionic compositions and sulphur isotope ratios of rainwater inputs and bog waters have been measured at Thorne Moors, a raised bog in eastern England. Rainwater sulphate isotopic composition shows the sulphur input at this site to be dominated by anthropogenic pollution from fossil fuel burning. Strong depletion of sulphate (low SO4(2-)/Cl-) and enrichment in 34S in sulphate occurs at depth in the bog porewaters due to bacterial sulphate reduction. Some surface waters have low SO4(2-)/Cl-) and are 34S enriched due to removal of sulphate by downward diffusion into a sulphate-reducing zone. Other sites have high SO4(2-)/Cl-) which appears to result from oxidation of organically bound sulphur in the peat. Sulphur is present in Sphagnum at around 0.2% by weight and is depleted by 0 to -9 per thousand in the heavier 34S isotope compared to sulphate. Comparison with similar data from pristine coastal sites shows that sulphur incorporation into Sphagnum is enhanced in the polluted site (as Sphagnum sulphur concentrations are higher at lower total sulphur inputs) and that sulphur incorporation is accompanied by a smaller isotopic shift than in the pristine sites. The data support a model of preferential incorporation of partially reduced sulphur species (probably HSO3-) into Sphagnum. In pristine sites these are only available as oxidation products of sulphide formed by sulphate reduction and are 32S depleted. In polluted sites this source is augmented by sulphur(IV) species in atmospheric inputs and the resultant mixture is less depleted in 32S. Thus, in the polluted sites more HSO3- is available for uptake and the isotopic shift between Sphagnum and aqueous sulphur species is smaller.  相似文献   

12.
GOAL, SCOPE AND BACKGROUND: One of the principal experimental variables which effect the results of phosphorus (P) sorption studies is the ionic composition, in addition to both species and concentrations of the contacting solution. In spite of the realization that ionic species, concentrations and their compositions effect P sorption and/or desorption, most of the salt-related studies are confined to Cl- (anion) in association with different cations. While the knowledge about the comparative response of P to Cl- and SO4(2-) ions was lacking, the current study was conducted to evaluate the comparative effects of anions (in association with cations) on inorganic P release and P fractions in the soil. METHODS: The test soil was amended with livestock compost manure (OP); KH2PO4 (IPk) or Ca(H2PO4)2 (IPc) at a rate of 1ppm. Soil was subjected to one salt and nine subsequent water extractions and different P fractions were measured. Four salt types, NaCl, Na2SO4, KCl and K2SO4, were used at levels of 0.5 M. RESULTS: Irrespective of P sources, P release was substantially increased in the salt-pretreated soil as compared to the non-saline soil. Sulfate salts released more P in subsequent water extractions than Cl-. Phosphorus release decreased for salt types with Na2SO4 > NaCl > K2SO4 > KCl and for P sources with OP approximately IPk > Control (without P application) > IPc, respectively. DISCUSSION: No previous study was found to compare the results of more P release by SO4(2-) than Cl- salt. Most of the previous studies focused on anion sorption capacities, but the mechanism for their adsorption is not fully known. Most of the authors suggested that the mechanisms of SO4(2-) and PO4(3-) adsorption are similar, and that both ions compete for the same sorption sites (Kamprath et al. 1956, Couto et al. 1979, Pasricha and Fox 1993). Although adsorbed SO4(2-) does not compete strongly with PO4(3-), there is likely to be some competition for sorption between these anions which may cause comparatively more P release by SO4(2-) than Cl- salts. Higher P release by Na-saturation could be due to the release of P associated with oxide surfaces or due to dissolution of Ca-P phases (Curtin et al. 1987). CONCLUSIONS: Study clearly showed that not only cations species differ for P desorption capacity, but associated anions also play a vital role in the fate of P under saline environments. Synergetic effects exist between Na and SO4(2-) ions which enhanced the P release. This study has also confirmed the fact that P from organic sources is available as well as from inorganic P sources. However, P release depends more on the type of P source applied than on total P. RECOMMENDATIONS AND PERSPECTIVES: It is highly recommended that more than one anion species must be used in the research plans for evaluating the P response in a saline environment. The results have important implications from the point of view of research, as most of the researchers focus on different cations only for evaluating P response to salts from an environmental point of view. However, our study has made it clear that anions in association with cations differed for their effects on P release.  相似文献   

13.
Air quality impacts of power plant emissions in Beijing   总被引:8,自引:0,他引:8  
The CALMET/CALPUFF modeling system was applied to estimate the air quality impacts of power plants in 2000 and 2008 in Beijing, and the intake fractions (IF) were calculated to see the public health risks posed. Results show that in 2000 the high emission contribution induced a relatively small contribution to average ambient concentration and a significant impact on the urban area (9.52 microg/m(3) of SO(2) and 5.29 microg/m(3) of NO(x)). The IF of SO(2), NO(x) and PM(10) are 7.4 x 10(-6), 7.4 x 10(-6) and 8.7 x 10(-5), respectively. Control measures such as fuel substitution, flue gas desulfurization, dust control improvement and flue gas denitration planned before 2008 will greatly mitigate the SO(2) and PM(10) pollution, especially alleviating the pressure on the urban area to reach the National Ambient Air Quality Standard (NAAQS). NO(x) pollution will be mitigated with 34% decrease in concentration but further controls are still needed.  相似文献   

14.
The Fenton reaction has been applied to the degradation of 4-chlorophenol in aqueous solutions containing various anions. The rate of the reaction was found to decrease in the following order of anions (at the same concentrations): CIO (4) ~ NO (3)- > SO(4) (2-) > CI(-)> >HPO(4) (2-) > HCO(3)(-). Degradation of the pollutant containing the above anions at concentrations typical of those found in groundwater and surface waters was affected in a similar way. The results are discussed in terms of the effects of these anions on the rates of the oxidation of ferrous anion as well as on their role in the scavenging of hydroxyl radical  相似文献   

15.
In Polar regions subject to acid precipitation, the spring flood period is swift and can be divided into three phases. In phase one, dilution and anion substitution by SO4 controls episodic acidification. Phase two is characterized by interaction of snowmelt water with the catchment. A combination of several factors contributes to declines in pH and ANC. In forest and wetland ecosystems, organic acids greatly contribute to the pH depression in the streams. In the coastal tundra and forest-tundra zones, "salt-effect" acidification predominantes. The increase in toxic forms of trace (Ni, Cu) and rare (Fe, Al, Mn) elements during pH depressions may create stress conditions for the fauna of polar fresh waters during a flood period.  相似文献   

16.
To evaluate the changes in sulphur pools in response to acidic deposition, two studies were made-one in southwest Sweden where podzolic B horizons originally sampled in 1951 were resampled in 1989. At the Norrliden site, northern Sweden, sulphur pools in control plots were compared to plots that had been subjected to H(2)SO(4) application between 1971 and 1976. The results show that in southwest Sweden neither organic S nor extractable SO(4)(2-) increased significantly over the 38-year period, despite a decreasing pH and a high S deposition. At Norrliden, about 37% of the applied S was still remaining in the upper and central parts of the Bs horizon, most of which was inorganic sulphate. These contrasting results are explained by intrinsic differences in the soil organic carbon status between the sites-in southwest Sweden, organic carbon concentrations were high which inhibited SO(4)(2-) adsorption. Low organic carbon concentrations and high extractable Fe/Al concentrations promoted SO(4)(2-) adsorption and caused a low subsequent SO(4)(2-) desorption rate at the Norrliden site. The results suggest that sulphate adsorption may be an important mechanism which delays the response in soil chemistry to H(2)SO(4) deposition, provided that soil organic carbon concentrations are low. Organic S retention was not shown to be an important S retention mechanism in any of the sites studied.  相似文献   

17.
Three sediment cores, collected nearby the effluent of a chlor-alkali industry, were sliced in 0.5-cm layers and centrifuged for pore water extraction. Mercury, Fe and Mn were determined in the solids as total concentration, hydroxylamine extractable fraction and HCl extractable fraction. Sulphur was determined in the HCl extraction. Total and reactive mercury, chlorinity, S(2-), SO(4)(2-), total Fe, and total Mn were measured in pore waters. The solids contained 3.0-60 nmol g(-1) of total Hg and pore waters 70-5800 pM of total Hg and 1.8-76 pM of reactive mercury. Pore waters presented 2.3-94 times more sulphate than the overlying estuarine waters due to the input from the industry. In layers where hydroxylamine extractable Fe exhibited a broad maximum (precipitation of Fe-oxides) sulphate was reduced to S(2-). The competition between the high content of SO(4)(2-) and Fe(III) as electron acceptors, in chemical reactions occurring in the upper sediments, may explain the co-existence of S(2-) and Fe-oxides in the same layers. Mercury was detected in the hydroxylamine extracts (20-29 nmolg(-1)) in the layers where Fe-oxides were formed, and reactive dissolved Hg showed minimum concentrations. The excess of sulphate in pore waters favoured the abundant Fe-oxides in the upper solid sediments, which appear to work as a barrier limiting the escape of mercury to the water column.  相似文献   

18.
Open pollinated families of loblolly pine differing in resistance to fusiform rust disease were screened in laboratory studies for responses to gaseous air pollutants. Twenty families were given acute exposures (2 fumigations for 4 h each) to SO(2) (0.4-1.0 ppm), O(3) (0.25 ppm), SO(2) (0.4-1.0 ppm) + O(3) (0.25 ppm) and control. Analyses of variance were performed to evaluate the treatment effects of these air pollutants on percent foliar injury, and to determine whether the families responded differentially to the air pollution treatments. Treatment effects were significant, with the combination treatment of SO(2) + O(3) producing a higher percentage of foliar injury than the controls; however, injury levels were very low and may not be of biological significance. Subsequently, twelve families were grown in two soil types for exposure to chronic levels of SO(2) (0.06 ppm), O(3) (0.07 ppm), SO(2) (0.06 ppm) + O(3) (0.07 ppm) and control. The families were then ranked for decreased primary shoot growth, shoot dry weight, root dry weight, total plant dry weight and root/shoot ratio after exposure to air pollution treatments. Air pollution treatments as a main effect were significant for only one of five growth parameters measured, that of primary shoot growth. The main effect of family, and the interaction of family and air pollution treatments, were significant for most growth parameters measured. In general, O(3) alone and in combination with SO(2) reduced growth more than SO(2) alone. Fumigation with O(3) reduced growth of two families in comparison with control groups, whereas SO(2) alone produced decreased growth in one family and stimulated growth in three families. Treatment with O(3) alone produced higher root/shoot ratios than fumigation with charcoal-filtered air in two families. Overall, families which were fast growers under control conditions maintained their ranking after exposure to air pollution. Families producing less growth in charcoal-filtered air also produced less growth under various air pollution regimes. Results indicated that these families exhibited a high degree of resistance to air pollution injury. Growth responses of seedlings may not reflect family differences in long-term productivity. No relationship was apparent between fusiform rust resistance and growth reductions due to air pollutants.  相似文献   

19.
Catalyst recovery studies were conducted for gasified chars produced from steam gasification of Illinois #6 coal catalyzed with two different catalyst systems. A ternary (43.5 mol% Li2CO3-31.5 mol% Na2COr-25 mol% K2CO3) and a binary (29 mol% Na2CO3-71 mol% K2CO3) eutectic catalyst system were used for gasifying coal. Various extraction schemes, such as water extraction, H2SO4 extraction, and acetic acid extraction, were evaluated with respect to their extraction efficiencies. Effects of major process variables, such as solvent-to-char ratio, mixing time, temperature, and concentration, on the extraction efficiency were evaluated. A process schematic for the entire catalyst recovery, regeneration, and recycle scheme was developed and the preliminary process economics were determined based on these extraction schemes. H2SO4 extraction was found to be the most desirable. It also turned out to be more attractive than a once-through throwaway system.  相似文献   

20.
In the vicinity of a large ammonia emission area, dry and wet deposition of acidifying and eutrophying compounds onto Douglas Fir forests was studied by sampling throughfall, stemflow and bulk precipitation. Deposition amounts of NH(4)(+) and SO(4)(2-) were recognised to be among the highest of Central Europe, resulting in extremely high inputs of (potential) acid to the forest soils (13.1 kEq ha(-1) year(-1)). The contribution of NH(3) emissions from agriculture to the total acid deposition to the forests was 52%. The total nitrogen deposition amounted to 115.0 kg ha(-1) year(-1), 83% originating from NH(3) emissions and 17% from NO(x) emissions. Calculated mean dry deposition velocities of NH(3) and SO(2) were much larger than reported in the literature. A synergistic effect between NH(3) and SO(2) in the process of dry deposition is suggested and evidence for this effect is discussed. When deposition models do not take this interaction into account, they will underestimate NH(3) and SO(2) deposition amounts in areas with intensive animal husbandry.  相似文献   

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