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1.
During the Arctic Gas and Aerosol Sampling Program (AGASP) in March 1983, two distinctly different mechanisms for transporting stratospheric air into the Arctic troposphere were documented. A tropopause folding event, associated with an Arctic front, injected ‘perturbed’ polar stratospheric air into the troposphere. This perturbed polar stratospheric air was characterized by enhanced condensation nuclei concentrations (up to 1800 cm−3), enhanced aerosol light scattering (up to 90 × 10−6m−1), and crustal aerosol particles of probable volcanic origin.The second mechanism, large-scale anticyclonic subsidence, transported relatively ‘clean’ stratospheric air into the Arctic troposphere. This clean stratospheric air was characterized by relatively low condensation nuclei concentrations (maximum of 300 cm−3), low aerosol light scattering ([5–7] × 10−6 m−1), and the absence of detectable crustal particles.  相似文献   

2.
Airborne particles of diameter > 0.4 μm reaching Dye 3, Greenland during April–May 1983 were highly variable in size and concentration from day to day. Five-day backward air mass trajectories suggest the importance of long-range transport from more northerly latitudes on days with high concentrations; particle sizes were larger on these days. Lower concentrations and smaller particle sizes were associated with transport from the south. It is inferred that Dye 3 may receive material emitted from Eurasian sources and transported over the Pole, similar to inferences for more northern Arctic sites.Elemental analysis of individual particles showed an abundance of crustal material, with many particles also containing sulfur. Bulk chemical analyses of airborne particles and fresh snow, collected during three snowstorms where ice nucleation dominated, provided data which were used to estimate mass-basis scavenging ratios. Average scavenging ratios were in the range ~1000–2000 for the crustal elements Al, Fe, K, Mg, Mn, and Na. Similar values were observed for Cd, Cu and NO3. The corresponding ratios for Pb and SO42− averaged less than 200. These ratios were used with precipitation rate data to estimate wet deposition velocities in the order of ~2 cm s−1 for the first nine species, and ~0.2 cm s−1 for Pb and SO42−. Comparing fresh and older surface snow concentrations gave an average dry deposition velocity of roughly 0.2 cm s−1 for the crustal elements, with the small fraction of large particles (~5–10 μm) dominating deposition; much smaller values were associated with the remaining species. When used with other data in the literature, the results of this study suggest that total deposition velocities of Pb and SO42− may be as small as 0.05 cm s−1 in relatively dry regions of the Arctic.  相似文献   

3.
Pine pollen concentrations in air at a semi-remote site in northern Wisconsin attained levels of 18 and 25 μ m−3 in late May and early June of 1979 and 1981, respectively. The upper and lower limits for the deposition velocity of pine pollen at this site are approximately 30 and 1.3 cm s−1, respectively. Consequently, the average annual pine pollen flux at this location for 1979 and 1981 was between 8.0 and 0.35 g m−2. Deposition of total phosphorus and organic C by pollen dispersal are about 5–100% and 11–240%, respectively, of the measured bulk atmospheric loading rate in the region. Pine pollen fluxes of water-extractable K are about 10–230% of the average annual wet deposition, while the fluxes of waterextractable NO3 and SO4−2 by pollen appear to be negligible in comparison to the total atmospheric deposition (wet plus dry deposition) by other particles. The annual pine pollen flux to Crystal Lake, an oligotrophic seepage lake in the region, was estimated to be 6.5 g m−2 during 1981. The deposition of total P by pollen to this lake was 5.8 kg a−1, which is 45 % of the external input of total phosphorus. About 60% of the total P in samples of Pinus strobus and P. resinosa was dissolved reactive P, which is readily available for plant uptake. Because P is the limiting nutrient for many lacustrine systems and pine pollen dispersal coincides with the period of phytoplankton blooms in temperate-region lakes, this episodic input of P may represent an important source for seepage lakes whose external inputs are dominated by atmospheric deposition.  相似文献   

4.

From November 1995 to October 1996 and from October 1997 to September 1998, samples of wet precipitation, cloud water, as well as of reactive gases and particulate matter, were collected at three elevational levels (920 m, 1280 m and 1758 m a.s.l.) in Achenkirch, Austria. The samples were analysed for ammonium and nitrate in wet precipitation and in cloud water, for ammonia, nitric acid and nitrogen dioxide in the gas phase and for particulate ammonium and particulate nitrate in aerosol. Total nitrogen deposition was calculated combining measured concentrations in wet, dry and occult depositions with the corresponding deposition fluxes. Two multilayer deposition models were used for the calculation of dry and occult deposition. The total nitrogen input in 1995/96 was estimated to be 29 kg N ha−1a−1 at the Christlumkopf station (1758 m), 20 kg N ha−1a−1 at the Christlumalm station (1280 m) and 28 kg N ha−1a−1 at the Talboden station (930 m). Respective data for the 1997/98 observation period were 31 kg N ha−1a−1 at the Christlumkopf station (1758 m) and 18 kg N ha−1a−1 at the Mühleggerköpfl station (920 m). Critical Loads of nitrogen for coniferous forests were exceeded significantly near-source regions represented by areas of intense agricultural use and at high elevation sites.

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5.
The airborne concentrations of soluble ions in fine particles and coarse particles have been measured indoors and outdoors at telephone offices in Wichita, Kansas and Lubbock, Texas, These concentrations are compared with the mean annual indoor surface accumulations of these ions on zinc and aluminum structural surfaces. On average, the major soluble ions contained in fine airborne particles are ammonium, sulfate, and nitrate, while those contained in coarse particles are calcium and nitrate. In the fine mode, potassium and chloride have indoor/outdoor ratios that are larger than those observed for the other ionic species, indicating the existence of a significant indoor source. In the coarse mode, similar comparisons show that sodium, chloride, and sometimes sulfate have significant indoor sources. For chloride, a simple model has been used for apportioning surface accumulation at each location due to corrosive chlorine gases, coarse particles, and fine particles. For other ions where corrosive gases are not important, the accumulation has been apportioned between coarse and fine particles. From these data, experimental deposition velocities for fine mode sulfate ions and coarse mode calcium ions were calculated to be 0.003 and l.0 cms−1, respectively, at Wichita, while those at Lubbock were 0.005 and 0.2 cms.  相似文献   

6.
The mass concentrations of inorganic ions, water-soluble organic carbon, water-insoluble organic carbon and black carbon were determined in atmospheric aerosol collected at three European background sites: (i) the Jungfraujoch, Switzerland (high-alpine, PM2.5 aerosol); (ii) K-puszta, Hungary (rural, PM1.0 aerosol); (iii) Mace Head, Ireland (marine, total particulate matter). At the Jungfraujoch and K-puszta the contribution of carbonaceous compounds to the aerosol mass was higher than that of inorganic ions by 33% and 94%, respectively. At these continental sites about 60% of the organic carbon was water soluble, 55–75% of the total carbon proved to be refractory and a considerable portion of the water soluble, refractory organic matter was composed of humic-like substances. At Mace Head the mass concentration of organic matter was found to be about twice than that of nonsea-salt ions, 40% of the organic carbon was water soluble and the amount of highly refractory carbon was low. Humic-like substances were not detected but instead low molecular weight carboxylic acids were responsible for about one-fifth of the water-soluble organic mass. These results imply that the influence of carbonaceous compounds on aerosol properties (e.g. hygroscopic, optical) might be significant.  相似文献   

7.
Wet deposition of phosphorus was measured at 10 sites across Florida originally established as part of the Florida Atmospheric Mercury Study conducted between 1992 and 1996. Monthly integrated samples were collected and analyzed using a total analytical protocol that incorporated “clean lab” conditions for sample equipment preparation and Aerochem Metrics collectors modified for suitability to use for ultra-trace elements. Samples also were collected aboard 15 m towers to minimize any influence on measured deposition by insects, etc., and locally originating particles that do not contribute to true net deposition. Extensive replication of samples in the field was conducted (ca. 83%). The average absolute difference between replicates was 16.2%, with a median absolute difference of 9.5%. Replicate precision was poorest for concentrations above 0.080 mg P l−1, suggesting that concentrations above this level are contaminated.The wet deposition concentrations and fluxes of phosphorus measured in this study are appreciably lower than those reported by previous investigators for wet deposition in Florida, and lie at the lower end of measurements reported in the recent literature. For example, the volume weighted mean concentration and flux for wet deposition across all our study sites averaged 0.005 mg P l−1 and 7.5 mg P m−2 yr−1, respectively, which is approximately 50% and 32% lower than that reported by Hendry et al. (1981 in Atmospheric Pollutants in Natural Waters. Ann Arbor Science, Ann Arbor. MI, pp. 199–215). Our lower measurements likely reflect three factors: (1) the ultra-trace element sampling and analytical protocols; (2) improved collector design to eliminate sampling artifacts (e.g., splash-off contamination and transfer of contaminants from the dry bucket); and (3) placement of collectors off the ground surface. Lower VWM concentrations were observed near the Florida coast; otherwise, strong spatial patterns across the state were absent. Seasonal variations in VWM also were not pronounced, although deposition fluxes were highest during the summer wet season in response to the strong seasonal distribution of rainfall.  相似文献   

8.
Size-resolved fog drop chemical composition measurements were obtained during a radiation fog campaign near Davis, California in December 1998/January 1999 (reported in Reilly et al., Atmos. Environ. 35(33) (2001) 5717; Moore et al., Atmos. Environ. this issue). Here we explore how knowledge of this size-dependent drop composition—particularly from the newly developed Colorado State University 5-Stage cloud water collector—helps to explain additional observations in the fog environment. Size-resolved aerosol measurements before and after fog events indicate relative depletion of large (>2 μm in diameter) particles during fog accompanied by a relative increase in smaller aerosol particle concentrations. Fog equivalent air concentrations suggest that entrainment of additional particles and in-fog sedimentation contributed to observed changes in the aerosol size distribution. Calculated deposition velocities indicate that sedimentation was an important atmospheric removal mechanism for some species. For example, nitrite typically has a larger net deposition velocity than water and its mass is found preferentially in the largest drops most likely to sediment rapidly. Gas–liquid equilibria in fog for NO3/HNO3, NH4+/NH3, and NO2/HONO were examined. While these systems appear to be close to equilibrium or relative equilibrium during many time periods, divergences are observed, particularly for low liquid water content (<0.1 g m−3) fogs and in different drop sizes. Knowledge of the drop size-dependent composition provided additional data useful to the interpretation of these deviations. The results suggest that data from multi-stage cloud water collectors are useful to understanding fog processes as many depend upon drop size.  相似文献   

9.
In a study on the mechanism of the air-pollution induced deterioration of the limestone St. Rombouts cathedral in Mechelen, Belgium, automated electron-probe X-ray micro-analysis combined with multivariate analysis was used to characterize the suspension particles in run-off water and in local wet and dry deposition samples.Altogether about 10,000 individual particles were sized, analyzed and classified, according to their chemical composition. It was found that the run-off water samples were highly enriched in CaCO3 particles, resulting from the stone-erosion by overflowing rainwater, while the Si-rich group was the most abundant one in the deposition samples. Several other particle types were found. Ion chromatography analysis of the run-off water showed 200–1700mg l−1 of sulphate and 20–110mg l−1 of nitrate.  相似文献   

10.
The organic carbon content of wet and bulk deposition was measured from February through to December 1981 at four stations surrounding Chesapeake Bay. Organic carbon is removed from the atmosphere in association with both wet and dry deposition. Regional yearly wet and dry depositional rates were approximately equal, with a total yearly deposition rate of 11.3 g C m−2 y−1. Atmospheric deposition provides an important flux of organic material to Chesapeake Bay and must be considered if biogeochemical cycles are to be fully understood.  相似文献   

11.
为了研究高原湖泊底泥沉积物中磷的释放负荷,对贵州红枫湖区10个地区的沉积物进行了磷形态分析。选取10个采样点中5个典型区域,研究结果表明,底泥中各形态磷占总磷比例Org-P为58.6%,NaOH-P为29.91%,Ca-P为11.48%,底泥中主要的磷形态为有机磷。上覆水溶解性总磷酸盐(TSP)与底泥中各形态磷的相关性研究表明,底泥中的Ca-P与上覆水中的TSP几乎没有相关性,NaOH-P与Org-P与上覆水的TSP有较高的相关性(R2>0.94),而底泥中的总磷(TP)与上覆水中的TSP相关性最高(R2>0.98),底泥中这种形态的结构有利于抑制底泥的释放。研究表明,在10点位样品中,间隙水中TP和SRP(溶解性正磷酸)浓度远大于上覆水体中相应磷形态的浓度,间隙水中TP平均浓度为0.37 mg/L,SRP平均浓度为0.18 mg/L,上覆水体中TP平均浓度为0.10 mg/L,SRP平均浓度为0.02 mg/L,间隙水中TP、SRP与上覆水中TP、SRP存在了一种浓度梯度。  相似文献   

12.
Because aerosol particle deposition is an important factor in indoor air quality, many empirical and theoretical studies have attempted to understand the process. In this study, we estimated the deposition rate of aerosol particles on smooth aluminum surfaces inside a test chamber. We investigated the influence of turbulent intensity due to ventilation and fan operation. We also investigated two important processes in particle deposition: turbophoresis, which is significant for micron particles, and coagulation, which is relevant to ultrafine particles (UFP diameter <0.1 μm) at high particle concentrations. Our analysis included semi-empirical estimates of the deposition rates that were compared to available deposition models and verified with simulations of an aerosol dynamics model. In agreement with previous studies, this study found that induced turbulent intensity greatly enhanced deposition rates of fine particles (FP diameter <1 μm). The deposition rate of FP was proportional to the ventilation rate, and it increased monotonically with fan speed. With our setup, turbophoresis was very important for coarse particles larger than 5 μm. The coagulation of aerosol particles was insignificant when the particle concentration was less than 104 cm?3 during fan operation. The model simulation results verified that the aerosol dynamics module incorporated in our Multi-Compartment and Size-Resolved Indoor Aerosol Model (MC-SIAM) was valid. The behavior of aerosol particles inside our chamber was similar to that found in real-life conditions with the same ventilation rates (0.018–0.39 h?1) and similar air mixing modes. Therefore, our findings provide insight into indoor particle behavior.  相似文献   

13.
In order to characterize atmospheric aerosol in the São Paulo Metropolitan Area, aerosols were sampled during the winter months of August 1999 and August 2000. A micro-orifice uniform deposit impactor (MOUDI) was used. Samples were submitted to gravimetry, as well as to proton-induced X-ray emission (PIXE), carbon (black and organic) and ion-chromatography analysis. These analyses supplied information about mass concentrations and physicochemical properties of the particles. Due to the higher humidity, which can increase soluble particles diameters, and reduced atmospheric stagnation seen in 2000, average PM10 concentrations were higher (105 μg m−3) in the winter of 1999 than in the winter of 2000 (60 μg m−3). The PIXE analysis revealed metals and metal compounds, soil-derived elements, Si-rich particles, sulfates, carbonates, chlorides and other anthropogenic air-borne particles, supposing molecules in their usual composition. Mass balance for PM2.5 revealed significant participation of organic and black carbon, probably resulting from diesel burning by the heavy-duty fleet.  相似文献   

14.
Concentrations of a suite of trace elements (Al, Ag, As, Cd, Co, Cr, Cu, Fe, Ni, Pb, Sr, V, Zn) were measured in aerosol and precipitation samples collected at a coastal site in New Castle, NH, from August 1996, through July 1997. Metal concentrations in aerosol and precipitation exhibit a high degree of temporal variability over the annual cycle, varying by approximately one order of magnitude or less for aerosol metals and by ∼2–3 orders of magnitude in precipitation. Estimates of the total annual atmospheric deposition of metals to the Gulf of Maine range from ∼103 kg yr−1 for Ag, ∼104–105 kg yr−1 for the majority of metals, and ∼106 kg yr−1 for the crustal elements Al and Fe.  相似文献   

15.
Atmospheric phosphorus in the northern part of Lake Taihu, China   总被引:1,自引:0,他引:1  
Luo J  Wang X  Yang H  Yu JZ  Yang L  Qin B 《Chemosphere》2011,84(6):785-791
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16.
Wet and dry deposition as collected by a bucket were measured at two sites in southeastern Michigan for two years. The precipitation had an average pH of 4.27 and a SO2−4 to NO3 ratio of 2.0. Particulate dry deposition velocities of 0.6 cm s−1 for SO2−4 and NO3 and > 2 cm s−1 for Cl, Ca2+, Mg2+,Na+ and K+ were calculated. The ambient particle composition, dry bucket collection and wet deposition were compared at two sites, one urban and the other rural. Higher ambient particle concentrations and dry deposition rates were measured at the urban site than the rural site, indicating the influence of local emissions. However, local emissions had no effect on the wet deposition concentrations. The influence of more distant source regions was examined by separating the precipitation events by wind direction. The events from the south and east had the highest SO2−4 to NO3 ratios, which corresponded to the areas with the highest sulfur emissions. NO3 showed no directional dependence.Wet deposition was examined for the effect of storm type and seasonal trends. Contrary to a recent study on Long Island, we found higher concentrations of H+, SO2−4 and NH+4 in winter rain compared to snow. The wet deposition concentrations of H+, SO2−4, and NH+4 were highest in the summer, while only Na+ and Cl concentrations were highest in the winter, presumably due to winter road salting. The total deposition of acidic ions was highest in the summer and lowest in the winter, due both to lower concentrations and lower precipitation volumes in the winter. The dry deposition as collected by a bucket accounted for 1 % of total H+ deposition, 21 % of SO2−4 deposition, 27% of NO3 deposition, 50% of Cl deposition and 61 % of Ca2+ deposition.  相似文献   

17.
The aerosol in a non-industrial town normally is dominated by emissions from vehicles. Whereas gasoline-powered cars normally only emit a small amount of particulates, the emission by diesel-powered cars is considerable. The aerosol particles produced by diesel engines consist of graphitic carbon (GC) with attached hydrocarbons (HCs) including also polyaromatic HCs. Therefore the diesel particles can be carcinogenic. Besides diesel vehicles, all other combustion processes are also a source for GC; thus source apportionment of diesel emissions to the GC in the town is difficult.A direct apportionment of diesel emissions has been made possible by marking all the diesel fuel used by the vehicles in Vienna by a normally not occurring and easily detectable substance. All emitted diesel particles thus were marked with the tracer and by analyzing the atmospheric samples for the marking substance we found that the mass concentrations of diesel particles in the atmosphere varied between 5 and 23 μg m−3. Busy streets and calm residential areas show less difference in mass concentration than expected. The deposition of diesel particles on the ground has been determined by collecting samples from the road surface. The concentration of the marking substance was below the detection limit before the marking period and a year after the period. During the period when marked diesel fuel was used, the concentrations of the diesel particles settling to the ground was 0.012–0.07 g g−1 of collected dust.A positive correlation between the diesel vehicle density and the sampled mass of diesel vehicles exists. In Vienna we have a background diesel particle concentration of 11 μg m−3. This value increases by 5.5 μg m−3 per 500 diesel vehicles h−1 passing near the sampling location.The mass fraction of diesel particles of the total aerosol mass varied between 12.2 and 33%; the higher values were found in more remote areas, since diesel particles apparently diffuse easily.Estimates of diesel particle concentration by emission inventory or by using lead concentrations as an indicator for vehicle emissions gave similar values to those obtained in this study.Using available cancer risk data and diesel particle concentration found in this study, 1–2.6 additional lung cancers per 100,000 persons yr−1 breathing diesel emissions in the measured concentration the whole lifetime can be expected.  相似文献   

18.
A laboratory study was conducted to examine formation of secondary organic aerosols. A smog chamber system was developed for studying gas–aerosol interactions in a dynamic flow reactor. These experiments were conducted to investigate the fate of gas and aerosol phase compounds generated from hydrocarbon–nitrogen oxide (HC/NOx) mixtures irradiated in the presence of fine (<2.5 μm) particulate matter. The goal was to determine to what extent photochemical oxidation products of aromatic hydrocarbons contribute to secondary organic aerosol formation through uptake on pre-existing inorganic aerosols in the absence of liquid water films. Irradiations were conducted with toluene, p-xylene, and 1,3,5-trimethylbenzene in the presence of NOx and ammonium sulfate aerosol, with propylene added to enhance the production of radicals in the system. The secondary organic aerosol yields were determined by dividing the mass concentration of organic fraction of the aerosol collected on quartz filters by the mass concentration of the aromatic hydrocarbon removed by reaction. The mass concentration of the organic fraction was obtained by multiplying the measured organic carbon concentration by 2.0, a correction factor that takes into account the presence of hydrogen, nitrogen, and oxygen atoms in the organic species. The mass concentrations of ammonium, nitrate, and sulfate concentrations as well as the total mass of the aerosols were measured. A reasonable mass balance was found for each of the aerosols. The largest secondary organic aerosol yield of 1.59±0.40% was found for toluene at an organic aerosol concentration of 8.2 μm−3, followed by 1.09±0.27% for p-xylene at 6.4 μg m−3, and 0.41±0.10% for 1,3,5-trimethylbenzene at 2.0 μg m−3. In general, these results agree with those reported by Odum et al. and appear to be consistent with the gas–aerosol partitioning theory developed by Pankow. The presence of organic in the aerosol did not affect significantly the hygroscopic properties of the aerosol.  相似文献   

19.
Number distribution data for 0.1–45 μm diameter aerosol were obtained using optical counting and sizing probes flown over the Alaskan Arctic during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), flights 201–203. Due to noise present in the lowest size channels of the optical probes, estimates of the H2SO4 component of Arctic haze were not attempted. Large particle (> 0.5 μm diameter) results are presented here. Large particle number and volume concentration were determined along with estimated mass, which was generally </ 0.1μg m−3. Lognormal fitting to > 0.3 μg m−3 mass loading sizedistributed aerosol data produced a means for comparing volume geometric median diameters (VGMD) for these higher-mass time intervals. These VGMDs showed that solid crustal particles previously observed during AGASP-II had VGMDs in the 1.2–1.6 μm range and that the shape of these fitted lognormal distributions was essentially constant. This result suggests very-long-range transport from a distant crustal source and, in conjunction with aerosol physical and chemical characterization data, argues against the presence of the Mt. Augustine eruptive particles during AGASP-II Alaskan Arctic sampling.  相似文献   

20.
Stable carbon isotope ratio (δ13C) data can provide important information regarding the sources and the processing of atmospheric organic carbon species. Formic, acetic and oxalic acid were collected from Zurich city in August–September 2002 and March 2003 in the gas and aerosol phase, and the corresponding δ13C analysis was performed using a wet oxidation method followed by isotope ratio mass spectrometry. In August, the δ13C values of gas phase formic acid showed a significant correlation with ozone (coefficient of determination (r2) = 0.63) due to the kinetic isotope effect (KIE). This indicates the presence of secondary sources (i.e. production of organic acids in the atmosphere) in addition to direct emission. In March, both gaseous formic and acetic acid exhibited similar δ13C values and did not show any correlation with ozone, indicating a predominantly primary origin. Even though oxalic acid is mainly produced by secondary processes, the δ13C value of particulate oxalic acid was not depleted and did not show any correlation with ozone, which may be due to the enrichment of 13C during the gas - aerosol partitioning.The concentrations and δ13C values of the different aerosol fractions (water soluble organic carbon, water insoluble organic carbon, carbonate and black carbon) collected during the same period were also determined. Water soluble organic carbon (WSOC) contributed about 60% to the total carbon and was enriched in 13C compared to other fractions indicating a possible effect of gas - aerosol partitioning on δ13C of carbonaceous aerosols. The carbonate fraction in general was very low (3% of the total carbon).  相似文献   

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