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1.
The chemical composition of winter and spring cloud water sampled at 1620 masl elevation on Mt Rigi in central Switzerland was dominated by NO3, SO42−, NH4+ and H+. A wide range of concentration levels was observed, with maxima of 3700, 1800 and 4600 micronormal for NO3, SO42− and NH4+, respectively. Concentrations at a lower elevation (1030 masl) site on the mountain were higher due to lower cloud liquid water contents and higher pollutant levels at that site. The lowest pH observed was 2.95; large concentrations of NH3 in the region prevented pH values from falling even lower. A comparison of simultaneously sampled cloud water and precipitation revealed much higher concentrations for most species in the cloud water, except in one case of extreme precipitation riming when the concentrations in the two phases converged. An exception to the pattern was H+; at times the precipitation was more acidic than the cloud water. The chemical composition of the cloud drops varied with drop size. Drops smaller than 10 μm diameter were enriched in NO3, SO42− and NH4+ relative to larger drops. Since the larger drops are the ones most effeciently captured by snow crystals, knowledge of their composition is essential to understanding the chemical implications of accretional growth of precipitation.  相似文献   

2.
The chemical composition of cloudwater in the Sierra Nevada is dominated by NO3, SO42−, and NH4+. Cloudwater pH is determined largely by the balance between the concentrations of these three species, although inputs of formic and acetic acid also are believed to be important, particularly when anthropogenic inputs are small. Cloudwater samples collected in Sequoia National Park (SNP) exhibited pH values ranging from 3.9 to 6.5; Yosemite National Park (YNP) cloudwater samples had pH values ranging from 3.8 to 5.2. Samples collected at YNP were more acidic than those collected at SNP. The difference in pH between the two regions appears to be due to relatively small differences in inputs of NO3, SO42−, and NH4+. In the absence of inputs of NH3, cloudwater pH values in the Sierra may fall below 3.Over 250 h of cloud interception were observed during a 12 month period at a cloud monitoring site at 1856 m elevaton in SNP. Estimates of cloudwater deposition of NO3, SO42−, and NH4+ indicate that cloud interception contributes significantly to regional acid deposition for closed forest canopies. Cloud interception may be the dominant deposition mechanism for isolated conifers and ridgetop canopies, where wind speeds are higher and cloudy air parcels can impact directly on foliar surfaces.  相似文献   

3.
Chemical composition of precipitation in Albany, NY from July 1986 to December 1988 has been studied. Mean volume-weighted concentrations (μeqℓ−1) were: acidity, 104.0; alkalinity, −63.7; SO42−, 52.8; NO3, 29.8; Cl, 5.6; F, 0.50; NH4+, 19.3; Ca2+, 6.5; Mg2+, 2.8; Na+, 3.5; and K+, 1.4. Mean pH was 4.2 . Seasonal patterns were pronounced for most species. Concentrations of H+, SO42−, NO3, NH4+ and Ca2+ peaked in the summer and spring. Deposition was related to rainfall amount by a power law relationship in which the exponent of the equation was ∮.6. Wet SO42− deposition was 2.35 keq ha−1 over a 30-month period. The SO42− and NO3 deposition rates observed at Albany indicate that transport from midwestern sources have a major influence at this site. On the average, free H+ ion concentrations determined from pH measurements accounted for 51% of the measured total acidity. There were unknown species, most likely organic acids, that could contribute to the acidity. Correlation and regression analyses indicated that major anions, SO42− and NO3, were closely associated with H+ and NH4+ ions. Factor analysis revealed four common factors which are related to fossil-fuel combustion, sea spray, cement factory and biomass burning.  相似文献   

4.
The precipitation chemistry of Greater Manchester, a Metropolitan County in the northwest of England, has been examined for small scale spatial variability using a network of 18 bulk precipitation collectors. Significant spatial variability was found for concentrations of non-marine SO42−, NO3, NH4+, Ca2+ and H+ ions. The statistical associations between the data were investigated using correlation, partial correlation and principal components analyses. It was found that zero-order correlation coefficients were inadequate for the interpretation of the data and that the computation of first, and higher order partial correlation coefficients was necessary in order to explain the interrelationships between the data and their spatial variability. The statistical associations between the data suggest relationships between Ca2+ and non-marine SO42−, and NO3+ in precipitation which are discussed in terms of their possible precursor species. Potential source effects were examined in conjunction with atmospheric removal processes. The dry deposition of SO4 particles, rather than the dry deposition of SO2, may explain the spatial variability of non-marine SO42−. The erosion of CaSO4 formed from the reaction of SO2 with CaCO3 on urban surfaces with subsequent resuspension is thought to be the basis of the relationship between Ca2+ and non-marine SO42− concentrations in precipitation. The wet and dry deposition of CaCO3 particles from local sources may be partially responsible for the spatial variability of H+, and dry deposition and scavenging of NH3, in conjunction with the predominant wind direction may explain the spatial variability of NO3 and NH4+ ions. Ammonia is thought to originate from sources both outside the study area and within it.  相似文献   

5.
Scavenging of sulfates and nitrates—two most common ions leading the cloudwater acidity—was investigated during field studies atop a site in Mt. Mitchell (35°44′05″N, 82°17′15″W) State Park where the highest peak (2038 m MSL) of the eastern U.S. is located. Experiments were conducted during the growing seasons (15 May–30 September) of 1986 and 1987 using an instrumented meteorological tower (16.5 m tall) and a passive cloudwater collector. A cloud episode that occurred on 12 October 1987, was also comprehensively investigated. Clouds were frequently observed in which the Fraser fir and red spruce stands stayed immersed 28% and 41% of the time during the 1986 and 1987 seasons, respectively. Rate of cloudwater deposition on the forest canopy was determined using an inferential cloud deposition model. It was found by analysing nine short duration (lasting 8 h or less) and 16 long duration cloud events that the ionic concentration (SO42− and NO3) is inversely proportional to the rate (Ic) of cloudwater deposition (in mm h−1) and can be expressed by the following relationship: [SO42−] = aIcb or [NO3] = aIcb. Theoretical arguments leading to these relationships are presented. The b values for predicting NO32− concentration are found in the range of 0.14–1.24 (mean = 0.48) for short duration and 0.062–0.63 (mean = 0.27) for long duration cloud events, respectively. The corresponding b values for predicting NO3 concentrations are 0.19–1.16 (mean = 0.49) and 0.072–0.59 (mean = 0.27), respectively. When the b parameter was between 0.2 and 0.6, the correlation coefficients between measured and predicted ionic concentrations were found to exceed 0.7. The parameter a is shown to represent the maximum ionic flux for a given cloud event. The ratio of the a parameter for SO42− to NO3 varied between 1.75 and 6.95, indicating that the SO42− contributes to the total ionic concentration substantially more than the NO3 leading to the conclusion that the cloudwater acidity is primarily due to the presence of sulfuric acid which has been demonstrated to cause foliar injury and growth retardation in red spruce trees. The above parameterization is similar to the one that is frequently used to relate ionic concentration in precipitation to the rainfall rate. In order to understand physico-chemical processes leading to the proposed parameterization schemes, meteorological and chemical variables are comprehensively analysed for one short duration and two long duration cloud events. The concentrations of principal ions (SO42−, NO3, H+ and NH4+) during the short duration cloud events were found to be much higher than those during the long duration ones, especially at colder temperatures. Such short cloud events have a potential of causing foliar narcosis in red spruce stands because of unusually acidic cloudwater to which these stands stay exposed intermittently during each growing season.  相似文献   

6.
Estimates of external and internal sources of ions in net througfall deposition were derived for a deciduous and coniferous canopy by use of multiple regression. The external source component appears to be dominated by dry deposition of Ca2+, SO2 and NO3 during dormant and growing seasons for the two canopy types. Increases in the leaching rates of K+ and Mg2+ during the growing season reflect the presence of leaves in the deciduous canopy and increased physiological activity in both canopies. Internal leaching rates for SO42− doubled during the growing season presumably caused by increased physiological activity and uptake of SO2 through stomates. Net deposition of SO42− in throughfall during the growing season appears highly dependent on stomatal uptake of SO2. Estimates of SO2 deposition velocities were 0.06 cm s−1 and 0.13 cm s−1 for the deciduous and coniferous canopies, respectively, during the dormant seasons, and 0.30 cm s−1 and 0.43 cm s−1 for the deciduous and coniferous canopies, respectively, during the growing season. For the ions of major interest with respect to ecosystem effects, namely H+, NO3 and SO42−, precipitation inputs generally outweighed estimates of dry deposition input. However, net throughfall deposition of NO3 and SO42− accounted for 20–47 and 34–50 per cent, respectively, of total deposition of those ions. Error estimates of ion sources were at least 50–100 per cent and the method is subject to several assumptions and limitations.  相似文献   

7.
Wet deposition measurements of H+, SO42− and NO3 from 29 monitoring sites located in (16) and around (13) Pennsylvania, U.S., were analyzed to quantify errors associated with extrapolating point estimates of deposition using five surface-fitting algorithms. The influence of site density on estimation errors associated with each surfacing algorithm was also investigated. The five surfacing differed little in their abilities to predict the concentration or deposition of individual ions found in precipitation in Pennsylvania. However, the size of estimation errors for all parameters, even those based on the densest network, were quite high relative to the variation observed among monitoring sites in Pennsylvania. All monitoring site observations were within 22.8, 17.6 and 23.1 per cent of the median concentration and 33.9, 35.3 and 36.7 per cent of the median deposition for H+, NO3 and SO42−, respectively. Maximum per cent errors indicate that estimation errors may severely obscure actual surface features in at least some portions of the estimated concentration and deposition grids in Pennsylvania. Deposition and concentration estimates based on higher density networks were generally more accurate; however, the improvements afforded by the additional sites were quite modest. Based on the magnitude of estimation errors, kriging produced the most accurate estimates, although no single algorithm consistently yielded the most accurate estimates for all parameters.  相似文献   

8.
Wet precipitation-only samplers were used to collect wet deposition at two sites in the Athens basin, Greece for the period March 1986–February 1987.Concentrations of major cations (H+, NH+4, Na+, K+, Ca2+ and Mg2+) and major anions (Cl, NO3 and SO2−4) were determined for the first time in rainwater samples in Greece. Bicarbonate concentrations were calculated. The relative importance of natural and anthropogenic sources were estimated by a chemical balance. The majority of rain collected has a neutral or alkaline character. Acidity was due to the presence of H2SO4 and HNO3. The statistical analysis of the correlation between the concentration of chemical species confirm the influence of natural and anthropogenic sources. In all samples, SO2−4 concentrations exceed NO3 concentrations despite the dominance of low S oil burning in the region. The wet flux of S was calculatd to be 0.34 gm−2a−1.  相似文献   

9.
Atmospheric dry deposition to branches of Pinus contorta and P. albicaulis was measured during summer 1987 in a sub-alpine zone at Eastern Brook Lake Watershed (EBLW), eastern Sierra Nevada, California. Results are presented as deposition fluxes of NO3, SO42−, PO43−, Cl, F, NH4+, Ca2+, Mg2+, Na+, K+, Zn2+, Fe3+, Mn2+, Pb2+ and H+, and compared with other locations in California and elsewhere. Deposition fluxes of anions and cations to the pine branches were low, several times lower than the values determined near the Emerald Lake Watershed (ELW), another sub-alpine location in the western Sierra Nevada. The sums of deposition fluxes of the measured cations and anions to pine surfaces were similar, in contrast to the ELW location where the sums of cation fluxes were much higher than the sums of anion fluxes. A strong positive correlation between depositions of NO3 and NH4+, as well as SO42− and Ca2+, suggested that large portions of these ions might have originated from particulate NH4NO3 and CaSO4 deposited on pine surfaces. An estimated total N dry deposition (surface deposition of NO3 and NH4+ and internal uptake of NO2 and HNO3) to the forested area of the EBLW was 29.54 eq ha−1 yr (about 414 g H ha−1 yr−1).  相似文献   

10.
Precipitation chemistry data collected between 1980 and 1987 for 11 NADP/NTN sites in Texas have been analyzed using factor analysis and a trend analysis of monthly averages. Factor analysis identified four major factors which differed significantly from site to site: (1) a Gulf factor of Na+, Cl-, and Mg2+; (a) a soil factor of Ca2+, K+, Na+, and Mg2+; (3) an acid factor of H+, NO3, and SO44−; and (4) an aged aerosol factor of NO3, SO42−, and NH4+. At Longview, the acid and Gulf factors accounted for 18 and 46%, respectively, of the variation of the data. A trend analysis was performed on the logarithm of the monthly averages at the Longview and Victoria sites, the two sites with the largest and most complete data. Results suggest that hydrogen ions have been increasing at both sites, while calcium ions have been decreasing.  相似文献   

11.
Daily measurements the atmospheric cocnentrations of HNO3, NO3-, NO2, SO2, SO42−, NH4+, and several trace metals were made at the University of Michigan Biological Station over a 124-day period during the 1984–1985 winter. The composition of the daily precipitation was also determined. The relative contributions of scavenged NO3 and HNO3 to the precipitation was estimated by assuming that the NO3 scavenging ratio was the same as that of trace metals with a similar particle size. Similarly, the SO42− and SO2 contributions were based on the scavenging ratios of NH4+ and trace metals. On this basis, it was determined that the event median NO3 and HNO3 scavenging ratios were 500 and 3500, respectively. HNO3 scavenging accounted for 83% of the total scavenged NO3. Scavenging of SO42− accounted for all the snow SO42− in 67% of the events. In the remaining events, some SO2 was scavenged, with a median scavenging ratio of 219. Overall, 67% of the snowfall acidity appeared to be due to HNO3 scavenging. Backward air-mass trajectories that were calculated for each event were used to determine the general source regions of the acidic species. Snow associated with air masses from the south and west accounted for 81 and 75% of the deposited NO3 and SO42−, respectively.  相似文献   

12.
Simultaneous aerosol and snow sampling was performed during a field campaign at the Alpine site Weissfluhjoch Davos, Switzerland (2540 m a.s.1.) from 1 January through 30 March 1988. In addition, a snow pit was sampled on 30 March 1988. Very good agreement between the new snow and pit snow samples was found for the measured major ions as well as for the stable isotopes δ18O and δD. Thus, snow pit samples obtained at this site during the winter months yield representative deposition patterns with a conserved stratigraphy. Generally, concentrations in snow were very low, with 3.5, 8.5, 5.2 and 2.4 μeq ℓ−1 for Cl, NO3, SO42−, respectively. The 36Cl and 10Be concentrations as well as the 10Be/36Cl ratios were comparable to the ones measured at Arctic sites. With the exception of NO3, no linear relation was obtained between atmospheric and snow concentrations, showing that the concept of scavenging ratios must be used with caution when looking at single snowfall events. The following precipitation-weighted mean scavenging ratios were found: 300 for NH4+, 350 for SO42−, 940 for total NO3(NO3+HNO3), 175 for 210Pb, and 750 for 10Be.  相似文献   

13.
A time series of wet deposition in Arnhem, the Netherlands, was analysed for the period 1984–1991. Precipitation was collected with four samplers on a daily basis. A comparative study by the Dutch National Precipitation Network showed significant biases for the observations of the National Network station due to longer exposure to dry deposition. Simultaneous operation of wet-only and bulk collectors demonstrated a concentration bias of about 10% for daily bulk sampling.Using a cluster analysis of backward trajectories, clear distinctions could be made between precipitation from continental and maritime origin. Event-to-event variations in deposition seemed to be determined largely by meteorological influences. As major anthropogenic source regions, the U.K., France, Belgium and the Netherlands itself were identified. The contribution of Dutch sources to wet acid deposition in Arnhem was estimated at 30–40%.Trends and seasonal variations were analysed with an advanced time-series model based on Kalman filtering. Similar seasonal variations were found for SO42− and NH4+. Also, seasonal variations in the concentrations of H+ and NO3 corresponded. Significant long-term changes in deposition and concentration were found for SO42− (about −3% yr−1) and H+ (about −9% yr−1) only. The analysed trends were decreasing, but decreases were larger in the years 1984–1986 than in the following years. The relative decrease in the wet deposition of SO42− was substantially smaller than decrease in dry-deposited SO2 and SO42−.  相似文献   

14.
Atmospheric dry deposition of ions to branches of native Pinus contorta and Pinus monticola (natural surfaces), and nylon filters and Whatman paper filters (surrogate surfaces) were measured in the summer of 1987 in the vicinity of Emerald Lake Watershed (ELW) of the Sequoia National Park located on the western slope of the Sierra Nevada in California. Deposition fluxes of airborne NO3, NH+4 and SO2−4 to native pines at the ELW were much higher than in the eastern Sierra Nevada, but several times lower than deposition fluxes to natural and surrogate surfaces at the highly polluted site in the San Gabriel Mountains of southern California. Deposition fluxes of NO3 and NH4+ to the natural and surrogate surfaces at the ELW were much higher than deposition of SO42−, providing the importance of N compounds in atmospheric dry deposition in this part of the western U.S. A deficit of inorganic anions in materials deposited to various surfaces indicated a possibility of substantial participation of organic acids in atmospheric dry deposition processes. Nylon and paper filters proved to be poor surrogate surfaces for the estimation of ionic dry deposition to conifer branches.  相似文献   

15.
The wet, dry and cloud water deposition of acidic substances on the forest canopy are considered as major mechanisms for pollutant induced forest decline at high elevations. Direct cloud capture plays a predominant role of intercepting acidic substances in above cloud-base forests. We conducted a field study at Mt. Mitchell, North Carolina (35°44′05″N, 82°17′15″W; 2038 m MSL)—the highest peak in the eastern U.S.—during May–September 1986 and 1987 in order to analyze the chemistry of clouds in which the red spruce and Fraser fir stands stay immersed. It was found that Mt. Mitchell was exposed to cloud episodes 71% of summer days, the cloud immersion time being 28% for 1986 (a record drought summer in southeastern U.S.) and 41% for 1987. Sulfate, NO3, NH4+ and H+ ions were found to be the major constituents of the cloud water, which was collected atop a 16.5 m tall meteorological tower situated among 6–7 m tall Fraser fir trees. The initiation of precipitation in clouds invariably diluted the cloud water acidity. The cloud water pH during short episodes (8 h duration or less), which resulted from the orographic lifting mechanisms, was substantially lower than that during long episodes, which were associated with meso-scale and synoptic-scale disturbances. Sulfate accounted for 65% acidity in cloud water, on the average, and contributed 2–3 times more than the NO3. Inferential micrometeorological models were used to determine deposition of SO42− and NO3 on the forest canopy and the hydrological input due to direct cloud capture mechanism. The cloud water deposition ranged between 32 and 55 cm a−1 in contrast to the bulk precipitation which was about 130 cm a−1 as measured by an on-site NADP (National Atmospheric Deposition Program) collector. For S compounds, wet, dry and cloud water deposition accounted for 19%, 11% and 70%, respectively for 1986, and 16%, 8% and 76%, respectively for 1987. For N compounds, dry deposition contributed 35% and 23% for 1986 and 1987, respectively, whereas, cloud water deposition contributed 50% and 65% for 1986 and 1987, respectively. Our estimates are compared with the reported literature values for the other sites.  相似文献   

16.
Wet precipitation was collected in Thessaloniki, Greece, during the period March 1989–December 1990 by using an automatic wet-only precipitation sampler.Rainwater samples were analysed for major cations (H+, NH4+, Na+, K+, Ca2+, Mg2+) and anions (Cl, NO3, SO42−), in addition to acidity and conductivity measurements. The majority of rain had a neutral or alkaline character as a result of neutralization, primarily caused by calcareous soil dust and secondarily by atmospheric ammonia. In all rain, SO42− concentration exceeded NO3 concentration. The contribution of maritime sources to the total SO42− concentration was very low (<2%).The chemical composition of precipitation was analysed in conjunction with meteorological variables (season of the year, precipitation type, airflow patterns) to evaluate temporal variations and chemical source influence. Rain caused by weak, localized flows showed the highest acidity and the minimum influence of neutralization processes.  相似文献   

17.
Measurements of inorganic aerosol and gas phase species are presented for three sites in central California during a 4 day period in April 1988. The measurement sites were located along an east-west transect at Visalia, Ash Mountain, and Lower Kaweah, with elevations of 90, 550 and 1900 m, respectively. Aerosol compositions were nearly neutral at all locations, however large concentrations of NH3 at Visalia contributed significant excess alkalinity to the air mass sampled there. Concentrations of all major species were observed to decrease with elevation during most of the sampling periods. Concentrations at the upper two sites exhibited diurnal fluctuations, with peaks in the late afternoon, consistent with the transport of pollutants from San Joaquin Valley sources by daytime upslope winds. Concentrations of most of these species reached a maximum at the elevated sites on 28 April, as a weak cold front approached, reducing the atmospheric stability over the valley floor. Concentrations at Visalia on this day were somewhat lower than those observed earlier in the week.Clouds intercepting the mountain slopes on 28 April were sampled at two locations. The coudwater pH at both sites was observed to fall throughout the event, dropping as low as 4.34. Precursor concentrations of aerosol NO3, SO42- and NH4+, and gas phase HNO3 and NH3, were sufficient to account for the observed cloudwater loadings of NO3, SO42- and NH4+. In-cloud measurements made near the cloud base indicated a considerable S(IV) oxidation potential in the form of H2O2, but only low S(IV) concentrations. Cloudwater concentrations of formic acid were approximately three times acetic acid concentrations. Carbonyl concentrations were dominated by formaldehyde and glyoxal.  相似文献   

18.
Rainwater samples in S. Paulo city were collected on an event basis from October 1983 to October 1985 covering two dry and two rainy periods. Bulk samples only were obtained. At the same site and period, fine, coarse and inhalable particles were also collected. Na+, Ca2+, K+, Mg2+, NO3, SO42− and NH4+ contents were determined in rainwater samples, while Na, Ca, K, Cl and S concentrations were measured in aerosol samples. Rainwater is slightly acid (mean pH = 5.0), and contains high concentrations of Ca2+, NO3, SO42− and NH4+. Dry and wet fluxes and washout ratios were determined for some elements. Results obtained suggest that the atmospheric composition in this city is strongly influenced by anthropogenic sources.  相似文献   

19.
A controlled field study was conducted at Research Triangle Park, NC, to determine how shape, size and orientation of galvanized steel structures affect (1) dry deposition of SOx and NOx compounds and (2) dissolution of Zn corrosion products resulting from such deposition. Thirteen structures of various shapes, sizes and orientations were exposed to dry deposition only for 100 weeks, during which they were rinsed with deionized water every 2 weeks and the rinses were analysed for Zn, Ca, and their ionic contents. The rinse data are consistent with size, orientation and exposure history affecting dry deposition of SO2−4 precursors such as SO2. Dry deposition of precursors of surface NO3, including HNO3, is affected by structure size. A model regression equation is presented that shows that Zn dissolution can be explained in terms of the SO−24 and NO3 rinse concentrations. The experimental results suggest that there is likely to be some error associated with extrapolating galvanized steel test panel results to actual structures.  相似文献   

20.
Measurements of wet deposited NH4+, SO42−, NO3 and Cl, as well as airborne concentrations of these species and gaseous HNO3, HCl and NH3, have been made at a site in eastern England. Scavenging ratios based solely upon aerosol-associated species and upon aerosol plus gaseous airborne species are presented and compared with literature values. It appears that HCl and HNO3 have only a rather minor influence upon wet deposition at our site. Gaseous NH3 influences ground-level air chemistry appreciably, but scavenging ratios for NH4+ are low, even when based upon aerosol NH4+ concentrations alone, presumably due to altitudinal gradients in this species. The problems inherent in interpretation of scavenging ratios are discussed. Deposition of nitrogen in various chemical forms is estimated from rainwater and air composition. If a transport-limited deposition velocity is assumed for ammonia gas, dry deposition of this species accounts for around 40% of total nitrogen deposition to the ground.  相似文献   

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