Condensable vapours such as sulphuric acid form aerosol in the atmosphere by the competing mechanisms of condensation on existing aerosol and the nucleation of new aerosol. Observational and theoretical evidence for the relative magnitudes of the competing processes is reviewed, and a number of general conclusions are made. Condensation is sensitive to the sticking probability of sulphuric acid molecules on aerosol particles, but there is now good evidence that it should be close to unity. In this case, equilibration timescales between acid vapour and the aerosol in most of the atmosphere are of the order of minutes or less, so that the acid concentration on such timescales given simply by the production rate times the equilibration time. When the acid concentration exceeds a threshold, nucleation will occur. The atmospheric aerosol therefore follows a history of initial formation in a nucleation burst followed by growth and coagulation with final removal by precipitation. This leads to the inverse correlation between aerosol number concentration and mass concentration found by Clarke (1992. Journal of Atmospheric Chemistry 14, 479–488) in the free troposphere. Binary homogeneous nucleation of sulphuric acid/water droplets, for which various simplified rates are compared, may dominate in such regions, but other mechanisms are possible elsewhere. A detailed analysis is performed of the number concentrations, removal rates, and masses of the components of the different types of global aerosols proposed empirically by Jaenicke (1993. Tropospheric Aerosols, Aerosol-Cloud-Climate Interaction. Academic Press, New York). There is a striking correlation between number concentrations in the nucleation and accumulation modes; and the giant aerosol mode, which if it is present dominates the mass, has little effect on the gas-to-particle conversion process. The mass of the atmospheric aerosol is therefore uncorrelated with the magnitude of molecular aerosol removal by condensation. 相似文献
The first observations of size-dependent cloud and fog drop inorganic ion and trace metal concentrations obtained using the Colorado State University 5-Stage cloud water collector (CSU 5-Stage) during field studies of orographic clouds (Whiteface Mountain, NY, July 1998) and radiation fogs (Davis, CA, January 1999) are reported. Although some mixing between drop sizes occurs, the CSU 5-Stage effectively separates the largest drops (>≈30 μm in diameter) from the smallest ones (<≈10 μm in diameter) permitting the discernment of size-dependent drop composition not possible with previous two- or three-stage collectors. At Whiteface, pH and the concentrations of the “major” ions −NH4+, NO3−, and SO42−—appeared largely independent of drop size as measured by a two-stage collector. The same major ion concentrations differed in Davis fogs by up to a factor of approximately 10 in the two-stage collector with consistently higher small drop concentrations. In both locations, CSU 5-Stage data generally indicate a greater range of concentrations is present across the drop size spectrum. CSU 5-Stage data show “U”- shaped profiles of major ion concentration vs. drop size at Whiteface and “L”- shaped profiles at Davis and the maximum/minimum concentration differences between fractions increased up to a factor of 2 (Whiteface) and 30 (Davis). Lower concentration species at both locations showed multiple concentration vs. drop size profiles with CSU 5-Stage data again exhibiting more variability than observed with the two-stage collector. While rarely reported, significant nitrite concentrations—relatively higher in the larger drops—were observed, and copper concentrations merit further investigation in the Davis fogs. The findings presented here are consistent with other studies. The implications and benefits of the increased resolution of size-dependent drop composition provided by the CSU 5-Stage are explored for the Davis fogs in a companion paper (Moore et al., Atmos. Environ. (2004), this issue). 相似文献
The size distribution of ambient air particles and associated organic pollutants, such as polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), and organochlorine pesticides (OCPs) including hexachlorocyclohexanes (HCHs), DDT and metabolites, etc., was investigated at a traffic-impacted site of Thessaloniki, Greece. Investigation took place during wintertime of 2006 at two heights above ground: at the street level (1.5 m) and at the rooftop level (15 m). Size-resolved samples (<0.95 μm, 0.95–1.5 μm, 1.5–3 μm, 3–7.5 μm and >7.5 μm) were concurrently collected from the two height levels using five-stage high volume cascade impactors. At both heights, particle mass exhibited bimodal distribution with peaks in the 0.95–1.5 μm and the 3–7.5 μm size fractions, whereas most organic pollutants exhibited one peak at 0.95–1.5 μm. Apart from the 0.95–1.5 μm fraction, particle concentrations of all size ranges were significantly higher at the street level than at the rooftop as a result of more intensive vehicular emissions and road dust resuspension. On the contrary, the concentrations of most organic pollutants did not differentiate significantly between the two elevations. 相似文献
Atmospheric aerosols have been collected at four sites around Japan during 2000. From systematically monitoring the major (Na, Mg, Al, K, Ca, and Fe) and trace (Rb and Sr) elements, along with the Sr isotope composition, we have tried to estimate the contribution of long-range-transported Asian dust (“Kosa”) to the atmospheric aerosols.The results are summarized as follows:(1) The concentration of each element in the aerosols increased during the “Kosa” period. The increase was particularly obvious in samples collected on 8 April 2000, when the “Kosa Phenomenon” was observed at all the sampling sites in Japan, 2 days after a very heavy dust storm had occurred in China.(2) The Rb–Sr isotopic diagram shows a two-component mixing relationship: one with a high 87Sr/86Sr ratio and a high 87Rb/86Sr ratio, and the other with a low 87Sr/86Sr ratio and a low 87Rb/86Sr ratio. There is a significant difference between that of the expected end member of the Asian dust and that of the reported Asian loess, which is thought to be the possible source of the components of the “Kosa”, although the lower component is consistent with the local component at Wako.(3) Plots of the 87Sr/86Sr ratio vs the Ca/Al and Sr/Al ratios support a two-component mixing suggested by the Rb–Sr systematics, and they indicate that the contributing continental soil components to the “Kosa” aerosols should be composed of the silicate fraction of Asian loess.(4) The discrepancy in the Rb–Sr systematics between the expected end member and the possible sources may be caused by the dissolution of the Ca-bearing minerals via long-range dust transport, or by a combination of source characteristics and grain size separation. 相似文献
In 2005, the concentrations of various metals and organic pollutants were analyzed in soils collected in different areas of Tarragona (Catalonia, Spain), where an important chemical/petrochemical complex is located. The levels of seven elements (As, Cd, Cr, Hg, Mn, Pb and V), as well as those of polychlorinated biphenyls (PCBs), polychlorinated naphthalenes (PCNs) and polycyclic aromatic hydrocarbons (PAHs) were determined in soils, and compared with those obtained in a background study carried out in 2002. Only Cd and Pb showed significant higher concentrations in the petrochemical zone, while no significant differences were found for the remaining elements. In turn, vanadium was the only element showing a significant increase in the concentration between 2002 and 2005. With regard to the organic pollutants, no significant differences were found according to the area of sampling. However, an increase in naphthalene levels was observed during the period 2002-2005 in soils of the chemical and petrochemical areas. According to the present results, it is suggested that the levels of vanadium must be periodically monitored to assure that the important industrialization of Tarragona does not mean health risks for the population living near the complex. 相似文献
We summarize the results from the various measurements and the inter-sampler comparisons from Southeastern Aerosol and Visibility Study (SEAVS), a study with one of its objectives to test for closure among chemical, gravimetric and optical measurements of atmospheric aerosol particles. Sulfate and organics are the dominant components of the SEAVS fine particles (nominally, particles with aerodynamic diameter < or = 2.5 microns) but between 28 and 42% (range over various samplers) of the gravimetrically measured total fine particle concentration is unidentified by the chemical measurements. Estimates of water associated with inorganic components and measurement imprecision do not totally explain the observed difference between gravimetric and chemical measurements. We examine the theoretical and empirical basis for assumptions commonly made in the published literature to extrapolate total fine particle concentration on the basis of chemical measurements of ions, carbon and elements. We then explore the more general question of closure using the SEAVS data as well as data from other, similar studies reported in the literature. In so combining the SEAVS measurements with other similar studies, we find a strong association between organic carbon and the unidentified component, that is, the fraction of the total fine particle concentration not identified by chemical measurements. We offer several tenable hypotheses for the relationship between the organic and unidentified components that deserve to be tested in future work. Specifically, we hypothesize that (1) errors in the sampling and analysis of organic carbon; (2) estimates of organic mass from measurements of organic carbon; and/or (3) water absorption by organics may all contribute to the observed relationship. 相似文献
The seasonal variability in the mass concentration and chemical composition of atmospheric particulate matter (PM10 and PM2.5) was studied during a 2-year field study carried out between 2010 and 2012. The site of the study was the area of Ferrara (Po Valley, Northern Italy), which is characterized by frequent episodes of very stable atmospheric conditions in winter. Chemical analyses carried out during the study allowed the determination of the main components of atmospheric PM (macro-elements, ions, elemental carbon, organic matter) and a satisfactory mass closure was obtained. Accordingly, chemical components could be grouped into the main macro-sources of PM: soil, sea spray, inorganic compounds from secondary reactions, vehicular emission, organics from domestic heating, organics from secondary formation, and other sources. The more significant seasonal variations were observed for secondary inorganic species in the fine fraction of PM; these species were very sensitive to air mass age and thus to the frequency of stable atmospheric conditions. During the winter ammonium nitrate, the single species with the highest concentration, reached concentrations as high as 30 μg/m3. The intensity of natural sources was fairly constant during the year; increases in natural aerosols were linked to medium and long-range transport episodes. The ratio of winter to summer concentrations was roughly 2 for combustion product, close to 3 for secondary inorganic species, and between 2 and 3 for organics. The winter increase of organics was due to poorer atmospheric dispersion and to the addition of the emission from domestic heating. A similar winter to summer ratio (around 3) was observed for the fine fraction of PM. 相似文献
Tonghui River, a typical river in Beijing, People's Republic of China, was studied for its water and sediment quality, by determining the levels of 16 polycyclic aromatic hydrocarbons (PAHs), 12 polychlorinated biphenyls (PCBs) and 18 organochlorine pesticides in water and sediment samples. Total PAHs, PCBs and organochlorine pesticides concentrations in water varied from 192.5 to 2651 ng/l, 31.58-344.9 ng/l and 134.9-3788 ng/l, respectively. The total PAHs, PCBs and organochlorine pesticides concentrations in surficial sediments were 127-928 ng/g, 0.78-8.47 ng/g and 1.79-13.98 ng/g dry weight, respectively. The results showed that the concentration of these selected organic pollutants in sediment was higher than those in surface water. It may be due to the fact that organic hydrophobic pollutants tend to stay in the sediments. The PAHs were dominated by 2-, 3-ring components in water samples and by 3- and 4-ring compounds in sediment. For organochlorines, alpha-HCH, delta-HCH, Heptachlor, Endosulfan II, DDT are the major organochlorine pesticides in water while Heptachlor, Dieldrin and DDE composed of 95% of total organochlorine pesticides in sediment. For HCHs (HCHs=alpha-HCH+beta-HCH+gamma-HCH+delta-HCH), the predominance of alpha-HCH of total HCHs were clearly observed in water and sediment. PCB18, PCB31 and PCB52 were predominant in water, on average these compounds collectively accounted for 67% of total PCBs. But in sediment, the predominant compounds were PCB28, PCB31 and PCB153, which accounted for 71% of total PCBs in sediment. The levels of micro pollutants in our study areas were compared with other studies. 相似文献
A major problem with the analysis and investigation of combustion aerosols in the real-world environment is related to strong stochastic variations of the external and environmental parameters and factors (e.g., atmospheric turbulence, traffic fluctuations, etc.). Therefore, this paper develops new powerful statistical methods based on the canonical correlation analysis and the moving average technique, applied to combustion aerosols near a busy road. As a result, a new physical insight into the evolution of combustion aerosols and possible sources of nano-particle modes is presented and discussed. Several new particle modes are identified, analysed and associated either with trucks or cars on the road. In particular, liquid and solid particle modes are identified, and the mechanism of thermal fragmentation of solid nano-particles is used for the interpretation of the obtained results. 相似文献
To investigate the chemical composition, size distribution, and mixing state of aerosol particles on heavy pollution days, single-particle aerosol mass spectrometry was conducted during 9–26 October 2015 in Xi’an, China. The measured particles were classified into six major categories: biomass burning (BB) particles, K-secondary particles, elemental carbon (EC)–related particles, metal-containing particles, dust, and organic carbon (OC) particles. BB and EC-related particles were the dominant types during the study period and mainly originated from biomass burning, vehicle emissions, and coal combustion. According to the ambient air quality index, two typical episodes were defined: clean days (CDs) and polluted days (PDs). Accumulation of BB particles and EC-related particles was the main reason for the pollution in Xi’an. Most types of particle size were larger on PDs than CDs. Each particle type was mixed with secondary species to different degrees on CDs and PDs, indicating that atmospheric aging occurred. The mixing state results demonstrated that the primary tracers were oxidized or vanished and that the amount of secondary species was increased on PDs. This study provides valuable information and a dataset to help control air pollution in the urban areas of Xi’an.
Persistent organic pollutants (PAHs and PCBs) in soil samples from seven sites across the Seine basin were analysed. Samples were taken from industrialized, urban, suburban and remote sites. Results showed spatial differences, in terms of concentrations and congener profiles. PAH (Sigma14 PAHs) and PCB (Sigma 7 PCBs) concentrations ranged from 450 to 5650 microg kg(-1) and 0.09 to 150 microg kg(-1), respectively. A clear gradient from industrial to remote sites was highlighted, with a ratio of up to one order of magnitude for PAHs and two orders of magnitude for PCBs. Fluoranthene and pyrene were predominant, while the carcinogenic PAHs represented 15-46% of the total PAH content. Using hierarchical cluster analysis, soil samples profiles were compared and the influence of site location and potential sources were identified: automobile traffic, domestic heating, and industrial emissions were the prevalent PAHs sources in the Seine basin. PCB profiles suggested different transport patterns among congeners. For remote sites, the congener fingerprint showed a relatively higher proportion of the most volatile congeners, which were attributed to increased atmospheric residence times. Thus, PAH and PCB distributions in soils provided information on sources and evidence for short-range transport, and profiles of compounds reflected differences between regional and local emissions. This study demonstrates that soil sampling can be used to investigate spatial differences in atmospheric inputs of persistent organic pollutants based on differences in the mixtures of compounds, reflecting differences in regional and local atmospheric emissions. 相似文献
During April 1996–June 1997 size-segregated atmospheric aerosol particles were collected at an urban and a rural site in the Helsinki area by utilising virtual impactors (VI) and Berner low-pressure impactors (BLPI). In addition, VI samples were collected at a semi-urban site during October 1996–May 1997. The average PM2.3 (fine particle) concentrations at the urban and rural sites were 11.8 and 8.4 μg/m3, and the PM2.3−15 (coarse particle) concentrations were 12.8 and about 5 μg/m3, respectively. The difference in fine particle mass concentrations suggests that on average, more than one third of the fine mass at the urban site is of local origin. Evaporation of fine particle nitrate from the VI Teflon filters during sampling varied similarly at the three sites, the average evaporation being about 50–60%.The average fine particle concentrations of the chemical components (25 elements and 13 ions) appeared to be fairly similar at the three sites for most components, which suggests that despite the long-range transport, the local emissions of these components were relatively evenly distributed in the Helsinki area. Exceptions were the average fine particles Ba, Fe, Sb and V concentrations that were clearly highest at the urban site pointing to traffic (Ba, Fe, Sb) and to combustion of heavy fuel oil (V) as the likely local sources. The average coarse particle concentrations for most components were highest at the urban site and lowest at the rural site.Average chemical composition of fine particles was fairly similar at the urban and rural sites: non-analysed fraction (mainly carbonaceous material and water) 43% and 37%, sulphate 21% and 25%, crustal matter 12% and 13%, nitrate 12% and 11%, ammonium 9% and 10% and sea-salt 2.5% and 3.2%, respectively. At the semi-urban site also, the average fine particle composition was similar. At the urban site, the year round average composition of coarse particles was dominated by crustal matter (59%) and the non-analysed components (28%, mainly carbonaceous material and water), while the other contributions were much lower: sea-salt 7%, nitrate 4% and sulphate 2%. At the rural site, the coarse samples were collected in spring and summer and the percentage was clearly lower for crustal matter (37%) and sea-salt (3%) but higher for the not-analysed fraction (51%). At the semi-urban site, the average composition of coarse particles was nearly identical to that at the urban site.Correlations between the chemical components were calculated separately for fine and coarse particles. In urban fine particles sulphate, ammonium, Tl, oxalate and PM2.3 mass correlated with each other and originated mainly from long-range transport. The sea-salt ions Na+, Cl− and Mg2+ formed another group and still another group was formed by the organic anions oxalate, malonate, succinate, glutarate and methane sulphonate. Ni and V correlated strongly pointing to combustion of heavy fuel oil as the likely source. In addition, some groups with lower correlations were detected. At the rural and semi-urban sites, the correlating components were rather similar to those at the urban site, although differences were also observed. 相似文献
This study investigated particle size and density distributions of polycyclic aromatic hydrocarbons (PAHs) in two surface sediments (JZ and KF), collected from the Yellow River of Henan section, China. The concentrations of Σ15PAHs ranged from 35.6 to 45862?ng g?1 dry wt, which were greatly elevated in coarse particles and low-density fractions. The Σ15PAHs concentrations in low-density fractions were 533 (JZ) and 996 (KF) times higher than those in the corresponding high-density fractions. However, due to relatively less quantities of low-density fractions (0.27–2.33%), most of the PAHs were contributed by the high-density components. For both sediments, the influence factors of PAHs source in the environment were very complex, more so than the level of TOC and BC content. JZ sediment was dominated by 4-ring to 6-ring PAHs (61.5–75.1%), while, 2-ring to 3-ring PAHs were abundant in KF samples (39.8–72.6%). Ratios of specific PAHs reflected PAHs among the size- and density-fraction of each sediment may be contaminated by mixed of pyrolytic and petrogenic origin. Additionally, ecological risk assessment of PAHs suggested that total toxic equivalent values of PAHs in the low-density fractions were much higher than those of the corresponding high-density fractions in the studied area. 相似文献
Recently, a comprehensive air quality modeling system was developed as part of the Southern Appalachians Mountains Initiative (SAMI) with the ability to simulate meteorology, emissions, ozone, size- and composition-resolved particulate matter, and pollutant deposition fluxes. As part of SAMI, the RAMS/EMS-95/URM-1ATM modeling system was used to evaluate potential emission control strategies to reduce atmospheric pollutant levels at Class I areas located in the Southern Appalachians Mountains. This article discusses the details of the ozone model performance and the methodology that was used to scale discrete episodic pollutant levels to seasonal and annual averages. The daily mean normalized bias and error for 1-hr and 8-hr ozone were within U.S. Environment Protection Agency guidance criteria for urban-scale modeling. The model typically showed a systematic overestimation for low ozone levels and an underestimation for high levels. Because SAMI was primarily interested in simulating the growing season ozone levels in Class I areas, daily and seasonal cumulative ozone exposure, as characterized by the W126 index, were also evaluated. The daily ozone W126 performance was not as good as the hourly ozone performance; however, the seasonal ozone W126 scaled up from daily values was within 17% of the observations at two typical Class I areas of the SAMI region. The overall ozone performance of the model was deemed acceptable for the purposes of SAMI's assessment. 相似文献
Size-resolved trace metal concentrations at two background sites were assessed during a 1-year observation campaign, with the measurements performed in parallel at two mountain sites, where Mt. Dinghu (DHS) located in the rural region of Pearl River Delta (PRD) and Mt. Gongga (GGS) located in the Tibetan Plateau region. In total, 15 selected trace elements (Mg, Al, K, V, Mn, Fe, Cu, Zn, As, Mo, Ag, Cd, Ba, Tl, and Pb) in aerosol samples were determined using inductively coupled plasma mass spectrometry (ICPMS). The major metals in these two mountain sites were Fe, K, Mg, and Ca with concentrations ranging between 241 and 1452 ng/m3, 428 and 1351 ng/m3, 334 and 875 ng/m3, and 376 and 870 ng/m3, respectively, while the trace metals with the lowest concentrations were Mo, Ag, Cd, and Tl with concentrations lower than 4 ng/m3 in DHS and 2 ng/m3 in GGS. The pronounced seasonal variability in the trace elements was observed in DHS, with lower concentrations in spring and summer and relatively high in winter and autumn, whereas seasonal variance of trace elements is hardly observed in Mt. Gongga. The size distribution pattern of crustal elements of Al, Mg, K, Ba, and Fe was quite similar in DHS and GGS, which were mainly found in coarse particles peaked at 4.7–5.8 μm. In addition, V, Mo, Ag, and Tl were also concentrated in coarse particles, although the high enrichment factor (EF?>?100) of which suggested anthropogenic origin, whereas trace metals of Cd, Mn, Zn, As, Cu, and Pb concentrated in fine mode particles. Specifically, these trace metals peak at approximately 1.5 μm in DHS, while those in GGS peaked at diameter smaller than 0.3 μm, indicating the responsible for long-range transport from the far urban and industrialized areas. Multivariate receptor model combined with the enrichment factor results demonstrated that the trace elemental components at these two background sites were largely contributed from the fossil fuel combustion (55.4% in DHS and 44.0% in GGS) and industrial emissions factors (20.1% vs. 26.5%), which are associated with long distance transport from the coastal area of Southeast China and the Northwestern India, respectively, as suggested by the backward air mass trajectory analysis. Local sources from soil dust contributed a minor variance for trace elements in DHS (9.7%) and GGS (13.8%), respectively.
In order to evaluate the composition of inhalable atmospheric particles and to study the relationship between trace element levels in PM10 and in leaves of two plant species, the amount of Ba, Cu, Fe, Mn, Pb, Ti and V were analysed in PM10 and in Nerium oleander L. and Lantana camara L. leaves from two sites in the city of Seville and one remote control site. In PM10, the Cu and Fe content was significantly lower (p<0.05) in the control site than in the other sites. No correlations between leaf content and air content were found for the elements in L. camara. On the contrary, positive and significant correlations (p<0.05) were found between leaf content of N. oleander and PM10 content for Cu and Fe. The data suggest that N. oleander can be used in atmospheric biomonitoring studies, because it is especially useful for Cu and Fe, N. oleander being a better indicator than L. camara. 相似文献
Characteristics of atmospheric aerosols in Kyoto, Japan and Seoul, Korea were investigated using particle-induced X-ray emission (PIXE), elemental analysis system (EAS) and ion chromatograph (IC). Atmospheric aerosols were collected into fine and coarse fractions using a two-stage filter pack sampler in Kyoto and Seoul in winter of 1998. PIXE was applied to analyze the middle and heavy elements with atomic number greater than 14 (Si), and EAS was applied to analyze the light elements such as H, C and N. The total mass concentration in Seoul was about two times higher than in Kyoto and the concentration of Ca, Si, and Ti that are mainly originated from soil were remarkably higher in Seoul. During an Asian dust storm event, the concentration of soil components increased dramatically and amounted to about 15 times higher than average concentration. The fine/coarse ratios of NH4+, NO3−, and SO42− were extremely high in both sites. The fact that nearly 70% of fine particles in both Kyoto and Seoul consist of the light elements (N, C, and H) suggests the importance of light elements measurement. Good mass closure for fine particles with light element data was achieved. 相似文献
The influence of PAH chemical structure and concentration, added in either single (75 or 300 mg kg−1) or multiple (2 × 75, 2 × 150 or 4 × 75 mg kg−1) applications as single- or multiple-contaminant systems, on the development of PAH biodegradation in a pristine soil was investigated. Development in microbial catabolic ability was assessed at 0, 28, 56 and 84 d by monitoring 14C-naphthalene, 14C-phenanthrene and 14C-pyrene mineralisation over 14 d in respirometric assays. The presence of other contaminants influenced the ability of the indigenous microflora to mineralise structurally different contaminants over time. 14C-Naphthalene mineralisation was inhibited by the presence of other contaminants; whereas the presence of naphthalene significantly enhanced rates of mineralisation in multiple-contaminant systems containing 14C-phenanthrene and 14C-pyrene. Generally, increasing the number of contaminant applications has implications for catabolic activity of soil microbes. It is suggested the toxic nature of PAHs retarded mineralisation at increased contaminant concentrations. 相似文献