Most cited article - PubMed ID 17554427
Trends in background levels of persistent organic pollutants at Kosetice observatory, Czech Republic.1) Part I. Ambient air and wet deposition 1996-2005
Long-term exposure to polycyclic aromatic hydrocarbons (PAHs) and their nitrated (NPAHs) and oxygenated (OPAHs) derivatives can cause adverse health effects due to their carcinogenicity, mutagenicity and oxidative potential. The distribution of PAH derivatives in the terrestrial environment has hardly been studied, although several PAH derivatives are ubiquitous in air and long-lived in soil and water. We report the multi-annual variations in the concentrations of NPAHs, OPAHs and PAHs in soils sampled at a semi-urban (Mokrá, Czech Republic) and a regional background site (Košetice, Czech Republic) in central Europe. The concentrations of the Σ18NPAHs and the Σ11+2OPAHs and O-heterocycles were 0.31 ± 0.23 ng g-1 and 4.03 ± 3.03 ng g-1, respectively, in Košetice, while slightly higher concentrations of 0.54 ± 0.45 ng g-1 and 5.91 ± 0.45 ng g-1, respectively, were found in soil from Mokrá. Among the 5 NPAHs found in the soils, 1-nitropyrene and less so 6-nitrobenzo(a)pyrene were most abundant. The OPAHs were more evenly distributed. The ratios of the PAH derivatives to their parent PAHs in Košetice indicate that they were long-range transported to the background site. Our results show that several NPAHs and OPAHs are abundant in soil and that gas-particle partitioning is a major factor influencing the concentration of several semi-volatile NPAHs and OPAHs in the soils. Complete understanding of the long-term variations of NPAH and OPAH concentrations in soil is limited by the lack of kinetic data describing their formation and degradation.
- Keywords
- Background, Nitrated PAHs, Polycyclic aromatic compounds, soil pollution, Soil exposure, Temporal variation,
- MeSH
- Nitrates MeSH
- Air Pollutants * analysis MeSH
- Environmental Monitoring methods MeSH
- Grassland MeSH
- Polycyclic Aromatic Hydrocarbons * analysis MeSH
- Soil MeSH
- Publication type
- Journal Article MeSH
- Names of Substances
- Nitrates MeSH
- Air Pollutants * MeSH
- Polycyclic Aromatic Hydrocarbons * MeSH
- Soil MeSH
A total of 74 high volume air samples were collected at a background site in Czech Republic from 2012 to 2014 in which the concentrations of 20 per- and polyfluoroalkyl substances (PFASs) were investigated. The total concentrations (gas + particle phase) ranged from 0.03 to 2.08 pg m-3 (average 0.52 pg m-3) for the sum of perfluoroalkyl carboxylic acids (∑PFCAs), from 0.02 to 0.85 pg m-3 (average 0.28 pg m-3) for the sum of perfluoroalkyl sulfonates (ΣPFSAs) and from below detection to 0.18 pg m-3 (average 0.05 pg m-3) for the sum of perfluorooctane sulfonamides and sulfonamidoethanols (ΣFOSA/Es). The gas phase concentrations of most PFASs were not controlled by temperature dependent sources but rather by long-range atmospheric transport. Air mass backward trajectory analysis showed that the highest concentrations of PFASs were mainly originating from continental areas. The average particle fractions (θ) of ΣPFCAs (θ = 0.74 ± 0.26) and ΣPFSAs (θ = 0.78 ± 0.22) were higher compared to ΣFOSA/Es (θ = 0.31 ± 0.35). However, they may be subject to sampling artefacts. This is the first study ever reporting PFASs concentrations in air samples collected over consecutive years. Significant decreases in 2012-2014 for PFOA, MeFOSE, EtFOSE and ∑PFCAs were observed with apparent half-lives of 1.01, 0.86, 0.92 and 1.94 years, respectively.
- Keywords
- Gas-particle partitioning, Long-range atmospheric transport, Multi-year variations, Per- and polyfluoroalkyl substances, Seasonal variations,
- MeSH
- Fluorocarbons analysis MeSH
- Carboxylic Acids MeSH
- Environmental Monitoring MeSH
- Publication type
- Journal Article MeSH
- Geographicals
- Czech Republic MeSH
- Europe MeSH
- Names of Substances
- Fluorocarbons MeSH
- Carboxylic Acids MeSH
Among the nitrated and oxygenated polycyclic aromatic hydrocarbons (NPAHs and OPAHs) are some of the most hazardous substances to public health, mainly because of their carcinogenicity and oxidative potential. Despite these concerns, the concentrations and fate of NPAHs and OPAHs in the atmospheric environment are largely unknown. Ambient air concentrations of 18 NPAHs, 5 quinones, and 5 other OPAHs were determined at two urban and one regional background sites in central Europe. At one of the urban sites, the total (gas and particulate) concentrations of Σ10OPAHs were 10.0 ± 9.2 ng/m3 in winter and 3.5 ± 1.6 ng/m3 in summer. The gradient to the regional background site exceeded 1 order of magnitude. Σ18NPAH concentrations were typically 1 order of magnitude lower than OPAHs. Among OPAHs, 9-fluorenone and (9,10)-anthraquinone were the most abundant species, accompanied by benzanthrone in winter. (9,10)-Anthraquinone represented two-thirds of quinones. We found that a large fraction of the target substance particulate mass was carried by submicrometer particles. The derived inhalation bioaccessibility in the PM10 size fraction is found to be ≈5% of the total ambient concentration of OPAHs and up to ≈2% for NPAHs. For 9-fluorenone and (9,10)-anthraquinone, up to 86 and 18%, respectively, were found at the rural site. Our results indicate that water solubility could function as a limiting factor for bioaccessibility of inhaled particulate NPAHs and OPAHs, without considerable effect of surfactant lipids and proteins in the lung lining fluid.
- MeSH
- Nitrates MeSH
- Air Pollutants * MeSH
- Humans MeSH
- Environmental Monitoring MeSH
- Particulate Matter MeSH
- Polycyclic Aromatic Hydrocarbons * MeSH
- Check Tag
- Humans MeSH
- Publication type
- Journal Article MeSH
- Research Support, Non-U.S. Gov't MeSH
- Geographicals
- Europe MeSH
- Names of Substances
- Nitrates MeSH
- Air Pollutants * MeSH
- Particulate Matter MeSH
- Polycyclic Aromatic Hydrocarbons * MeSH
Polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) are ubiquitous and toxic contaminants. Their atmospheric deposition fluxes on the regional scale were quantified based on simultaneous sampling during 1 to 5 years at 1 to 6 background/rural sites in the Czech Republic and Austria. The samples were extracted and analysed by means of gas chromatography coupled to mass spectrometry. For all seasons and sites, total deposition fluxes for Σ15PAHs ranged 23-1100 ng m-2 d-1, while those for Σ6PCBs and Σ12OCPs ranged 64-4400 and 410-7800 pg m-2 d-1, respectively. Fluoranthene and pyrene were the main contributors to the PAH deposition fluxes, accounting on average for 19% each, while deposition fluxes of PCBs and OCPs were dominated by PCB153 (26%) and γ-hexachlorobenzene (30%), respectively. The highest deposition flux of Σ15PAHs was generally found in spring, while no seasonality was found for PCB deposition. For deposition fluxes for Σ12OCPs, no clear spatial trend was found, confirming the perception of long-lived regional pollutants. Although most OCPs and PCBs hardly partition to the particulate phase in ambient air, on average, 42% of their deposition fluxes were found on filters, confirming the perception that particle deposition is more efficient than dry gaseous deposition. Due to methodological constraints, fluxes derived from bulk deposition samplers should be understood as lower estimates, in particular with regard to those substances which in ambient aerosols mostly partition to the particulate phase.
- Keywords
- Bulk atmospheric deposition, Central Europe, Deposition fluxes, OCPs, PAHs, PCBs, POPs,
- MeSH
- Hydrocarbons, Chlorinated analysis MeSH
- Hexachlorobenzene analysis MeSH
- Air Pollutants analysis MeSH
- Environmental Monitoring * MeSH
- Pesticides analysis MeSH
- Gas Chromatography-Mass Spectrometry MeSH
- Polychlorinated Biphenyls analysis MeSH
- Polycyclic Aromatic Hydrocarbons analysis MeSH
- Publication type
- Journal Article MeSH
- Geographicals
- Czech Republic MeSH
- Europe MeSH
- Austria MeSH
- Names of Substances
- Hydrocarbons, Chlorinated MeSH
- Hexachlorobenzene MeSH
- Air Pollutants MeSH
- Pesticides MeSH
- Polychlorinated Biphenyls MeSH
- Polycyclic Aromatic Hydrocarbons MeSH
Concentrations and isomer compositions of hexabromocyclododecane (HBCD) were measured in six matrices in the Czech Republic (HBCD technical mixture; consumer products; indoor and outdoor air at industrial, urban and background locations; soils; and sediments) to provide insight into changes in concentrations and isomer profiles between environmental sources and environmental sinks. A distinct gradient of air concentrations was observed, from 1600 ng/m3 in the industrial area to < 10 pg/m3 in urban and background air. Isomer profiles also showed a distinct gradient in air, from 95% γ-HBCD in industrial air to 40% γ-HBCD in background air, suggesting the influence of differential atmospheric transport and phototransformation of γ- to α-HBCD. Concentrations and isomer compositions in consumer products were highly variable and indicated differences between products with intentional addition of HBCD as a flame retardant versus those with HBCD as an impurity, e.g., from recycled plastic. Understanding the isomer-specific environmental distributions and processes remains important for risk assessment and toxicology, considering the continued use of HBCD and the isomer-specific differences in uptake, metabolism, and toxicity, and further, demonstrates the utility of isomer profiles to better understand environmental processes of HBCDs.
- Keywords
- Atmospheric transport, Consumer products, Flame retardants, HBCD, Isomer profiles, Sources,
- MeSH
- Hydrocarbons, Brominated analysis chemistry MeSH
- Isomerism MeSH
- Environmental Pollutants analysis chemistry MeSH
- Environmental Monitoring methods MeSH
- Soil chemistry MeSH
- Flame Retardants analysis MeSH
- Consumer Product Safety MeSH
- Air analysis MeSH
- Publication type
- Journal Article MeSH
- Geographicals
- Czech Republic MeSH
- Names of Substances
- Hydrocarbons, Brominated MeSH
- hexabromocyclododecane MeSH Browser
- Environmental Pollutants MeSH
- Soil MeSH
- Flame Retardants MeSH
Organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) were studied to determine occurrence, levels and spatial distribution in the marine atmosphere and surface seawater during cruises in the German Bight and the wider North Sea in spring and summer 2009-2010. In general, the concentrations found in air are similar to, or below, the levels at coastal or near-coastal sites in Europe. Hexachlorobenzene and α-hexachlorocyclohexane (α-HCH) were close to phase equilibrium, whereas net atmospheric deposition was observed for γ-HCH. The results suggest that declining trends of HCH in seawater have been continuing for γ-HCH but have somewhat levelled off for α-HCH. Dieldrin displayed a close to phase equilibrium in nearly all the sampling sites, except in the central southwestern part of the North Sea. Here atmospheric deposition dominates the air-sea exchange. This region, close to the English coast, showed remarkably increased surface seawater concentrations. This observation depended neither on riverine input nor on the elevated abundances of dieldrin in the air masses of central England. A net depositional flux of p,p'-DDE into the North Sea was indicated by both its abundance in the marine atmosphere and the changes in metabolite pattern observed in the surface water from the coast towards the open sea. The long-term trends show that the atmospheric concentrations of DDT and its metabolites are not declining. Riverine input is a major source of PCBs in the German Bight and the wider North Sea. Atmospheric deposition of the lower molecular weight PCBs (PCB28 and PCB52) was indicated as a major source for surface seawater pollution.
- Keywords
- Air-sea exchange, North Sea, Organochlorine pesticides, Polychlorinated biphenyls,
- MeSH
- Atmosphere chemistry MeSH
- Hydrocarbons, Chlorinated analysis MeSH
- Air Pollutants analysis MeSH
- Environmental Monitoring * MeSH
- Seawater chemistry MeSH
- Pesticides analysis MeSH
- Polychlorinated Biphenyls analysis MeSH
- Air analysis MeSH
- Publication type
- Journal Article MeSH
- Geographicals
- England MeSH
- North Sea MeSH
- Names of Substances
- Hydrocarbons, Chlorinated MeSH
- Air Pollutants MeSH
- Pesticides MeSH
- Polychlorinated Biphenyls MeSH
Semi-volatile organic compounds were monitored over a whole year, by collection of gas and particle phases every sixth day at a suburban site in Izmir, Turkey. Annual mean concentrations of 32 polychlorinated biphenyls (∑32PCBs) and 14 polycyclic aromatic hydrocarbons (∑14PAHs) were 348 pg/m3 and 36 ng/m3, respectively, while it was 273 pg/m3 for endosulfan, the dominant compound among 23 organochlorine pesticides (OCPs). Monte Carlo simulation was applied to the USEPA exposure-risk models for the estimation of the population exposure and carcinogenic risk probability distributions for heating and non-heating periods. The estimated population risks associated with dermal contact and inhalation routes to ∑32PCBs, ∑14PAHs, and some of the targeted OCPs (α-hexachlorocyclohexane (α-HCH), β-hexachlorocyclohexane (β-HCH), heptachlor, heptachlor epoxide, α-chlordane (α-CHL), γ-chlordane (γ-CHL), and p,p'-dichlorodiphenyltrichloroethane (p,p'-DDT)) were in the ranges of 1.86 × 10-16-7.29 × 10-9 and 1.38 × 10-10-4.07 × 10-6, respectively. The inhalation 95th percentile risks for ∑32PCBs, ∑14PAHs, and OCPs were about 6, 3, and 4-7 orders of magnitude higher than those of dermal route, respectively. The 95th percentile inhalation risk for ∑32PCBs and OCPs in the non-heating period were 1.8- and 1.2-4.6 folds higher than in the heating period, respectively. In contrast, the 95th percentile risk levels for ∑14PAHs in the heating period were 4.3 times greater than that of non-heating period for inhalation, respectively. While risk levels associated with exposure to PCBs and OCPs did not exceed the acceptable level of 1 × 10-6, it was exceeded for 47 % of the population associated with inhalation of PAHs with a maximum value of about 4 × 10-6.
- Keywords
- Carcinogenic risk *, Exposure *, OCPs *, PAHs *, PCBs *, Persistent organic pollutants *,
- MeSH
- Chlordan analysis MeSH
- Hydrocarbons, Chlorinated analysis MeSH
- DDT analysis MeSH
- Endosulfan analysis MeSH
- Heptachlor analysis MeSH
- Hexachlorocyclohexane analysis MeSH
- Carcinogens, Environmental analysis MeSH
- Air Pollutants analysis MeSH
- Humans MeSH
- Environmental Monitoring * MeSH
- Pesticides analysis MeSH
- Polychlorinated Biphenyls analysis MeSH
- Polycyclic Aromatic Hydrocarbons analysis MeSH
- Seasons * MeSH
- Check Tag
- Humans MeSH
- Publication type
- Journal Article MeSH
- Geographicals
- Turkey MeSH
- Names of Substances
- alpha-hexachlorocyclohexane MeSH Browser
- beta-hexachlorocyclohexane MeSH Browser
- Chlordan MeSH
- Hydrocarbons, Chlorinated MeSH
- DDT MeSH
- Endosulfan MeSH
- Heptachlor MeSH
- Hexachlorocyclohexane MeSH
- Carcinogens, Environmental MeSH
- Air Pollutants MeSH
- Pesticides MeSH
- Polychlorinated Biphenyls MeSH
- Polycyclic Aromatic Hydrocarbons MeSH
Using pine needles as a bio-sampler of atmospheric contamination is a relatively cheap and easy method, particularly for remote sites. Therefore, pine needles have been used to monitor a range of semi-volatile contaminants in the air. In the present study, pine needles were used to monitor polychlorinated biphenyls (PCBs) in the air at sites with different land use types in Sweden (SW), Czech Republic (CZ), and Slovakia (SK). Spatiotemporal patterns in levels and congener profiles were investigated. Multivariate analysis was used to aid source identification. A comparison was also made between the profile of indicator PCBs (ind-PCBs-PCBs 28, 52, 101, 138, 153, and 180) in pine needles and those in active and passive air samplers. Concentrations in pine needles were 220-5100 ng kg(-1) (∑18PCBs - ind-PCBs and dioxin-like PCBs (dl-PCBs)) and 0.045-1.7 ng toxic equivalent (TEQ) kg(-1) (dry weight (dw)). Thermal sources (e.g., waste incineration) were identified as important sources of PCBs in pine needles. Comparison of profiles in pine needles to active and passive air samplers showed a lesser contribution of lower molecular weight PCBs 28 and 52, as well as a greater contribution of higher molecular weight PCBs (e.g., 180) in pine needles. The dissimilarities in congener profiles were attributed to faster degradation of lower chlorinated congeners from the leaf surface or metabolism by the plant.
- Keywords
- Active and passive samplers, Atmospheric pollution, Bio-sampler, Europe, Pine needle, Polychlorinated biphenyls, Sources, Spatial and temporal distribution,
- MeSH
- Pinus sylvestris chemistry metabolism MeSH
- Dioxins chemistry metabolism MeSH
- Plant Leaves chemistry MeSH
- Environmental Monitoring methods MeSH
- Polychlorinated Biphenyls chemistry metabolism MeSH
- Polychlorinated Dibenzodioxins chemistry metabolism MeSH
- Incineration MeSH
- Publication type
- Journal Article MeSH
- Geographicals
- Europe MeSH
- Names of Substances
- Dioxins MeSH
- Polychlorinated Biphenyls MeSH
- Polychlorinated Dibenzodioxins MeSH
Although passive sampling has been previously used for the monitoring of volatile and semi-volatile contaminants in air, there are limited data on the use of this technique coupled with bioassays based on specific biological responses. Biological responses including those mediated by the aryl hydrocarbon (AhR) receptor as well as (anti-)estrogenicity and (anti-)androgenicity of samples from four Eastern European countries (Lithuania, Slovakia, Romania, and Serbia) were determined. To address the potential differences of specific toxic potencies of pollutant mixtures in ambient air in Eastern Europe, each country was characterized by a single more remote location that served to determine regional background conditions and one location in more urbanized and industrialized locations, which were defined as "impacted" areas. Besides samples from Lithuania, a significant gradient in concentrations of AhR-mediated potency from background and impacted localities was observed. Greatest potencies were measured in samples from impacted locations in Romania and Slovakia. Concentrations of polycyclic aromatic hydrocarbons (PAHs) that were quantified accounted for 3-33 % of the 2,3,7,8-tetrachlorodibenzo-p-dioxin equivalents determined by use of the bioassay. No significant estrogenic potency was detected but anti-estrogenic effects were produced by air from two background locations (Lithuania, Slovakia) and three impacted locations (Lithuania, Romania, and Serbia). Anti-androgenic potency was observed in all samples. The greatest anti-estrogenic potency was observed at the background location in Slovakia. Anti-estrogenic and anti-androgenic potencies of studied air samples were probably associated with compounds that are not routinely monitored. The study documents suitability of passive air sampling for the assessment of specific toxic potencies of ambient air pollutants.
- MeSH
- Estrogens analysis MeSH
- Air Pollutants analysis MeSH
- Environmental Monitoring methods MeSH
- Polychlorinated Dibenzodioxins analysis MeSH
- Polycyclic Aromatic Hydrocarbons analysis MeSH
- Receptors, Aryl Hydrocarbon MeSH
- Air Pollution statistics & numerical data MeSH
- Publication type
- Journal Article MeSH
- Research Support, Non-U.S. Gov't MeSH
- Geographicals
- Europe, Eastern MeSH
- Names of Substances
- Estrogens MeSH
- Air Pollutants MeSH
- Polychlorinated Dibenzodioxins MeSH
- Polycyclic Aromatic Hydrocarbons MeSH
- Receptors, Aryl Hydrocarbon MeSH
Atmospheric particulate matter (PM) abundance, mass size distribution (MSD) and chemical composition are parameters relevant for human health effects. The MSD and phase state of semivolatile organic pollutants were determined at various polluted sites in addition to the PM composition and MSD. The distribution pattern of pollutants varied from side to side in correspondence to main particle sources and PM composition. Levels of particle-associated polycyclic aromatic hydrocarbons (PAHs) were 1-30 ng m(-3) (corresponding to 15-35 % of the total, i.e., gas and particulate phase concentrations), of polychlorinated biphenyls (PCBs) were 2-11 pg m(-3) (4-26 % of the total) and of DDT compounds were 2-12 pg m(-3) (4-23 % of the total). The PM associated amounts of other organochlorine pesticides were too low for quantification. The organics were preferentially found associated with particles <0.45 μm of aerodynamic equivalent diameter. The mass fractions associated with sub-micrometer particles (PM0.95) were 73-90 %, 34-71 % and 36-81 % for PAHs, PCBs and DDT compounds, respectively. The finest particles fraction had the highest aerosol surface concentration (6.3-29.7)×10(-6) cm(-1) (44-70 % of the surface concentration of all size fractions). The data set was used to test gas-particle partitioning models for semivolatile organics for the first time in terms of the organics' MSD and size-dependent PM composition. The results of this study prove that at the various sites particles with diverse size, matrix composition, amount of contaminants and toxicological effects occur. Legislative regulation based on gravimetric determination of PM mass can clearly be insufficient for assessment.
- MeSH
- Aerosols analysis MeSH
- Atmosphere chemistry MeSH
- Hydrocarbons, Chlorinated analysis MeSH
- Inhalation Exposure analysis MeSH
- Air Pollutants analysis MeSH
- Humans MeSH
- Environmental Monitoring MeSH
- Pesticides analysis MeSH
- Particulate Matter analysis MeSH
- Polychlorinated Biphenyls analysis MeSH
- Polycyclic Aromatic Hydrocarbons analysis MeSH
- Check Tag
- Humans MeSH
- Publication type
- Journal Article MeSH
- Research Support, Non-U.S. Gov't MeSH
- Names of Substances
- Aerosols MeSH
- Hydrocarbons, Chlorinated MeSH
- Air Pollutants MeSH
- Pesticides MeSH
- Particulate Matter MeSH
- Polychlorinated Biphenyls MeSH
- Polycyclic Aromatic Hydrocarbons MeSH