南京大气细粒子中重金属污染特征及来源解析简

利用2011年1月、4月、7月和10月在南京市区和北郊采集的气溶胶样品，研究了南京大气细粒子中Zn、Pb、Hg、As和Cd 5种重金属的污染水平，通过元素相关性分析和因子分析方法，对细粒子中这些重金属的污染来源进行了初步解析。结果表明，南京大气细粒子及其重金属污染严重，北郊普遍比市区严重；As严重超标，Cd在南京北郊超标约5倍，Zn在市区与北郊的质量浓度均高于其他重金属元素。每种重金属的浓度均随季节而变化。市区细粒子中，As和Zn可能主要与燃煤、轮胎灰尘和建筑扬尘等有关，Pb、Hg和Cd主要来自交通尘、城市垃圾焚烧等。北郊细粒子中，As、Hg和Zn主要来源于燃煤、钢铁冶炼等工业，Pb和Cd主要与农作物秸秆燃烧、汽车尾气、道路扬尘等影响有关。     

南京大气细粒子中重金属污染特征及来源解析

利用2011年1月、4月、7月和10月在南京市区和北郊采集的气溶胶样品，研究了南京大气细粒子中zn、Ph、Hg、As和cd5种重金属的污染水平，通过元素相关性分析和因子分析方法，对细粒子中这些重金属的污染来源进行了初步解析。结果表明，南京大气细粒子及其重金属污染严重，北郊普遍比市区严重；As严重超标，cd在南京北郊超标约5倍，zn在市区与北郊的质量浓度均高于其他重金属元素。每种重金属的浓度均随季节而变化。市区细粒子中，As和zn可能主要与燃煤、轮胎灰尘和建筑扬尘等有关，Pb、Hg和cd主要来自交通尘、城市垃圾焚烧等。北郊细粒子中，As、Hg和zn主要来源于燃煤、钢铁冶炼等工业，Pb和cd主要与农作物秸秆燃烧、汽车尾气、道路扬尘等影响有关。     

Dissolution and solubility of trace metals from natural and anthropogenic aerosol particulate matter

An open flow reactor is used to simulate the dissolution process of mineral aerosol particles in atmospheric water droplets. Data on dissolution kinetic and solubility are provided for the major trace metals from two kinds of matrix: alumino-silicated and carbonaceous sample. The results emphasise that the metals contained in the carbonaceous aerosols are easier dissolved than in the alumino-silicated particles. The released concentrations are not related to the total metal composition or the origin of particles, but are directly associated with the type of liaisons whereby the metals are bound in the solid matrix. Thus, the metals coming from carbonaceous particles are adsorbed impurities or salts and hence are very soluble and with a dissolution hardly dependent on pH, whereas the metals dissolved from alumino-silicated particles are less soluble, notably the ones constitutive of the matrix network (Fe, Mn), and with a dissolution highly influenced by pH. Consequently, in the regions with an anthropogenic influence, the dissolved concentrations of metals found in the atmospheric waters are mainly governed by the elemental carbon content. Moreover, it appears that the dissolution kinetic of metals is not constant as a function of time. The dissolution rates are very rapid in the first 20 min of leaching and then they are stabilised to lower values in comparison to initial rates. By consequence, the total dissolved metal content is provided after the first 20 min of the droplet lifetime. For this reason, the effects of trace metals on the atmospheric aqueous chemistry and as atmospheric wet input to the marine biota are maximal for "aged" droplets.     

The spatial and temporal characteristics of TOMS AI over the Tarim Basin,China

This paper has a dual focus. One is to study the spatial characteristics of dust activities over the Tarim Basin by locating dust active hot spots. The other is to study the temporal characteristics of dust activities over the Tarim Basin by applying the Extreme Value Analysis (EVA).Hot spots (in terms of dust loading) refer to relatively small (compared to the size of the whole source area), consistently active, dust producing areas. In this paper, Total Ozone Mapping Spectrometer (TOMS) Aerosol Index (AI) is used to identify hot spots in the Tarim Basin. This hot spot study suggests that dust emissions are inhomogeneous in the Tarim Basin area and the formation of the two hot spots is linked to both (1) a large amount of fine sandy sediments accumulated at the hot spot areas and (2) the basin's internal dust transport pathways which are controlled by the extreme bounding topography of the basin.Extreme Value Analysis (EVA) has been widely used in a variety of areas, but has not yet been applied in dust storm research. In this paper, 13 years Tarim Basin regional daily maximum TOMS AI data time series are constructed. By examining the statistics of the time series, a new method (outlier method) is developed to identify extreme values. EVA is applied and 100-year-return values are suggested. The interpretation of the 100-year-return values is discussed by referring to historical meteorological records and also climate change projections.     

Potentially toxic metal contamination of urban soils and roadside dust in Shanghai, China

A detailed investigation was conducted to understand the contamination characteristics of a selected set of potentially toxic metals in Shanghai. The amount of Pb, Zn, Cu, Cr, Cd and Ni were determined from 273 soil/dust samples collected within urban area. The results indicated that concentration of all metals except Ni in soils was significant, and metal pollution was even severer in roadside dust. A series of metal spatial distribution maps were created through geostatistical analysis, and the pollution hotspots tended to associate with city core area, major road junctions, and the regions close to industrial zones. In attempt of identifying the source of metals through geostatistical and multivariate statistical analyses, it was concluded as follows: Pb, Zn and Cu mainly originated from traffic contaminants; soil Ni was associated with natural concentration; Cd largely came from point-sourced industrial pollution; and Cr, Ni in dust were mainly related to atmospheric deposition.     

Variation of the mixing state of Saharan dust particles with atmospheric transport

Mineral dust is an important aerosol species in the Earth’s atmosphere and has a major source within North Africa, of which the Sahara forms the major part. Aerosol Time of Flight Mass Spectrometry (ATOFMS) is first used to determine the mixing state of dust particles collected from the land surface in the Saharan region, showing low abundance of species such as nitrate and sulphate internally mixed with the dust mineral matrix. These data are then compared with the ATOFMS single particle mass spectra of Saharan dust particles detected in the marine atmosphere in the vicinity of the Cape Verde islands, which are further compared with those from particles with longer atmospheric residence sampled at a coastal station at Mace Head, Ireland. Saharan dust particles collected near the Cape Verde Islands showed increased internally mixed nitrate but no sulphate, whilst Saharan dust particles collected on the coast of Ireland showed a very high degree of internally mixed secondary species including nitrate, sulphate and methanesulphonate. This uptake of secondary species will change the pH and hygroscopic properties of the aerosol dust and thus can influence the budgets of other reactive gases, as well as influencing the radiative properties of the particles and the availability of metals for dissolution.     

Size distribution and diurnal characteristics of particle-bound metals in source and receptor sites of the Los Angeles Basin

Measurement of daily size-fractionated ambient PM₁₀ mass, metals, inorganic ions (nitrate and sulfate) and elemental and organic carbon were conducted at source (Downey) and receptor (Riverside) sites within the Los Angeles Basin. In addition to 24-h concentration measurements, the diurnal patterns of the trace element and metal content of fine (0–2.5 μm) and coarse (2.5–10 μm) PM were studied by determining coarse and fine PM metal concentrations during four time intervals of the day.The main source of crustal metals (e.g., Al, Si, K, Ca, Fe and Ti) can be attributed to the re-suspension of dust at both source and receptor sites. All the crustals are predominantly present in supermicron particles. At Downey, potentially toxic metals (e.g., Pb, Sn, Ni, Cr, V, and Ba) are predominantly partitioned (70–85%, by mass) in the submicron particles. Pb, Sn and Ba have been traced to vehicular emissions from nearby freeways, whereas Ni and Cr have been attributed to emissions from powerplants and oil refineries upwind in Long Beach. Riverside, adjacent to Southern California deserts, exhibits coarser distributions for almost all particle-bound metals as compared to Downey. Fine PM metal concentrations in Riverside seem to be a combination of few local emissions and those transported from urban Los Angeles. The majority of metals associated with fine particles are in much lower concentrations at Riverside compared to Downey. Diurnal patterns of metals are different in coarse and fine PM modes in each location. Coarse PM metal concentration trends are governed by variations in the wind speeds in each location, whereas the diurnal trends in the fine PM metal concentrations are found to be a function both of the prevailing meteorological conditions and their upwind sources.     

Chemical characterization and source identification/apportionment of fine and coarse air particles in Thessaloniki,Greece

The distribution of air particulate mass and selected particle components (trace elements and polycyclic aromatic hydrocarbons (PAHs)) in the fine and the coarse size fractions was investigated at a traffic-impacted urban site in Thessaloniki, Greece. 76±6% on average of the total ambient aerosol mass was distributed in the fine size fraction. Fine-sized trace elemental fractions ranged between 51% for Fe and 95% for Zn, while those of PAHs were between 95% and 99%. A significant seasonal effect was observed for the size distribution of aerosol mass, with a shift to larger fine fractions in winter. Similar seasonal trend was exhibited by PAHs, whereas larger fine fractions in summer were shown by trace elements. The compositional signatures of fine and coarse particle fractions were compared to that of local paved-road dust. A strong correlation was found between coarse particles and road dust suggesting strong contribution of resuspended road dust to the coarse particles. A multivariate receptor model (multiple regression on absolute principal component scores) was applied on separate fine and coarse aerosol data for source identification and apportionment. Results demonstrated that the largest contribution to fine-sized aerosol is traffic (38%) followed by road dust (28%), while road dust clearly dominated the coarse size fraction (57%).     

Characterization of the winter atmospheric aerosols in Kyoto and Seoul using PIXE,EAS and IC

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.     

Metal content in street dust as a reflection of atmospheric dust emissions from coal power plants, metal smelters, and traffic

Resuspended street dust is a source of inhalable particles in urban environments. Despite contaminated street dust being a possible health risk factor for local population, little is known about the contribution of atmospheric dust emissions and other factors to the content of toxic metals in street dust. The impact of smelting, traffic, and power plants on metal contaminates in street dust is the focus of street dust sampling at 46 locations in the Witbank area (Republic of South Africa). This area is characterized by numerous open-pit coal mines in the Karoo coal basin, which provides a cheap source of energy to numerous metallurgical smelters and ironworks and supplies coal to the coal-fired power plants located nearby. Street dust was collected on asphalt or concrete surfaces with hard plastic brushes, avoiding collecting of possible sand, soil, or plant particles. Chemical analysis was done on the <0.125 mm fraction using inductively coupled plasma mass spectrometry subsequent to total digestion. Exceptionally high concentrations of metals were detected with concentrations of Fe reaching 17.7 %, Cr 4.3 %, Mn 2 %, Ni 366 mg/kg, and V 4,410 mg/kg. Factor analysis indicates three sources for the pollution. Road traffic which contributes to the high concentrations of Cu, Pb, Sb, and Sn, with the highest impacts detected in the town of Witbank. The second source is associated with the metal smelting industry, contributing to Fe, Co, Mn, and V emissions. The highest factor scores were observed around four metallurgical smelter operations, located in the Ferrobank, Highveld, and Clewer industrial areas. Impact of vanadium smelter to street dust composition could still be detected some 20 km away from the sources. Exceptionally high concentrations of Cr were observed in four samples collected next to the Ferrobank industrial area, despite Cr not being loaded in factor 2. The last source of the pollution is most probably fly ash associated with the coal-fired power plants and fly ash dumps. Elements which are associated with this source are Al, Sr, and Li. This factor is abundant in the coal mining part of the study area.     

Source-to-receptor pathways of anthropogenic PM2.5 in Detroit,Michigan: Comparison of two inhalation exposure studies

Recent studies have attributed toxic effects of ambient fine particulate matter (aerodynamic diameter ≤ 2.5 μm; PM_2.5) to physical and/or chemical properties rather than total mass. However, identifying specific components or sources of a complex mixture of ambient PM_2.5 that are responsible for adverse health effects is still challenging. In order to improve our understanding of source-to-receptor pathways for ambient PM_2.5 (links between sources of ambient PM_2.5 and measures of biologically relevant dose), integrated inhalation toxicology studies using animal models and concentrated air particles (CAPs) were completed in southwest Detroit, a community where the pediatric asthma rate is more than twice the national average. Ambient PM_2.5 was concentrated with a Harvard fine particle concentrator housed in AirCARE1, a mobile air research laboratory which facilitates inhalation exposure studies in real-world settings. Detailed characterizations of ambient PM_2.5 and CAPs, identification of major emission sources of PM_2.5, and quantification of trace elements in the lung tissues of laboratory rats that were exposed to CAPs for two distinct 3-day exposure periods were completed.This paper describes the physical/chemical properties and sources of PM_2.5, pulmonary metal concentrations and meteorology from two different 3-day exposure periods—both conducted at the southwest Detroit location in July 2003—which resulted in disparate biological effects. More specifically, during one of the exposure periods, ambient PM_2.5-derived trace metals were recovered from lung tissues of CAPs-exposed animals, and these metals were linked to local combustion point sources in southwest Detroit via receptor modeling and meteorology; whereas in the other exposure period, no such trace metals were observed. By comparing these two disparate results, this investigation was able to define possible links between PM_2.5 emitted from refineries and incinerators and biologically relevant dose, which in turn may be associated with observed health effects.     

Using PM10 geochemical maps for defining the origin of atmospheric pollution in Andalusia (Southern Spain)

In this work we present a detailed study of atmospheric PM₁₀ pollution in Andalusia (Southern Spain) based on geochemical maps. The study includes determination of PM₁₀ levels and bulk chemical composition with samples from 17 representative monitoring stations (rural, urban background, traffic hot spot, and urban zones with industrial influence) during 2007. The knowledge of background levels and concentrations of relevant chemical compounds and elements allows the quantification of the main sources of pollution in relevant cities and sites of ecological interest.In comparison to other stations in Spain and mainland Europe, PM₁₀ in Andalusia is characterized by high levels of crustal matter and secondary inorganic components (SIC). This has been attributed to the following causes: 1) High road traffic and industrial emissions, 2) High frequency of North African air mass outbreaks contributing between 3 and 4 μg m^?3 in western Andalusia and 4–7 μg m^?3 in eastern Andalusia, and 3) Climate factors such as low rainfall, dry soils favouring resuspension, and high photochemical activity.Atmospheric particulate matter in urban areas located in the vicinity of industrial estates is enriched in secondary inorganic compounds and metals. Three main hot spots have been identified according their high trace element concentrations: Huelva (As, Cu, Zn, Se, and Bi), Strait of Gibraltar (V, Ni, Cr, and Co) and Bailén (V and Ni). The transport of pollutants from cities and industrial estates to areas of ecological interest (e.g. Doñana National Park) has been found to cause the increase in background levels in a number of trace elements (e.g. As) in the air. An important outcome of this study is that geochemical maps of atmospheric matter are a powerful tool for illustrating spatial variation patterns of geochemical components and identifying specific pollution hot spots.     

Long-range transport of polycyclic aromatic hydrocarbons (PAHs) from the eastern Asian continent to Kanazawa,Japan with Asian dust

Aerosol particles were collected for 1 year, starting in April 2003, in rural areas of Kanazawa, Ishikawa, Japan to understand the role of Asian dust as a long-range transporter of polycyclic aromatic hydrocarbons (PAHs). Three sampling intervals were designated in this study, namely: (1) Dust period 1 (March 11–19, 2003); (2) Dust period 2 (March 28, 2003–April 9, 2003); and (3) Dust period 3 (April 9, 2004–April 25, 2004). The Asian dust particles are predominantly in the coarse particle size range (2.1–11 μm). PAH analyses were performed separately on both the coarse and fine (<1.1 μm) particle ranges. Seasonal trends in PAH concentrations for coarse and fine particles showed that the Asian dust particles in Dust period 3 contained significant amounts of less-volatile PAHs such as benzo[a]pyrene (BaP) and benzo[g,h,i]perylene (BghiP). A kinetic model developed in this study shows that almost none of these PAHs would be accumulated on Asian dust particles in the atmosphere, due to their extremely slow adsorption rates. These PAHs would have to originate from PAH-polluted soil particles around industrialized areas. Back trajectory analyses suggest that the Asian dust in Dust period 3 came from loess regions around industrialized areas. This indicates that geologic materials play a significant role in the atmospheric circulation of PAHs.     

Land Use-related Chemical Composition of Street Sediments in Beijing

BACKGROUND: More than 10 million people are currently living in Beijing. This city faces severe anthropogenic air pollution caused by an intense vehicle increase (11% per year in China), coal combusting power plants, heavy industry, huge numbers of household and restaurant cookers, and domestic heating stoves. Additionally, each year dust storms are carrying particulate matter from the deserts of Gobi and Takla Makan towards Beijing, especially in spring. Other geogenic sources of particulate matter which contribute to the air pollution are bare soils, coal heaps and construction sites occurring in and around Beijing. Streets function as receptor surfaces for atmospheric dusts. Thus, street sediments consist of particles of different chemical compositions from many different sources, such as traffic, road side soils and industry. METHODS: Distributions and concentrations of various chemical elements in street sediments were investigated along a rural-urban transect in Beijing, China. Chemical elements were determined with X-ray fluorescence analysis. Factor analysis was used to extract most important element sources contributing to particulate pollution along a main arterial route of the Chinese capital. RESULTS AND DISCUSSION: The statistical evaluation of the data by factor analysis identifies three main anthropogenic sources responsible for the contamination of Beijing street sediments. The first source is a steel factory in the western part of Beijing. From this source, Mn, Fe, and Ti were emitted into the atmosphere through chimneys and by wind from coal heaps used as the primary energy source for the factory. The second source is a combination of traffic, domestic heating and some small factories in the center of Beijing discharging Cu, Pb, Zn and Sn. Calcium and Cr characterize a third anthropogenic element source of construction materials such as concrete and mortar. Beside the anthropogenic contamination, some elements like Y, Zr, Nb, Ce, and Rb are mainly derived from natural soils and from the deserts. This is supported by mineral phase analysis, which showed a clear imprint of material in road dusts coming from the West-China deserts. CONCLUSIONS: Our results clearly show that the chemical composition of urban road dusts can be used to identify distinct sources responsible for their contamination. The study demonstrates that the chemistry of road dusts is an important monitor to assess the contamination in the urban environment. Chemical composition of street sediments in Beijing comprises the information of different sources of atmospheric particles. RECOMMENDATIONS AND OUTLOOK: This study is only a small contribution to the understanding of substance fluxes related to Beijing's dust. More effort is required to assess Beijing's dust fluxes, since the dust harms the living quality of the inhabitants. Especially the measurable superimposing of long scale transported dust from dry regions with the anthropogenic polluted urban dust makes investigations of Beijing's dust scientifically valuable.     

Identification of particles containing chromium and lead in road dust and soakaway sediment by electron probe microanalyser

Individual particles containing Cr and/or Pb and other major components were identified in road dust from a heavily used road (hereinafter 'heavy traffic road dust'), road dust from a residential area and soakaway sediment by electron probe microanalyser to locate their sources and carrier particles. Individual particles containing high levels of Cr and/or Pb (>or=0.2%) were identified using wavelength dispersive spectrometry (WDS) map analysis. Chromium, Pb and other major elements were then determined by means of a combination of WDS and energy-dispersive spectrometry in all identified particles, 50 particles containing neither Cr nor Pb from each type of road dust and soakaway sediment, and yellow road line markings. WDS map analysis revealed that many particles containing both Cr and Pb were present among the identified particles in heavy traffic road dust, whereas they were minor components in road dust from the residential area and soakaway sediment. The plots of X-ray intensities of Cr vs. Pb were linear for the identified particles containing both Cr and Pb in heavy traffic road dust, and the line closely fitted the plots for the three yellow road line marking samples. Individual particles were then classified using cluster analysis of element components. The results revealed that the adsorption of source materials or released metals onto soil minerals occurred in road dust and soakaway sediment, that the yellow road line markings were sources of Cr and Pb in heavy traffic road dust, and that materials containing Fe as a major component, such as stainless steel, were additional sources of Cr in both road dust and soakaway sediment.     

Considering the functional value of common marine species as a conservation stake: the case of sandmason worm Lanice conchilega (Pallas 1766) (Annelida, Polychaeta) beds

Conservation of the marine environment mainly focuses on threatened elements and more precisely on vulnerable and endangered species like birds and mammals. When dealing with the conservation of marine habitats, the scientific community is mainly interested in hot spots of diversity, like seagrass beds in Europe, or hot spots of endemism, like coral reefs in tropical areas. Nevertheless, using the example of a common and widespread marine invertebrate, the sandmason worm (Lanice conchilega, Polychaeta, Terebellidae), we show that vulnerability and rarity are not the only criteria to take into account in order to select the best natural element for conservation. This species can form dense beds that increase biodiversity, are attractive feeding grounds for birds and fishes, and have a high socioeconomic value. In consequence, they have a high functional value that should be considered as an important conservation stake. Through the example of the Chausey archipelago and the Bay of the Mont Saint-Michel (France), we propose a synthetic interdisciplinary approach to evaluate the conservation needs of these beds. The issue is even more pressing when one considers that these natural elements and many similar ones still do not benefit from any legal protection in Europe despite their high heritage value.     

Differentiation of the contribution of local resuspension from that of regional and remote sources on trace elements content in the atmospheric aerosol in the Mediterranean area

For the determination of effects of contaminated crude soil on the content of trace elements in the atmospheric aerosol, trace elements in crude soil samples from within the area of influence of local resuspension were analysed. The obtained results were used for determining the contribution of local resuspension on contents of trace elements in the atmospheric aerosol using the enrichment factors (EF) method. The content of trace elements in a crude soil could arise from the geochemical background of the soil or from anthropogenic contributions. Analysis of the quantile showed that Cd, Se and Ni originate from local emission sources. PCA showed that four groups of sources contributed to the content of trace elements in PM in part of the receptor. Using EF, it was ascertained that local resuspension of crude soil particles had a dominant influence on the content of Fe, Mn and Ti in the atmospheric aerosol, and that local resuspension had no influence on the content of Se in the atmospheric aerosol. Dust originating from deserts of North Africa and Middle East, through long-range transport and through resuspension of settled dust particles, significantly contributes to the content of Fe, Mn and Ti in the atmospheric aerosol. Cd originated from contaminated crude soil. The other investigated elements originated partly from crude soil but also from some other emission sources in the region.     

Seasonal variations in the chemical composition of particulate matter: a case study in the Po Valley. Part II: concentration and solubility of micro- and trace-elements

Size distribution (fine and coarse fraction) and solubility distribution (extracted and residual fraction) of 20 elements (As, Ba, Be, Cd, Co, Cu, Fe, Li, Mn, Pb, Ni, Rb, S, Sb, Se, Sn, Sr, Ti, Tl, V) in atmospheric particulate matter (PM) were determined during a 5-year field study carried out in the Po Valley (peri-urban area of Ferrara, in Northern Italy). By studying the contribution of the two size fractions and the two solubility fractions to the atmospheric concentration of each element, it was possible to obtain interesting information about the variability of PM sources, to assess the role played by atmospheric stability in determining pollution episodes, and to obtain an estimate of the bio-accessible fraction. Atmospheric stability is confirmed to be one of the main causes of atmospheric pollution in this area and is to be responsible for the pronounced winter increase in both PM and elemental concentration. Long-range transport of natural and polluted air masses caused temporary increases in PM and elemental concentration, while local industrial emission seemed to play a secondary role. Regulated elements were well below their concentration limit, but many toxic elements were in the form of fine particles and soluble chemical species, more accessible to the environment, and the human body.     

Concentration, size distribution, and dry deposition rate of particle-associated metals in the Los Angeles region

Daily averaged atmospheric concentrations and dry deposition fluxes of particulate metals were measured seasonally at six urban sites and one non-urban coastal site in the Los Angeles region using a conventional total suspended particulate matter (TSP) filter, surrogate surface deposition plates, and a Noll Rotary Impactor (NRI), which provides information about particle size distribution in four size ranges above 6 μm. With the exception of the non-urban site, particulate metal concentrations and deposition fluxes were remarkably uniform spatially and temporally. At all sites there were significant metal concentrations on particles greater than 10 μm, a commonly used upper limit for many air quality monitoring studies, and these large particles were estimated to be responsible for most of the deposited mass of metals. Annual averaged values of deposition rates measured with a surrogate surface were in good agreement with values estimated using theoretical deposition velocities in conjunction with measured size-segregated particle concentrations. Image analysis of particles deposited on NRI stage A, which collects all particles greater than 6 μm, indicated nighttime metal concentrations and deposition at the non-urban coastal site was higher than in the day time due to offshore advection of urban air associated with the diurnal land breeze. Measured enrichments of crustal elements and metals were correlated, indicating efficient mixing of natural and anthropogenic material from different sources, hypothesized to be the result of cyclical resuspension and deposition of dust by moving vehicles and wind.     

Changes in the atmospheric deposition of minor and rare elements between 1975 and 2000 in south Sweden, as measured by moss analysis

Elements emitted to the atmosphere are partly exported to more remote areas and contribute to the regional and territorial deposition rates. This study is based on the principle that carpet-forming bryophytes (pleurocarpic mosses) absorb elements and particles from rain, melting snow and dry deposition. We compare the concentrations of 60 elements in carpets of the forest moss Pleurozium schreberi sampled in 1975 and 2000 within a sparsely inhabited area dominated by forest and bogland in south Sweden. As an average for all the 60 elements, the median concentration was 2.7 times higher in 1975 than in 2000. The greatest difference was measured for Pb, although In, Bi, Ge, V, Sn, As and Ag had more than 5 times higher concentrations in 1975 than in 2000. Somewhat lower 1975/2000 concentration ratios (3.0-3.8) were measured for U, Sb, Cd, W, Ga, Fe, Li, and Be. The rare-earth elements (Y, La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu), except Eu as well as Th, Ni, Al, Ti, Hf, Nb, and Zr, had concentration ratios around the average (2.5-2.8). Possible causes of these changes are discussed. We conclude that reductions in anthropogenic dust emissions during recent decades have decreased the atmospheric deposition over northern Europe of most elements in the periodical system, as previously reported for a limited number of transition and heavy metals. Changes in the deposition of soil dust would be of minor importance to the decreased deposition rates.