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1.
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   

2.
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   

3.
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   

4.
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   

5.
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   

6.
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   

7.
Fog, aerosol, and gas samples were collected during the winter of 1986 at Riverside, California. The dominant components of the aerosol were NH4+, NO3, and SO42−. Gaseous NH3 was frequently present at levels equal to or exceeding the aerosol NH4+. Maximum level were 3800, 3100, 690 and 4540 neq m−3 for NH4+, NO32− and NH3(g), respectively. The fogwater collected at Riverside had very high concentrations, particularly of the major aerosol components. Maximum concentrations were 26,000 29,000 and 6200 μM for NH4+, NO3 and SO42−, respectively. pH values in fogwater ranged from 2.3 to 5.7. Formate and acetate concentrations as high as 1500 and 580 μM, respectively, were measured. The maximum CH2O concentration was 380 μM. Glyoxal and methylglyoxal were found in all the samples; their maximum concentrations were 280 and 120 μM, respectively. Comparison of fogwater and aerosol concentrations indicates that scavenging of precursor aerosol by fog droplets under the conditions at Riverside is less than 100% efficient.The chemistry at Riverside is controlled by the balance between HNO3 production from NOx emitted throughout the Los Angeles basin and NH3 emitted from dairy cattle feedlots just west of Riverside. The balance is controlled by local mixing. Acid fogs result at Riverside when drainage flows from the surrounding mountains isolate the site from the NH3 source. Continued formation of HNO3(g) in this air mass eventually depletes the residual NH3(g). A simple box model that includes deposition, fog scavenging, and dilution is used to assess the effect of curtailing the dairy cattle feedlot operations. The calculations suggest that the resulting reduction of NH3 levels would decrease the total NO3 in the atmosphere, but nearly all remaining NO3 would exist as HNO3. Fogwater in the basin would be uniformly acidic.  相似文献   

8.
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   

9.
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   

10.
The use of filter packs and a cascade impactor during a series of research cruises in the southern area of the North Sea has yielded detailed spatial distribution patterns of aerosol concentrations, Cl, NO3, SO42−1 and NH4+ and gaseous concentrations, HCl, HNO3 and NH3. The overall distribution of the atmospheric concentrations closely parallels published modelled results for metallic species. The chemical transformations of these aerosols and gases are investigated together with their interactions with the seasalt aerosol. Aerosol chloride loss is greatest in the more polluted areas, whilst concentrations products of NH3 with HNO3 and HCl appear insufficient to sustain the existence of NH4NO3 and NH4Cl. Nitrate is associated predominantly with larger particles and appears to be present substantially as a surface coating on marine aerosol. The total dry deposition input for nitrogen species is calculated for the southern sector with extrapolation to the whole of the North Sea, using particle size weighted deposition velocities of 0.63 and 0.21 cm s−1 for NO3−1 and NH4+, respectively, and literature-derived values for the gaseous constituents. Finally the use of air-mass back trajectories illustrates the role of source regions in influencing the chemical composition of the North Sea atmosphere.  相似文献   

11.
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   

12.
Rainwater and atmospheric bulk deposition samples were collected at a station on the rooftop of the Research Institute of King Fahd University of Petroleum and Minerals in Dhahran. Continuous sampling was carried out manually throughout the rainy season between December 1987 and February 1988, and for one rainfall event in March 1987. A total number of 13 samples were collected and investigated for pH and dissolved ionic composition using inductivity coupled plasma emission spectrometry (ICP) and ion chromatography (IC). The range and volume-weighted average pH were 5.1–7.2 and 5.48, respectively. Significant negative linear correlations were observed between the precipitation pH and rain depth, and between pH and the summation of dissolved {(Ca2+ + Mg2+)−(SO42− + NO3 + NO2)} (in μeqℓ−1). The ionic summation also correlated negatively with rain depth. The ionic abundance in rainwater (in μeqℓ−1) expressed in concentration order showed the general trend SO42− > HCO3−1 = Cl = NO3 > NO2 for anions and Ca2+ > Na+ > Mg2+ > NH4+ > K+ > H+ > Sr2+ for cations. Good mass balance between cations and anions was observed. Total NO3 contribute equally to precipitation acidity as SO42− and Ca2+ plus Mg2+ in alkaline suspended particulates from natural sources are the major ions which buffer the acidity of precipitation. The NH4+ ion which is also present plays an insignificant role in the acid/base equilibrium of rainwater.  相似文献   

13.
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   

14.
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   

15.
Emission densities of air pollutants are higher in Europe than in the U.S. as a whole, suggesting similar differences in atmospheric deposition. We determined air concentrations and deposition during the warm season at conifer forests in Tennessee and northern Germany. Our results confirmed major differences in both chemistry and fluxes. Atmospheric and precipitation concentrations of all ions except H+ were higher at the German site, most significantly for the nitrogen species. The much higher levels of NH4+ at this site reflect higher emissions of NH3, which was the species largely responsible for the lower levels of H+. Total airborne nitrate was dominated by HNO3 in Tennessee. In Germany we found comparable amounts of HNO3 and aerosol NO3, the concentration of which varied seasonally, apparently in response to agricultural emissions of NH3 that reacted to form NH4NO3. Total deposition of all major ions was much higher at the German site, particularly for the nitrogen species, which exhibited a marked edge effect in throughfall. Dry deposition was determined from air concentrations by using a canopy resistance model and from a statistical model of throughfall fluxes, each of which yielded comparable fluxes for several ions. Dry deposition contributed 10–70% of the ion input and was most important at the German site. Both forest canopies absorbed 40–50% of total deposited nitrogen, primarily from dry deposition.  相似文献   

16.
The changes in the pH and the contents of NH4+, NO3 and 10 other components including trace elements were studied in precipitation samples for a period of up to 300 days. The concentration of free H+ ions is affected after deposition by several processes, the most important being bioconsumption of NH4+ leading to an increase in the H+ ion level depending on the length of the sampling interval, the time of year and the way of storing the samples prior to their analysis. It is proposed that, for the purpose of comparing the acidities of precipitation waters and their effects on acidification of the environment, the corrected H+ ion concentration (Hc+) be calculated from the pH value and the concentrations of NH4+ and NO3 (Hc+ = H++NH4+−NO3). The Hc+ value depends little on the bioconsumption of NH4+ and NO3 after deposition and thus is not very sensitive to the way of storing the samples, the sampling interval and the time elapsed between deposition and the sample analysis. Dissolution of Fe, Al, Si and some trace elements from the particles scavenged during precipitation was slow in the studied samples; it is advantageous to digest the sample in a microwave oven prior to determination of these elements.  相似文献   

17.
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   

18.
An iterative least-squares method with a receptor model was applied to the analytical data of the precipitation samples collected at 23 points in the suburban area of Tokyo, and the number and composition of the source materials were determined. Thirty-nine monthly bulk precipitation samples were collected in the spring and summer of 1987 from the hilly and mountainous area of Tokyo and analyzed for Na+, K+, NH4+, Mg2+, Ca2+, F, Cl, Br, NO3 and SO42− by atomic absorption spectrometry and ion chromatography. The pH of the samples was also measured. A multivariate ion balance approach (Tsurumi, 1982, Anal. Chim. Acta138, 177–182) showed that the solutes in the precipitation were derived from just three major sources; sea salt, acid substance (a mixture of 53% HNO3, 39% H2SO4 and 8% HCl in equivalent) and CaSO4. The contributions of each source to the precipitation were calculated for every sampling site. Variations of the contributions with the distance from the coast were also discussed.  相似文献   

19.
This paper addresses two hypothesis that try to explain the difference observed between the estimated NH3 emission levels in The Netherlands and those indicated by atmospheric measurements, the so called ‘ammonia gap’: the role of SO2 emissions regulating ambient NH3 concentrations through co-deposition, and long-term NH3 emissions after slurry injection. It was found that throughfall measurements of NH4+ could not be used as indicator for changes in NH3 emissions. The throughfall deposition of NH4+ is in close equilibrium to SO42− and NO3 and is thus regulated by the equilibrium of ambient NH3 and NH4+ in wet deposition and canopy water layers. When SO2 emissions decrease, the amount of available SO42− decreases, which imposes a limit on the deposition of (NH4)2SO4. Long-term emissions of NH3 after application of manure were monitored using a new technique, which continuously measures the concentration of NH3 in a cross-section of the emission plume downwind of the source. The emissions could be registered for 3 weeks after application of manure. The results indicate that the long-term emissions only contribute 1–2% to the total emission level. Both the effect of SO2 on the NH3 deposition levels and the long-term emission fluxes are not enough to explain the observed ammonia gap. It seems that several counteracting effects, some of them emerging from the new emission reduction regulations, contribute to the ammonia gap. An integrated approach to abate ammonia emissions is, therefore, needed. The implementation and regulation of production ceilings for reactive nitrogen might be a good option.  相似文献   

20.
As part of the second Arctic Gas and Aerosol Sampling Program (AGASP-II), Arctic aerosol samples were collected by the NOAA WP-3D aircraft in spring 1986. The samples were analyzed in bulk and individual-particle form, using ion chromatography (IC) and electron microscopy (EM), respectively. Information on the chemical composition of the aerosol as determined by various techniques is presented, as well as morphology, concentration, and size distribution data obtained from individual particle analyses. For most flights, a stratospheric sample and a haze profile samople were collected. Haze samples exhibited greater particle concentrations than stratospheric samples, the highest concentrations in haze reaching ∼103 cm−3 (non-volatile particles > 0.05 μm diam). Sulfur was consistently observed to be a major element in both large and small particles in haze samples. Crustal elements such as Si, Al, K, Ca and Fe were often present in significant concentrations together with S. Particles that did not emit X-rays, possibly organic or sooty C, were observed in significant concentrations in both tropospheric and stratospheric samples. Chemical spot tests confirmed that SO42− was the major S-containing species and that NO3 was not nearly as prevalent as SO42− in the Arctic aerosol particles. The mass concentrations of major anions (Cl, SO42− and NO3) and cations (Na+, K+, NH4+, Ca2+ and Mg2+) in the bulk aerosols were determined using IC. The ratios between ion concentrations, e.g. Ca2+/Na+, SO42−/Na+ and Cl/Na+, may serve as indicators of aerosol origins and mixing status of various air masses. Aerosols collected on six flights demonstrated variability of particle characteristics in relation to sources and transport of Arctic haze.  相似文献   

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