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1.
Acidic (acid neutralizing capacity [ANC] < or = 0) surface waters in the United States sampled in the National Surface Water Survey (NSWS) were classified into three groups according to their probable sources of acidity: (1) organic-dominated waters (organic anions > SO4*; (2) watershed sulphate-dominated waters (watershed sulphate sources > deposition sulphate sources); and (3) deposition-dominated waters (anion chemistry dominated by inputs of sulphate and nitrate derived from deposition). The classification approach is highly robust; therefore, it is a useful tool in segregating surface waters into chemical categories. An estimated 75% (881) of acidic lakes and 47% (2190) of acidic streams are dominated by acid anions from deposition and are probably acidic due to acidic deposition. In about a quarter of the acidic lakes and streams, organic acids were the dominant source of acidity. In the remaining 26% of the acidic streams, watershed sources of sulphate, mainly from acid mine drainage, were the dominant source of acidity.  相似文献   

2.
This study was conducted to evaluate the potential applicability of an in situ biological reactive barrier system to treat nitrate-contaminated bank filtrate. The reactive barrier consisted of sulfur granules as an electron donor and autotrophic sulfur-oxidizing bacteria as a biological component. Limestone was also used to provide alkalinity. The results showed that the autotrophic sulfur oxidizers were successfully colonized on the surfaces of the sulfur particles and removed nitrate from synthetic bank filtrate. The sulfur-oxidizing activity continuously increased with time and then was maintained or slightly decreased after five days of column operation. Maximum nitrate removal efficiency and sulfur oxidation rate were observed at near neutral pH. Over 90% of the initial nitrate dissolved in synthetic bank filtrate was removed in all columns tested with some nitrite accumulation. However, nitrite accumulation was observed mainly during the initial operation period, and the concentration markedly diminished with time. The nitrite concentration in effluent was less than 2 mg-N/l after 12 days of column operation. When influent nitrate concentrations were 30, 40, and 60 mg-N/l and sulfur content in column was 75%, half-order autotrophic denitrification reaction rate constants were 31.73 x 10(-3), 33.3 x 10(-3), and 36.4 x 10(-3) mg(1/2)/l(1/2)min, respectively. Our data on the nitrate distribution profile along the column suggest that an appropriate wall thickness of a reactive barrier for autotrophic denitrification may be 30 cm when influent nitrate concentration is less than 60 mg-N/l.  相似文献   

3.
Long-term changes in stream water chemistry in the upper Duddon catchment (southwest Lake District, UK) were investigated. Ten streams were sampled and analysed weekly during 1998, and the results compared with data for the early 1970s and 1986. The waters exhibited a range of pH, average values for 1998 being 5.04-7.04. For all the streams, the average pH in 1998 was greater than that during 1971-73. Statistical analysis was carried out, using the 1970s data to estimate the magnitude of inter-annual variation, and taking discharge into account on the basis of antecedent rainfall. The results showed that for two of the streams the pH increase was significant at the 2.5% level, while for a further three it was significant at the 10% level. Comparison of the 1998 concentrations of nitrate and non-marine sulphate with data obtained for five streams in 1973-74 showed that average nitrate concentration had increased from 11 to 20 microeq dm(-3) while that of non-marine sulphate had decreased from 94 to 50 microeq dm(-3). For four of the streams, comparisons were also made between the 1998 data and those for 1986. In three cases, pH in 1998 was generally higher, and Al generally lower, than the values for 1986, but in the fourth case little difference was evident. The present results support observations for five nearby standing waters, strengthening the evidence for a general reversal of acidification in the southwest part of Lake District, due to a decline in the deposition of pollutant sulphur.  相似文献   

4.
During four intensive observation periods in 1992 and 1993, dry deposition of nitrogen dioxide (NO(2)) and ammonia (NH(3)), and wet deposition of nitrogen (N) were determined. The measurements were carried out in a small, extensively managed litter meadow surrounded by intensively managed agricultural land. Dry deposition of NH(3) was estimated by the gradient method, whereas eddy correlation was used for NO(2). Rates of dry deposition of total nitrate (= nitric acid (HNO(3)) + nitrate (NO(3)(-))), total nitrite (= nitrous acid (HONO) + nitrite (NO(2)(-))) and aerosol-bound ammonium (NH(4)(+)) were estimated using deposition velocities from the literature and measured concentrations. Both wet N deposition and the vertical NH(3) gradient were measured on a weekly basis during one year. Dry deposition was between 15 and 25 kg N ha(-1) y(-1), and net wet deposition was about 9.0 kg N ha(-1) y(-1). Daily average NO(2) deposition velocity varied from 0.11 to 0.24 cm s(-1). Deposition velocity of NH(3), was between 0.13 and 1.4 cm s(-1), and a compensation point between 3 and 6 ppbV NH(3) (ppb = 10(-9)) was found. Between 60 and 70% of dry deposition originated from NH(3) emitted by farms in the neighbourhood. It is concluded that total N deposition is exceeding the critical load for litter meadows, is highly correlated to local NH(3) emissions, and that NH(3) is of utmost importance with respect to possible strategies to reduce N deposition in rural regions.  相似文献   

5.
The General Motors mobile Atmospheric Research Laboratory was situated in rural western Massachusetts in the Berkshire Mountains for 62 days during the summer of 1984. One purpose of this study was to determine the source regions of wet acid deposition for this northeastern U.S. location. First, to apportion the precursors (sulfate, sulfur dioxide and nitrate) to source regions, daily ambient air samples were analyzed for the precursors as well as for tracer species that are associated with particular sources. Factor and trajectory analyses were then used to deduce the contributions of the Midwest and the Northeast to these precursors. Finally, the contribution of the precursors to precipitation acidity was estimated by analyzing the chemical constituents in the rain during seven precipitation events. Averaged over the entire duration of the study, the data show that Northeast sources accounted for about 60% of the precipitation sulfate and nitrate, while Midwest sources accounted for about 30%. The balance (~ 10%) was accounted for by background sulfate. A more useful way of examining the data is according to the type of storm that caused the wet deposition. The site was affected by two basic types of storms: coastal low-pressure systems that traveled up the Atlantic Coast, and cold fronts that approached from the west. During the coastal lowpressure events, the Midwestern contribution to precipitation acidity was zero, as easterly flows from the Atlantic Ocean dominated. The cold front events, however, were all associated with southwesterly flows, and the Midwest contributions exceeded the Northeast contributions. During these events, the average Midwest contribution to precipitation acidity was about 50%. For all events, the ratio of sulfate to nitrate was approximately 2:1 on an equivalent basis. During the coastal lows, the relative nitrate contributions were the highest. It was estimated that particulate sulfate scavenging was responsible for about half of the sulfate in the rain, while the other half was due to in-cloud oxidation of gaseous sulfur dioxide.  相似文献   

6.
An intercomparison study involving eight long-range transport models for sulfur deposition in East Asia has been initiated. The participating models included Eulerian and Lagrangian frameworks, with a wide variety of vertical resolutions and numerical approaches. Results from this study, in which models used common data sets for emissions, meteorology, and dry, wet and chemical conversion rates, are reported and discussed. Model results for sulfur dioxide and sulfate concentrations, wet deposition amounts, for the period January and May 1993, are compared with observed quantities at 18 surface sites in East Asia. At many sites the ensemble of models is found to have high skill in predicting observed quantities. At other sites all models show poor predictive capabilities. Source–receptor relationships estimated by the models are also compared. The models show a high degree of consistency in identifying the main source–receptor relationships, as well as in the relative contributions of wet/dry pathways for removal. But at some locations estimated deposition amounts can vary by a factor or 5. The influence of model structure and parameters on model performance is discussed. The main factors determining the deposition fields are the emissions and underlying meteorological fields. Model structure in terms of vertical resolution is found to be more important than the parameterizations used for chemical conversion and removal, as these processes are highly coupled and often work in compensating directions.  相似文献   

7.
Throughfall was collected in a Scots pine forest exposed to about 14 microg m(-3) of both SO2 and NO2, and in a control forest with 1 microg m(-3) SO2 and < 1 microg m(-3) NO2. Precipitation was collected in a nearby open field. Collection was performed on an event basis during the whole vegetation period. Exposure was made by an open-air release system during the vegetation period, except during rain and at night. Additional sulfate deposition in the exposed forest (compared to control forest) was nearly equal to dry deposition of sulfur dioxide, as estimated with a stomatal conductance model adapted for the particular forest. It is thus concluded that essentially all of the dry deposited sulfur dioxide is eventually extracted and appears in throughfall-including the fraction that has been deposited through stomata. Attempts to relate net throughfall deposition to dry deposition of sulfate in the control forest were inconclusive, since a minor (10%) uncertainty in the water balance had a major influence on calculated deposition velocity for particulate sulfate. Nitrate throughfall deposition is about half of the open field wet deposition, both for the exposed and control forest. Thus, a long-term exposure with about 14 microg m(-3) NO2 decreased nitrate throughfall deposition.  相似文献   

8.
Intensive forest monitoring by means of harmonised methods has been conducted in Europe for more than a decade. Risks of atmospheric nitrogen and sulphur deposition are assessed by means of calculations of critical loads and their exceedances. In the present study throughfall and bulk deposition of nitrate (N-NO(3)), ammonium (N-NH(4)) and sulphate (S-SO(4)) show marked spatial patterns and temporal trends. In the period of observation (1999-2004), sulphate deposition on intensive monitoring plots decreased by about one quarter. This is in line with the reduction of S deposition by 70% since 1981 in Europe as a result of successful air pollution control politics under the Convention on Long-range Transboundary Air Pollution (CLRTAP). However, sulphate and especially nitrate and ammonium deposition were found to still exceed critical loads at many forest sites, indicating a continued need for further implementation of air pollution abatement strategies.  相似文献   

9.
Background Biomass burning is a source of carbon, sulfur and nitrogen compounds which, along with their photochemically generated reaction products, can be transported over very long distances, even traversing oceans. Chemical analyses of rain and fogwater samples collected in the mountaineous rain forest of south Ecuador show frequent episodes of high sulfate and nitrate concentration, from which annual deposition rates are derived comparable to those found in polluted central Europe. As significant anthropogenic sources are lacking at the research site it is suspected that biomass burning upwind in the Amazon basin is the major source of the enhanced sulfate and nitrate imput. Methods Regular rain and fogwater sampling along an altitude profile between 1800 and 3185 m has been carried out in the Podocarpus National Park close to the Rio SanFrancisco (3°58'S, 79°5'W) in southern Ecuador. pH values, electrical conductivity and chemical ion composition were measured at the TUM-WZW using standard methods. Results and Discussion Results reported cover over one year from March 2002 until May 2003. Annual deposition rates of sulfate were calculated ranging between 4 and 13 kg S/ha year, almost as high as in polluted central Europe. Nitrogen deposition via ammonia (1.5–4.4 kg N/ha year) and nitrate (0.5–0.8 kg N/ha year) was found to be lower but still much higher than to be expected in such pristine natural forest environment. By means of back trajectory analyses it can be shown that most of the enhanced sulfur and nitrogen deposition is most likely due to forest fires far upwind of the Ecuadorian sampling site, showing a seasonal variation, with sources predominantly found in the East/NorthEast during January–March (Colombia, Venezuela, Northern Brazil) and East/SouthEast during July–September (Peru, Brazil). Conclusion Our results show that biomass burning in the Amazon basin is the predominant source of sulfur and nitrogen compounds that fertilize the mountaineous rain forest in south Ecuador. Recommendation and Outlook The mountaineous rain forest in south Ecuador has developed on poor and acid soils, with low nutrient availability. The additional fertilization resulting from anthropogenic biomass burning constitutes a significant disturbance of this ecosystem, its functioning and biodiversity. Thus it is planned to employ isotope analyses for quantifying the pathways of nitrate and sulfate deposition in these natural forests.  相似文献   

10.
Data for precipitation and acidic pollutant concentration from the MAP3S network in the eastern United States were analyzed to assess the probability distributions of acidic deposition and the spatial and temporal character of high deposition events (or ‘episodes’). About 20% of the precipitation events account for about 55% of the deposition of the major species (sulfur, nitrate, free hydrogen, and ammonium). The mean ‘episodicity’, as defined by Smith and Hunt (Atmospheric Environment12, 461–477, 1978), is 7%; this is not considered highly episodic. The distribution characteristics are spatially quite uniform over the MAP3S region, suggesting a homogeneous pollution-exposure environment. Occurrences of the leading deposition events generally follow the seasonal trends in concentration, and the major episodes usually account for about 10% or less of a given year's total deposition. Most episode events are characterized by above-normal values of both precipitation amount and concentration.  相似文献   

11.
de Wit HA  Wright RF 《Ambio》2008,37(1):56-63
Fluctuations in the 20-year record of nitrate (NO3) and total organic carbon (TOC) concentrations and fluxes in runoff at the small headwater catchment Storgama, southern Norway, were related to climate and acid deposition. The long-term decline in NO3 related to reduced NO3 deposition and increased winter discharge, whereas the long-term increase in TOC related to reduced sulfur deposition. Multiple regression models describing long-term trends and seasonal variability in these records were used to project future concentrations given scenarios of climate change and acid deposition. All scenarios indicated reduced NO3 fluxes and increased TOC fluxes; the largest projected changes for the period 2071-2100 were -86% and +24%, respectively. Uncertainties are that the predicted future temperatures are considerably higher than the historical record. Also, nonlinear responses of ecosystem processes (nitrogen [N] mineralization) to temperature, N-enrichment of soils, and step-changes in environmental conditions may affect future leaching of carbon and N.  相似文献   

12.
Seasonal snowpack chemistry data from the Rocky Mountain region of the US was examined to identify long-term trends in concentration and chemical deposition in snow and in snow-water equivalent. For the period 1993–2004, comparisons of trends were made between 54 Rocky Mountain Snowpack sites and 16 National Atmospheric Deposition Program wetfall sites located nearby in the region. The region was divided into three subregions: Northern, Central, and Southern. A non-parametric correlation method known as the Regional Kendall Test was used. This technique collectively computed the slope, direction, and probability of trend for several sites at once in each of the Northern, Central, and Southern Rockies subregions. Seasonal Kendall tests were used to evaluate trends at individual sites.Significant trends occurred during the period in wetfall and snowpack concentrations and deposition, and in precipitation. For the comparison, trends in concentrations of ammonium, nitrate, and sulfate for the two networks were in fair agreement. In several cases, increases in ammonium and nitrate concentrations, and decreases in sulfate concentrations for both wetfall and snowpack were consistent in the three subregions. However, deposition patterns between wetfall and snowpack more often were opposite, particularly for ammonium and nitrate. Decreases in ammonium and nitrate deposition in wetfall in the central and southern rockies subregions mostly were moderately significant (p<0.11) in constrast to highly significant increases in snowpack (p<0.02). These opposite trends likely are explained by different rates of declining precipitation during the recent drought (1999–2004) and increasing concentration. Furthermore, dry deposition was an important factor in total deposition of nitrogen in the region. Sulfate deposition decreased with moderate to high significance in all three subregions in both wetfall and snowpack. Precipitation trends consistently were downward and significant for wetfall, snowpack, and snow-telemetry data for the central and southern rockies subregions (p<0.03), while no trends were noted for the Northern Rockies subregion.  相似文献   

13.
The South Pennines, an area of acid-sensitive geology at the centre of a major industrial region, have undergone perhaps the most severe historic exposure to sulphur and nitrogen deposition in the UK. This study addresses a lack of existing research on the region by presenting the findings of a survey of 62 surface waters sampled during a 1-week period in April 1998. Results indicate that acidification in the region is acute; 27 of the sampled surface waters had a negative acid neutralising capacity (ANC) and 28 had a pH below 5.0. Minimum recorded pH values were below 4.0. Non-marine sulphate levels were extremely high (median 222 microeq/1), and widespread high nitrate concentrations (median 41 microeq/1) suggest that soils in the region as a whole may be at an advanced stage of nitrogen saturation. A consistent relationship was identified between site acidity and the balance between the major weathering-derived cations, calcium and magnesium, and sulphate. This could in turn be linked to catchment soil type and land use, with the most acidic conditions occurring in peat-dominated catchments, where weathering is minimal and the influence of atmospheric deposition most pronounced. Percentage of peat in each catchment was the single best predictor of surface water acidity. Nitrate concentrations, although not a dominant control on acidity, varied significantly according to land use. Elevated concentrations were observed in catchments containing forestry, due to enhanced deposition inputs, and in catchments containing improved land, linked to fertiliser use. Ammonium concentrations, although low at most catchments, were a significant component of the inorganic nitrogen total in a number of surface waters draining waterlogged peat catchments.  相似文献   

14.
Measurement of the deposition of sedimenting particles requires a sampling device, which avoids simultaneous deposition of gases and aerosols to the collection surface. A sampler constructed for the purpose of collecting rain and sedimenting particles is described and characterized in detail, in particular with regard to its collection efficiency for rain. Its collection properties for gases and aerosols are shown to be negligible. From two years of sampling at different heights it was found that resuspension of particles and co-condensation of gases near the plant canopy may lead to a major overestimation of bulk deposition. As a consequence, the extension towards the canopy of the constant flux layer for sedimenting particles has to be determined experimentally. Bulk deposition of sodium, potassium, magnesium, calcium, lead, copper, cadmium, manganese, iron, ammonium, nitrate, phosphate, sulfate, total sulfur and chloride at Braunschweig-V?lkenrode, Southeast Lower Saxony, Germany, were recorded for six years. During this period a considerable decrease was observed in the deposition of lead, cadmium, nitrate, sulfate and total sulfur.  相似文献   

15.
Abstract

The Interagency Monitoring of Protected Visual Environments (IMPROVE) particulate monitoring network has been collecting aerosols for visibility apportionment at remote sites in the United States since 1988. The measurements include the major PM2.5 components, such as sulfur, carbon, and nitrate, and trace elements, such as selenium. This paper will examine the relationship between the sulfurs and selenium concentrations at 61 sites for samples collected in the seasonal year 1993. Maps of mean sulfur and selenium measurements in summer 1993 and winter 1993-1994 indicate that there are well-defined regional patterns for both elements, with concentrations in the Appalachian region that are ten times those in areas of the Pacific Northwest. The S/Se ratios of means are relatively uniform across the United States, at around 2000 in summer and 1000 in winter, indicating a strong sulfur-selenium relationship. The role of conversion of S02 to sulfate can also be deduced from the means. For individual samples taken during summer 1993, there is a high correlation between the two variables in the East, especially at sites in the Northeast, where the correlation coefficients (r2) are around 0.9. In the West, the correlation is much lower. This is attributed to fewer sources and differing emission factors.  相似文献   

16.
The influence of atmospheric deposition on the chemical characteristics of soil solutions in a small catchment area in NW Spain was studied. The soils, developed from slates, were sampled from seven sites supporting different forms of vegetation (deciduous and pine forest and heath). Soil solutions were extracted, by the column displacement method, from soil samples collected monthly from March 1992 until November 1993. The solutions were acidic with a low content of basic cations. The most common ions in all horizons were Cl(-) and Na(+), due to marine influence. In the surface horizons (0-10 cm), relatively high concentrations of SO(2-)4 (150-380 micromol litre(-1)) and Zn (approximately 2 micromol litre(-1)) were obtained, with good correlation between the two ions. These results, along with the prevalence of inorganic forms of Al (50-90% of total Al), were related to the effects of acidic deposition in the catchment area. The more rapid breakdown of litter in the soils under deciduous forest explains the greater ionic concentrations obtained in these solutions.  相似文献   

17.
Maps of the distribution of environmental pollution by sulfur (S), zinc (Zn), cadmium (Cd), lead (Pb), copper (Cu), and arsenic (As) for the territory of Poland and the Warsaw (Warszawa) district were developed on the basis of chemical analysis of Scots pine (Pinus sylvestris L.) needles collected from randomly selected sampling points during 1983-1985. The maps show deposition zones for the studied elements and can help in identification of sources and directions of air pollution dispersion. This study indicated that vegetation in Poland is greatly endangered by sulfur dioxide (SO(2)) and other sulfurous air pollutants, whereas Zn, Cd, Pb, and As do not pose an immediate threat to vegetation in most of the country's territory. However, in the urban-industrial agglomeration of Katowice-Cracow, very high pollution with Z, Cd, Pb and As could limit growth and development of some sensitive plant species. Higher than normal levels of As in some areas of Poland (Upper Silesia, Glogow-Lubin Copper Region, and areas close to the Russian border near Braniewo) might affect the health of humans and animals. Results of this study indicated that Poland's environment was not contaminated with Cu.  相似文献   

18.
Abstract

Chemical mass balance receptor models (CMBs) use measured pollutant concentrations, along with source information, to apportion the contributions of primary sources to the measured concentrations. CMBs can be used to evaluate the accuracy of the emission inventories that underlie State Implementation Plan (SIP) modeling, by providing an allocation of emissions to individual source categories. CMBs, however, traditionally have not accounted for the chemical reaction and differential deposition or fractionation that occur between the source and receptor. This means that they have historically had severe limitations in apportioning secondary particulate matter (PM), which is an especially important component of fine PM (PM2.5). Stafford and Liljestrand developed a method to account for fractionation in CMBs using depletion factors based on a solution of the steady-state advection-dispersion equation, including gravitational settling, dry deposition, and first-order chemical reaction. In the research presented here, the method of Stafford and Liljestrand was tested using gaseous and PM ambient concentration data from the Los Angeles, CA, air shed, along with traffic source profiles specific to Los Angeles and the CMB7 receptor model of the U.S. Environment Protection Agency. Including fractionation increased nitrate apportioned from 5% and 6% to 83% and 86% for Claremont, CA, and Long Beach, CA, respectively. This is significant, because CMBs have historically had difficulty apportioning nitrate. Including fractionation increased the ammonium apportioned by a factor of 7. The method could be used in future case studies to apportion secondary organic carbon as well.  相似文献   

19.
Nitrate and water supplies in the United Kingdom   总被引:9,自引:0,他引:9  
Nitrate concentrations in UK waters are rising, with the highest levels occurring in the south and east of England, particularly Lincolnshire, Cambridgeshire and East Anglia. The source of the nitrate is arable agriculture where intensification in the last few decades has increased nitrate leaching from soils into both surface and underground waters. Concentrations in underground waters are expected to reach 150 to 200 mg litre(-1) nitrate (i.e. NO(3)) in the future, if agricultural losses remain stable. No widespread environmental deterioration due to nitrate has been observed in rivers or lakes. Excessive concentrations of nitrate in drinking waters can cause methaemoglobinaemia (blue-baby syndrome) in bottle-fed infants and the government Chief Medical Officer has recommended that a maximum concentration of 100 mg litre(-1) is appropriate for public water supplies in the UK. This level has not been exceeded in public water supplies in the UK, but maintaining it has cost approximately 15m pounds in borehole replacement and arrangements to blend high and low nitrate waters. Future capital costs are estimated as 37m pounds over the next 20 years. The European Economic Community (EEC) Drinking Water Directive (80/778/EEC) sets a maximum admissible concentration of 50 mg litre(-1) nitrate. Adherence to this standard will cost 199m pounds over the same period.  相似文献   

20.
Concern regarding the impacts of continued nitrogen and sulfur deposition on ecosystem health has prompted the development of critical acid load assessments for forest soils. A critical acid load is a quantitative estimate of exposure to one or more pollutants at or above which harmful acidification-related effects on sensitive elements of the environment occur. A pollutant load in excess of a critical acid load is termed exceedance. This study combined a simple mass balance equation with national-scale databases to estimate critical acid load and exceedance for forest soils at a 1-km(2) spatial resolution across the conterminous US. This study estimated that about 15% of US forest soils are in exceedance of their critical acid load by more than 250eqha(-1)yr(-1), including much of New England and West Virginia. Very few areas of exceedance were predicted in the western US.  相似文献   

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