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1.
A study of sulfate aerosol acidity in Metropolitan Toronto was conducted during the summer of 1986. Fine-fraction aerosol (<2.5-μm) were collected using Teflon membrane filters and analyzed for major ionic species (H+, NH+4, NO3, SO2−4). Samples were collected for 6 weeks at three study sites: one in the Center City and the others 13 km (WNW) and 20 km (NE) away. There were very strong correlations among the three sites with respect to measured aerosol species (r2 > 0.9 for 24-h data). However, spatial variations in the magnitude of aerosol acidity were observed during sulfate episodes. For example, the peak concentrations for all sites occurred on 25–26 July 1986. While the 24-h data for sulfate were quite uniform at the three sites (34, 34 and 35 μg m−3), H+ concentrations were 9.4, 8.3 and 6.0 μg m−3 (as H2SO4) for the NE, WNW and Center City sites, respectively. For most of the summertime episodes, the downtown area also had lower aerosol acidity compared to the two sites in suburban areas.  相似文献   

2.
Air sample filters from a Local Authority archive have been analyzed for sulphate using XRF. This has allowed an assessment to be made of the spatial distribution of 24-h sulphate concentrations in the city of Norwich in eastern England, over a 9-month period. The overall mean sulphate concentration was 10.4 μg m−3, with a range of overall mean values between the sites of 7.7–12.2 μg m−3. This spatial variability within the city is similar to the spatial variability between cities found in another previous study. The mean SO2−4/SO2 and smoke/SO2−4 ratios at the different sites are similar, but there are distinct variations in the overall mean ratios over the measurement period. There appear to be relationships between the SO2−4/SO2 ratio and temperature and humidity. The ratios are also related to wind direction, with some evidence that a proportion of the SO2−4 in the urban atmosphere of Norwich originates via long-distance transport from the east.  相似文献   

3.
Measurements of the dry deposition of pollen were made during the months of May and June 1987 in northern Wisconsin, using a smooth surrogate surface. Samples were taken on a raft located on Little Rock Lake and at a nearby field monitoring station. Rain samples were also collected at the field station. The wet SO42− flux was 102.7 mg m−2, compared with a dry SO42− flux of 118 mg m−2 at the field monitoring site and 45 mg m−2 at the lake site.The SO42− content of pollen ranged from 0.2 to 0.8% of the weight of the pollen, and NO3 concentrations were an order of magnitude lower. Between 9 and 22% of the pollen weight was available as total organic carbon (TOC) upon addition to water.The addition of pollen to distilled water produced an acid reaction, due to organic acids and not inorganic acidity.  相似文献   

4.
The concentration (μgC m−3) of aerosol organic carbon as determined by collection with quartz fiber filters was found to exhibit a significant decrease with increasing filter face velocity. A similar face velocity dependence was found for organic carbon on back-up quartz fiber filters behind either quartz fiber front filters (QQ combination) or Teflon membrane front filters (TQ combination). Additionally, the concentration of organic carbon on the back-up filter in the TQ combination was always greater than on the back-up filter in the QQ combination. The most likely explanation for these observations is the adsorption or organic vapors onto the filter medium itself. The amount of organic carbon adsorbed onto the quartz fiber front filter can be approximated by measuring the amount of organic carbon on a quartz fiber back-up filter behind a Teflon front filter with both filter combinations sampling at the same face velocity. Making the correction in such a manner removes most of the face velocity dependence inthe resultant concentrations. For 24 h sampling in Portland, Oregon, at a face velocity of 40 cm s−1, the correction exceeded 50% for uncorrected organic carbon concentrations of 2 μgC m−3 but decreased to 15% at 16 μgC m−3.  相似文献   

5.
Monthly mean chemical composition of aerosol with diameter less than 8 μm was identified in Sapporo in 1982. The mass of aerosol was made up of nine components: elemental C, organics, SO42−, NO3, NH4+, Cl, Na+, soil particles and water. The concentrations of carbonaceous particles (elemental C and organics) was relatively high (12.7–16.0μ m−3) in autumn and winter (October–February) due to emission from domestic heating and comprised 36–41% of total aerosol mass. Higher concentration of soil particles was observed in spring (March–May) (9.7–13.1 μg m−3) and comprised 22–29% of total aerosol mass due to suspension by strong wind. On the other hand, the concentration of excess SO42− (non-sea salt SO42−), which ranged from 2.6–5.2 μg m−3, did not change remarkably with season, and the fraction of excess sulfate increased to 21% in summer (July–August) probably due to photochemical transformation from SO2. Nitrate concentration was far less than that of SO42− throughout the year in Sapporo.  相似文献   

6.
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   

7.
A 2-week intensive ambient aerosol study was conducted in December 1988 in Wuhan (Hubei Province), a city of nearly 2 million located on the Yangtze River in central China (P.R.C.). This is an industrial region where soft coal burning is widespread, and emission controls for vehicles and industrial facilities are minimal. The sampling site was located in one of the civic centers where residential and commercial density is highest. An Andersen dichotomous sampler was operated with Teflon membrane filters to collect fine (dp < 2.5 μmad) and coarse (2.5 ⩽ dp < 10 μmad) particles for total mass and element determinations. An annular denuder system (ADS) was used to collect fine fraction aerosols for analyses of ionic species including strong acidity (H+).The study was conducted between 18 and 30 December, which was rainless, consistently cool (3–10°C) and overcast, but without fog or acute stagnation. Fine particulate mass (PM, as μ m−3) averaged 139 (range 54–207); coarse PM averaged 86 (range 29–179). Trace element concentrations were also high. Crustal elements (Si, Al, Ca and Fe) were found primarily in the coarse fraction, while elements associated with combustion (S, K, Cl, Zn and Se) were enriched in the fine fraction. The concentrations of arsenic and selenium were evidence of a large source of coal burning, while vanadium levels (associated with fuel oil use) were not especially enriched.Despite the seemingly high PM loadings, ionic concentrations were not especially high. The average composition of soluble fine aerosol species (in neq m−3) were SO42−: 520 (range 180–980), NO3: 225 (range 50–470), Cl: 215 (range 20–640), and NH4+: 760 (range 280–1660). A deficit in accountable FP components (total mass compared to the total of ionic plus element masses) as well as the black appearance of collected materials indicate an abundance of carbonaceous aerosol, as high as 100 μ m−3. (total mass compared to the total of ionic plus element masses) as well as the black appearance of collected materials indicate an abundance of carbonaceous aerosol, as high as 100 μ m−3Aerosol acidity was negligible during most monitoring periods, H+: 14 (range 0–50 neq m−3, equivalent to 0–2.5 μm m−3 as H2SO4). Sulfur dioxide, measured by the West-Gaeke method for part of the study, concentrations were low. Although not directly measured, the aerosol measurments suggested that gaseous HCl (from refuse incineration) and NH3 (animal wastes) concentrations might have been high. Higher aerosol acidity might be expected if HCl sources were more prominent and not neutralized by local ammonia or other base components.  相似文献   

8.
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   

9.
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   

10.
Atmospheric deposition of SO2, and fine particles of Pb and Cd are calculated over a one-year period in a 66 km2 airshed with a segment-puff model. Emission variations, hourly mixing heights and meteorological values are considered to compute monthly averages of concentrations and deposition. Dry deposition is calculated by means of deposition velocities which are season- and land use-dependent. Wet deposition is determined using a washout coefficient. To assess the simulation performance, calculated SO2 results from the combination between the deposition velocity, the windspeed and direction and the location and type of sources. As annual averages, results for dry plus wet deposition are computed to be 0.84 mg m−2d−1 for sulfur, 4.15 μgm−2d−1 for lead and 0.0013 μgm−2d−1 for cadmium. A variation factor is derived from a sensitivity analysis. This factor amounts to 2.3−2.8 for the concentrations and 2.6−3.1 for the deposition, depending on the pollutant.  相似文献   

11.
The cyclone/annular denuder/filter pack sampling system (ADS) was used to collect and evaluate ambient air pollutants in Chicago. Eighty-one 12-h samples, equally divided into day/night intervals, were collected from April 1990 to March 1991. The chemical species measured were HNO3, HNO2, SO2 and NH3 in the gas phase, and SO42−, NO3, NH4+, and H+ in the particulate phase.The ADS data were collected simultaneously with PM10 samples. The particulate matter was analysed for elemental composition. These compositions were combined with the ADS observations and subjected to evaluation using a chemical mass balance receptor model (CMB). From the CMB analysis, the sum of the contributions from soil (15%), mobile (14%), incinerator (2%), coal (0.6%), steel (0.3%) and refinery (0.2%) was 32% of the PM10. NO3, which was not included in the fingerprints, represented an additional 9% of the PM10. Residual SO42− and residual organic carbon, possibly formed in the atmosphere, represented an additional 22 and 20% of the PM10, respectively, leaving only 17% from other unidentified sources. From the standpoint of source contributions of sulfur and nitrogen compounds, coal combustion (23%) and refinery emissions (23%) are the major contributors of ambient sulfur (with 49% from unidentified sources). Mobile sources (87%) contributed most of the ambient nitrogen (with only 2% from unidentified sources).  相似文献   

12.
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   

13.
The pH is not sufficient to characterize the acidity of precipitation, but rather its acid-base components must be described. The chemistry of natural emission sources as well as the mechanism of precipitation formation determine the chemistry of precipitation at mid-latitude, Northern Hemisphere locations. With the ocean biota as a source of atmospheric aerosol SO42−, it is expected that this “background” chemistry will be dominated by SO42−. For the purpose of this study, background was defined as a remote site generally upwind of urban areas, with the additional requirement that samples with evidence of contamination by anthropogenic sources be excluded. Canadian and U.S. data from long term precipitation monitoring sites along the coasts of British Columbia, Oregon, and Washington were evaluated to estimate a background SO42− concentration in rainwater. In addition to screening the data for charge balance, collection efficiency, and anthropogenic influence, the data were corrected for SO42− associated with sea salt. The results of this analysis suggest that the mid-latitude, Northern Hemisphere background excess SO42− concentration in rainfall occurs most frequently in the range of 2–16 μeqℓ−1 with a mean of 5.5 μeqℓ−1 and an average measured pH of 5.3.  相似文献   

14.
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   

15.
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   

16.
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   

17.
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   

18.
During a joint U.S./U.S.S.R. research cruise from 3 May to 27 July 1987 both total and fine (< 2 μm) particulate material was sampled. This cruise started in the Hawaiian Islands and then proceeded to the Kamchatka peninsula, south to Wellington, New Zealand, south of Australia into the Indian Ocean, to Singapore and then returned to the Hawaiian Islands by sailing just north of the Equator. Particulate samples, collected on quartz fiber and Teflon filters, were analysed for organic and elemental carbon by transmission thermo-optical carbon analysis and for trace elements by energy dispersive X-ray fluorescence.In the Northern Hemisphere the total particulate, organic carbon and elemental carbon concentration ranges were, respectively, 10–25, 0.5–2.5 and 0–0.3 μg m−3. In the Southern Hemisphere they were, respectively, 5–10, <0.6 and <0.02 μg m−3. In the Northern Hemisphere the fine particulate concentration range was 2–15 μg m−3 and the fine fraction varied from 20 to 80% of total aerosol loading. In the Southern Hemisphere the fine particulate loading was 1.2–1.7 μg m−3 and was usually less than 20% of the total particulate mass.Chemical mass balance (CMB) modeling was used to determine possible anthropogenic particulate contributions to the ocean aerosol. Readily available source profiles were used for CMB modeling. Sea-salt aerosol was represented by either the conventional EPA marine source profile or by the average of ambient ocean aerosols sampled in very clean mid-ocean regions. Usually 60–90% of ambient particulate mass was “explained” by the CMB model. Sources such as soil, catalytic auto emissions and wood-burning emissions were found to be possible contributors to the ocean aerosol, especially in the Northern Hemisphere. Anthropogenic contributions were estimated to contribute from 10 to 30% of oceanic aerosol mass. Emissions from a hugh forest fire that burned in northern China during the spring of 1987 were possibly detected, but the CMB model cannot distinguish this source from emissions from heating and cooking with wood.Since anthropogenic emissions are mainly combustion emissions which usually contain a large carbon component, carbon data is essential to CMB modeling. The relatively good CMB results obtained in this study suggest that it might be useful to develop source profiles for major emission sources in those countries which contribute most directly to oceanic aerosols. Perhaps characteristic national or regional source profiles could be developed.  相似文献   

19.
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   

20.
In the present work we report the results of the analysis of the aerosol sampled in an industrial area in the neighborhood of the city of Barcelona using the exploratory FA technique. For this purpose samples of aerosol have been collected and analyzed for Zn, Pb, Ni, Mn, Fe, V, Ca and Al as well as for NO3, Br, SO2−4 and Cl. After performing the factor analysis on the correlation matrix the factors have been rotated by means of the VARIMAX procedure. Finally, it is shown that the combination of metals and anions as tracers in addition to the use of factor analysis as a receptor model is satisfactory.  相似文献   

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