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1.
An arsenic speciation study has been performed in PM10 samples collected on a fortnight basis in the city of Huelva (SW Spain) during 2001 and 2002. The arsenic species were extracted from the PM10 filters using a NH2OH x HCl solution and sonication, and determined by HPLC-HG-AFS. The mean bulk As concentration of the samples analyzed during 2001 and 2002 slightly exceed the mean annual 6 ng m(-3) target value proposed by the European Commission for 2013, arsenate [As(V)] being responsible for the high level of arsenic. The speciation analyses showed that As(V) was the main arsenic species found, followed by arsenite [As(III)] (mean 6.5 and 7.8 ng m(-3) for As(V), mean 1.2 and 2.1 ng m(-3) for As(III), in 2001 and 2002, respectively). The high levels of arsenic species found in PM10 in Huelva have a predominant industrial origin, such as the one from a nearby copper smelter, and do not present a seasonal pattern. The highest daily levels of arsenic species correspond to synoptic conditions in which the winds with S and SW components transport the contaminants from the main emission source. The frequent African dust outbreaks over Huelva may result in an increment of mass levels of PM10, but do not represent a significant input of arsenic in comparison to the anthropogenic source. The rural background levels of arsenic around Huelva are rather high, in comparison to other rural or urban areas in Spain, showing a relatively high atmosphere residence time of arsenic. This work shows the importance of arsenic speciation in studies of aerosol chemistry, due to the presence of arsenic species [As(III) and As(V)] with distinct toxicity.  相似文献   

2.
Daily fine particulate matter (PM2.5) samples were collected at Gwangju, Korea, during the Aerosol Characterization Experiments (ACE)-Asia Project to determine the chemical properties of PM2.5 originating from local pollution and Asian dust (AD) storms. During the study period, two significant events occurred on April 10-13 and 24-25, 2001, and a minor event occurred on April 19, 2001. Based on air mass transport pathways identified by back-trajectory calculation, the PM2.5 dataset was classified into three types of aerosol populations: local pollution and two AD aerosol types. The two AD types were transported along different pathways. One originated from Gobi desert area in Mongolia, passing through Hunshandake desert in Northern Inner Mongolia, urban and polluted regions of China (AD1), and the other originated in sandy deserts located in the Northeast Inner Mongolia Plateau and then flowed southward through the Korean peninsula (AD2). During the AD2 event, a smoke plume that originated in North Korea was transported to our study site. Mass balance closures show that crustal materials were the most significant species during both AD events, contributing -48% to the PM2.5 mass; sulfate aerosols (19.1%) and organic matter (OM; 24.6%) were the second greatest contributors during the AD1 and AD2 periods, respectively, indicating that aerosol properties were dependent on the transport pathway. The sulfate concentration constituted only 6.4% (4.5 microg/m3) of the AD2 PM2.5 mass. OM was the major chemical species in the local pollution-dominated PM2.5 aerosols, accounting for 28.7% of the measured PM2.5 mass, followed by sulfate (21.4%), nitrate (15%), ammonium (12.8%), elemental carbon (8.9%), and crustal material (6.5%). Together with substantial enhancement of the crustal elements (Mg, Al, K, Ca, Sc, Ti, Mn, Fe, Sr, Zr, Ba, and Ce), higher concentrations of pollution elements (S, V, Ni, Zn, As, Cd, and Pb) were observed during AD1 and AD2 than during the local pollution period, indicating that, in addition to crustal material, the AD dust storms also had a significant influence on anthropogenic elements.  相似文献   

3.
The concentrations of monosaccharide anhydrides (levoglucosan, mannosan, galactosan) in PM1 and PM2.5 aerosol samples were measured in Brno and ?lapanice in the Czech Republic in winter and summer 2009. 56 aerosol samples were collected together at both sites to investigate the different sources that contribute to aerosol composition in studied localities. Daily PM1 and PM2.5 aerosol samples were collected on pre-fired quartz fibre filters.The sum of average atmospheric concentration of levoglucosan, mannosan and galactosan in PM1 aerosol in ?lapanice and Brno during winter was 513 and 273 ng m?3, while in summer the sum of average atmospheric concentration of monosaccharide anhydrides (MAs) was 42 and 38 ng m?3, respectively. The sum of average atmospheric concentration of MAs in PM1 aerosol formed 71 and 63% of the sum of MA concentration in PM2.5 aerosol collected in winter in ?lapanice and Brno, whereas in summer the sum of average atmospheric concentration of MAs in PM1 aerosol formed 45 and 43% of the sum of MA concentration in PM2.5 aerosol in ?lapanice and Brno, respectively.In winter, the sum of MAs contributed significantly to PM1 mass ranging between 1.37% and 2.67% of PM1 mass (Brno – ?lapanice), while in summer the contribution of the sum of MAs was smaller (0.28–0.32%). Contribution of the sum of MAs to PM2.5 mass is similar both in winter (1.37–2.71%) and summer (0.44–0.55%).The higher concentrations of monosaccharide anhydrides in aerosols in ?lapanice indicate higher biomass combustion in this location than in Brno during winter season. The comparison of levoglucosan concentration in PM1 and PM2.5 aerosol shows prevailing presence of levoglucosan in PM1 aerosol both in winter (72% on average) and summer (60% on average).The aerosol samples collected in ?lapanice and Brno in winter and summer show comparable contributions of levoglucosan, mannosan and galactosan to the total amount of monosaccharide anhydrides in both aerosol size fractions. Levoglucosan was the most abundant monosaccharide anhydride with a relative average contribution to the total amount of MAs in the range of 71–82% for PM1 aerosols and 52–79% for PM2.5 aerosols.  相似文献   

4.
The tests of standard mixtures and four sets of atmospheric particulate samples showed that an acid-wash (AW) pretreatment of fluorocarbon-coated glass fiber filters prior to aerosol sampling enhanced the quantifiable organic compounds for more than 29% (or 66 ng m−3); in particular, 47–273 ng m−3 (21–366%) more water-soluble organic compounds (WSOCs) were measured. When the acid-pretreated filters were employed, up to nine more organic species were measured in the individual daily samples. Because the acid pretreatment reduced the metal contaminants in the glass fiber filters, using the AW filters for aerosol sampling allows higher extraction recoveries of organic compounds. Since the fingerprinting compounds were more accurately determined when the aerosol samples were collected on the AW filters, better assessment of emission sources and toxicity of air pollutants can be obtained.  相似文献   

5.
The Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS) has been previously verified as being capable of measuring total fine particulate matter (PM2.5), including semi-volatile species. The present study was conducted to determine if the simple modification of a commercial speciation sampler with a charcoal denuder followed by a filter pack containing a quartz filter and a charcoal-impregnated glass (CIG) fiber filter would allow for the measurement of total PM2.5, including semi-volatile organic material. Data were collected using an R&P (Rupprecht and Pastasnik Co., Inc.) Partisol Model 2300 speciation sampler; an R&P Partisol speciation sampler modified with a BOSS denuder, followed by a filter pack with a quartz and a CIG filter; a Met One spiral aerosol speciation sampler (SASS); and the PC-BOSS from November 2001 to March 2002 at a U.S. Environmental Protection Agency (EPA) Science to Achieve Results (STAR) sampling site in Lindon, UT. Total PM2.5 mass, ammonium nitrate (both nonvolatile and semi-volatile), ammonium sulfate, organic carbon (both non-volatile and semi-volatile), and elemental carbon were determined on a 24-hr basis. Results obtained with the individual samplers were compared to determine the capability of the modified R&P speciation sampler for measuring total PM2.5, including semi-volatile components. Data obtained with the modified speciation sampler agreed with the PC-BOSS results. Data obtained with the two unmodified speciation samplers were low by an average of 26% because of the loss of semi-volatile organic material from the quartz filter during sample collection.  相似文献   

6.
Experimental relationships between the mass concentration of suspended particulate matter and the optical density of particulates collected on paper tape have been determined for the atmospheric aerosol and for aerosols of constant optical properties. Simultaneous samples were obtained on membrane filters (for gravimetric analysis) and on Whatman No. 4 paper tape (for optical evaluation). Sampling procedures were adopted which ensured that the efficiency of sampling was the same in both cases.

Consistent relationships between mass concentrations of suspended particulate matter and optical density expressed in terms of per cent transmittance or per cent reflectance were found for dispersions of coal, limestone, fly ash, and a coal-limestone mixture.

For atmospheric aerosol samples collected on the roof of the Graduate School of Public Health, University of Pittsburgh, the relationship between mass concentration and per cent transmittance or per cent reflectance was found to be linear over the range of values observed. The correlation coefficients were ?0.93 (for concentration versus per cent transmittance) and ?0.89 (for concentration versus per cent reflectance).  相似文献   

7.
Samples of fine particulate organic matter were collected outside Durham, NC in the Duke Research Forest as part of the CELTIC study in July 2003. Particulate samples were collected on quartz filters using high volume air sampling equipment, and samples were analyzed for polar and non-polar organic species. Among compounds analyzed, oxidation products of α-pinene, namely pinic acid and pinonic acid, were identified in all samples. Pinic acid, being a dicarboxylic acid, has a low vapor pressure of the order of 10−8 Torr and is expected to contribute significantly to secondary organic aerosol (SOA) formation from the oxidation of α-pinene. Source contribution estimates from primary organic aerosol emissions were computed using the organic species as molecular markers with the chemical mass balance (CMB) model. The unapportioned organic carbon (OC) was determined as the difference between measured OC and OC apportioned to primary sources. This unapportioned OC was then correlated with pinic and pinonic acid to get a better understanding of the role of monoterpene oxidation products to form SOA. A reasonably good fit between pinic acid concentrations and unapportioned OC levels is indicative of the contribution of α-pinene oxidation products to SOA formation in ambient atmosphere. The results are significant considering the role of monoterpene emissions to global atmospheric chemistry.  相似文献   

8.
BACKGROUND: Arsenic speciation in environmental samples is essential for studying toxicity, mobility and bio-transformation of As in aquatic and terrestrial environments. Although the inorganic species As(III) and As(V) have been considered dominant in soils and sediments, organisms are able to metabolize inorganic forms of arsenic into organo-arsenic compounds. Arsenosugars and methylated As compounds can be found in terrestrial organisms, but they generally occur only as minor constituents. We investigated the dynamics of arsenic species under anaerobic conditions in soils surrounding gold mining areas from Minas Gerais State, Brazil to elucidate the arsenic biogeochemical cycle and water contamination mechanisms. METHODS: Surface soil samples were collected at those sites, namely Paracatu Formation, Banded Iron Formation and Riacho dos Machados Sequence, and incubated in CaCl2 2.5 mmol L(-1) suspensions under anaerobic conditions for 1, 28, 56 and 112 days. After that, suspensions were centrifuged and supernatants analyzed for soluble As species by IC-ICPMS and HPLC-ICPMS. RESULTS: Easily exchangeable As was mainly arsenite, except when reducible manganese was present. Arsenate was mainly responsible for the increase in soluble arsenic due to the reductive dissolution of either iron or manganese in samples from the Paracatu Formation and Riacho dos Machados Sequence. On the other hand, organic species of As dominated in samples from the Banded Iron Formation during anaerobic incubation. DISCUSSION: Results are contrary to the expectation that, in anaerobic environments, As release due to the reductive dissolution of Fe is followed by As(V) reduction to As(III). The occurrence of organo-arsenic species was also found to be significant to the dynamics of soluble arsenic, mainly in soils from the Banded Iron Formation (BIF), under our experimental conditions. CONCLUSIONS: In general, As(V) and organic As were the dominant species in solution, which is surprising under anaerobic conditions in terrestrial environments. The unexpected occurrence of organic species of As was attributed to enrollment of ternary organic complexes or living organisms such as algae or cyanobacteria. PERSPECTIVES: These findings are believed to be useful for remediation strategies in mine-affected regions, as the organic As species are in general considered to be less toxic than inorganic ones and even As(V) is considered less mobile and toxic than As(III).  相似文献   

9.
The determination of arsenic compounds in algae collected on the Catalan coast (Western Mediterranean) is reported. Ten algae species and the seagrass Posidonia oceanica were analyzed. Total arsenic in the samples was determined by microwave digestion and inductively coupled plasma mass spectrometry (ICPMS). Arsenic speciation in water extracts of samples was analyzed by liquid chromatography with both anionic and cationic exchange with ICPMS detection (LC-ICPMS). The total arsenic content of the algae samples ranged from 2.96 to 39.0mg As kg(-1). The following compounds were detected: arsenite (As(III)), arsenate (As(V)), methylarsonate (MA), dimethylarsinate (DMA), sulfonate sugar (SO3-sug), sulfate sugar (SO4-sug), phosphate sugar (PO4-sug), arsenobetaine (AB), arsenocholine (AC), trimethylarsine oxide (TMAO) and glycerol sugar (Gly-sug). The main arsenic species found were arsenosugars. Significant percentages of arsenobetaine (0.54 mg As kg(-1), 28% of the extractable arsenic and 0.39 mg As kg(-1), 18% of the extractable arsenic) were found in Ulva rigida and Enteromorpha compressa. These results are discussed in relation to the presence of epiphytes.  相似文献   

10.
The mass size distribution of atmospheric aerosol particles was determined by means of an electric low pressure impactor (ELPI) in rural air in Hungary. The particles captured on different stages of the impactor were chemically analyzed by capillary zone electrophoresis to quantify ionic components as well as by catalytic combustion method to detect total carbon in the samples. The results show that fine aerosol consists mainly of ammonium sulfate and organic carbon. These two species have rather different size distributions since very small particles are composed almost of carbon compounds. The analysis of fine aerosol samples collected simultaneously on filters indicates that an important part of organics is soluble in water. The mass balance of fine particles as a function of their size is estimated by taking into account the liquid water adsorbed by ammonium sulfate and by converting the mass of carbon to the mass of carbon compounds. Finally, the size resolved mass balance of fine aerosol particles is presented and discussed as a function of the origin of air masses.  相似文献   

11.
The Brigham Young University (BYU) organic sampling system (BOSS) and the high flow rate multi-system BYU organic sampling system (BIG BOSS), which use multichannel diffusion denuder sampling techniques, were both used to collect samples of atmospheric fine particulate organic material. Both systems were used at the Meadview sampling site located at the western boundary of the Grand Canyon National Park in northwestern Arizona for the Project MOHAVE summer intensive sampling program in August 1992. The concentrations of total fine particulate carbonaceous material determined by temperature programmed volatilization for BOSS collocated replicate samples were in agreement with an uncertainty of ±14%. A comparable agreement was seen between the BOSS and BIG BOSS samples. Carbonaceous material collected by the second of two sequential quartz filters was shown to have originated from organic material lost from particles during sampling. About one-half of the fine particulate organic material was lost from particles during sample collection. These semi-volatile organic compounds lost from particles during sampling were characterized by GC/MS analysis. The concentrations of n-alkanes, n-fatty acids, n-fatty methyl esters, and phthalic acid as a function of fine particulate size were obtained for compounds both retained by and lost from particles during sampling. The possible sources of fine particulate semi-volatile organic material collected at Meadview, and the particle size distribution of fine particulate organic material, n-alkanes, n-fatty acids, and n-fatty esters are discussed.  相似文献   

12.
Hydroxymethanesulfonate (HMS), a product of the heterogeneous reaction between S(IV) and HCHO, was measured in atmospheric aerosol samples collected at two locations indicating it can exist outside of clouds. Sampling was performed through collection with filters and analysis using ion chromatography with a treatment step to distinguish between HMS and uncomplexed S(IV). Concentrations of HMS were found to range from below the detection limit to 6.5 ng m-3 for samples collected in central New Mexico in the summer and around 30 ng m-3 for two samples collected in Seattle, Washington in the spring. Higher concentrations were associated with greater occurrence of clouds, which is the presumed source of the HMS. In the samples collected in Seattle, about half of the HMS was found associated with fine particles. In the central New Mexico samples, molar ratios of HMS to sulfate in particulate matter were found to be less than 0.002 indicating that HMS was a minor contributor of aerosol sulfur under the conditions of the measurements.  相似文献   

13.
The objectives of this study were to quantitatively estimate the distribution of arsenic with its speciation and to identify potential pathways for transformation of arsenic species from samples of water, sediments, and plants in the ecosystem affected by the Cheongog Spring, where As(V) concentration reached levels up to 0.270 mg L−1. After flowing about 100 m downstream, the arsenic level showed a marked reduction to 0.044 mg L−1 (about 84% removal) without noticeable changes in major water chemistry. The field study and laboratory hydroponic experiments with the dominant emergent plants along the creek (water dropwort and thunbergian smartweed) indicated that arsenic distribution, reduction, and speciation appear to be controlled by, (i) sorption onto stream sediments in exchangeable fractions, (ii) bioaccumulation by and possible release from emergent plants, and (iii) transformation of As(V) to As(III) and organic species through biological activities.  相似文献   

14.
An analysis of fine particulate data in eastern North Carolina was conducted to investigate the impact of the hog industry and its emissions of ammonia into the atmosphere. The fine particulate data are simulated using ISORROPIA, an equilibrium thermodynamic model that simulates the gas and aerosol equilibrium of inorganic atmospheric species. The observational data analyses show that the major constituents of fine particulate matter (PM2.5) are organic carbon, elemental carbon, sulfate, nitrate, and ammonium. The observed PM2.5 concentration is positively correlated with temperature but anticorrelated with wind speed. The correlation between PM2.5 and wind direction at some locations suggests an impact of ammonia emissions from hog facilities on PM2.5 formation. The modeled results are in good agreement with observations, with slightly better agreement at urban sites than at rural sites. The predicted total inorganic particulate matter (PM) concentrations are within 5% of the observed values under conditions with median initial total PM species concentrations, median relative humidity (RH), and median temperature. Ambient conditions with high PM precursor concentrations, low temperature, and high RH appear to favor the formation of secondary PM.  相似文献   

15.
Abstract

The hygroscopic properties of the organic fraction of aerosols are poorly understood. The ability of organic aerosols to absorb water as a function of relative humidity (RH) was examined using data collected during the 1999 Big Bend Regional Aerosol and Visibility Observational Study (BRAVO). (On average, organics accounted for 22% of fine particulate matter with an aerodynamic diameter less than 2.5 µm (PM2.5) mass). Hourly RH exceeded 80% only 3.5% of the time and averaged 44%. BRAVO aerosol chemical composition and dry particle size distributions were used to estimate PM2.5 light scattering (Bsp) at low and high ambient RH. Liquid water growth associated with inorganic species was sufficient to account for measured Bsp for RH between 70 and 95%.  相似文献   

16.
The Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study was conducted in Big Bend National Park, Texas, July through October 1999. Daily PM2.5 organic aerosol samples were collected on pre-fired quartz fiber filters. Daily concentrations were too low for detailed organic analysis by gas chromatography-mass spectrometry (GC-MS) and were grouped based on their air mass trajectories. A total of 12 composites, each containing 3–10 daily samples, were analyzed. Alkane carbon preference indices suggest primary biogenic emissions were small contributors to primary PM2.5 organic matter (OM) during the first 3 months, while in October air masses advecting from the north and south were more strongly influenced by biogenic sources. A series of trace organic compounds previously shown to serve as particle phase tracers for various carbonaceous aerosol source types were examined. Molecular tracer species were generally at or below detection limits, except for the wood smoke tracer levoglucosan in one composite, so maximum possible source influences were calculated using the detection limit as an upper bound to the tracer concentration. Wood smoke was found not to contribute significantly to PM2.5 OM, with contributions for most samples at <1% of the total organic particulate matter. Vehicular exhaust also appeared to make only minor contributions, with maximum possible influences calculated to be 1–4% of PM2.5 OM. Several factors indicate that secondary organic aerosol formation was important throughout the study, and may have significantly altered the molecular composition of the aerosol during transport.  相似文献   

17.
Outdoor and indoor fine particulate species were measured at the Lindon Elementary School in Lindon, Utah, to determine which components of ambient fine particles have strong indoor and outdoor concentration correlations. PM2.5 mass concentrations were measured using tapered element oscillating microbalance (TEOM) monitors and by gravimetric analysis of Teflon filter samples. Gas-phase HNO3, sulfur dioxide, particulate nitrate, strong acid, and particulate sulfate were measured using annular denuder samplers. Soot was measured using quartz filters in filter packs. Total particulate number was measured with a condensation nucleus counter (CNC). Total particulate number and fine particulate sulfate and soot were correlated for ambient and indoor measurements. Indoor PM2.5 mass showed a low correlation with outdoor PM2.5 mass because of the influence of coarse material from student activities on indoor PM2.5. Fine particle acidity and the potentiation of biological oxidative mechanisms by iron were not correlated indoors and outdoors.  相似文献   

18.
Size distribution and selected element concentrations of atmospheric particulate matter (PM) were investigated in the Venice Lagoon, at three sites characterised by different anthropogenic influence. The PM10 samples were collected in six size fractions (10-7.2, 7.2-3.0, 3.0-1.5, 1.5-0.95; 0.95-0.49 and <0.49 μm) with high volume cascade impactors, and the concentration of 17 elements (Al, As, Ca, Cd, Co, Cu, Fe, K, Li, Mg, Mn, Na, Ni, Pb, Sr, V, Zn) was determined by inductively coupled plasma quadrupole mass spectroscopy. More than 1 year of sampling activities allowed the examination of seasonal variability in size distribution of atmospheric particulates and element contents for each site.At all the stations, particles with an aerodynamic diameter <3 μm were predominant, thus accounting for more than 78% of the total aerosol mass concentration. The highest PM10 concentrations for almost all elements were found at the site which is more influenced by industrial and urban emissions. Similarity in size distribution of elements at all sites allowed the identification of three main behavioural types: (a) elements found mainly within coarse particles (Ca, Mg, Na, Sr); (b) elements found mainly within fine particles (As, Cd, Ni, Pb, V) and (c) elements with several modes spread throughout the entire size range (Co, Cu, Fe, K, Zn, Mn).Factor Analysis was performed on aerosol data separately identified as fine and coarse types in order to examine the relationships between the inorganic elements and to identify their origin. Multivariate statistical analysis and assessment of similarity in the size distribution led to similar conclusions on the sources.  相似文献   

19.
Factors controlling the transport of geogenically-derived arsenic from a coastal acid sulfate soil into downstream sediments are identified in this study with both solid-phase associations and aqueous speciation clearly critical to the mobility and toxicity of arsenic. The data from both sequential extractions and X-ray adsorption spectroscopy indicate that arsenic in the unoxidised Holocene acid sulfate soils is essentially non-labile in the absence of prolonged oxidation, existing primarily as arsenopyrite or as an arsenopyrite-like species, likely arsenian pyrite. Anthropogenically-accelerated pedogenic processes, which have oxidised this material over time, have greatly enhanced the potential bioavailability of arsenic, with solid-phase arsenic almost solely present as As(V) associated with secondary Fe(III) minerals present. Analyses of downstream sediments reveal that a portion of the arsenic is retained as a mixed As(III)/As(V) solid-phase, though not at levels considered to be environmentally deleterious. Determination of arsenic speciation in pore waters using high performance liquid chromatography/Inductively Coupled Plasma-Mass Spectrometry shows a dominance of As(III) in upstream pore waters whilst an unidentified As species reaches comparative levels within the downstream, estuarine locations. Pore water As(V) was detected at trace concentrations only. The results demonstrate the importance of landscape processes to arsenic transport and availability within acid sulfate soil environments.  相似文献   

20.
Environmental Science and Pollution Research - Zhengzhou is one of the most heavily polluted cities in China. This study collected samples of PM2.5 (atmospheric fine particulate matter with...  相似文献   

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