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1.
Chemosphere ; 118: 81-6, 2015 Jan.
Article in English | MEDLINE | ID: mdl-25014662

ABSTRACT

Polybrominated diphenyl ethers (PBDEs), used as flame retardants since the 1970s, are being phased out of use, but are persistent and widespread in the environment. Historical declines in Eurasian otter (Lutra lutra) populations have been associated with exposure to dieldrin and polychlorinated biphenyls (PCBs), but links with other persistent organic pollutants have not been explored. In this study, liver samples from 129 otters, collected across England and Wales from 1995-2006, were analysed for PBDEs, together with PCBs, DDT breakdown products, and hexachlorobenzene. Associations with geographical location and life history parameters were explored. Concentrations of PBDEs in otters (∑BDE 12-70000ngg(-1) lipid) paralleled those measured in marine mammals, with PBDE-47 the dominant congener and high levels of PBDE-99 and -100. Otter livers contained high concentrations of PBDE-153 and -209, typical of terrestrial top predators. Inter-individual variation in PBDE concentrations was high and correlated with geographical location. ∑PBDE was 25% of ∑PCB, and comparable with ∑DDT, identifying PBDEs as a major contaminant in otter populations in England and Wales.


Subject(s)
Environmental Pollutants/analysis , Halogenated Diphenyl Ethers/analysis , Liver/chemistry , Otters/metabolism , Age Factors , Animals , England , Environmental Monitoring , Environmental Pollutants/pharmacokinetics , Female , Halogenated Diphenyl Ethers/pharmacokinetics , Liver/metabolism , Male , Principal Component Analysis , Wales
2.
Toxicol Appl Pharmacol ; 248(1): 12-9, 2010 Oct 01.
Article in English | MEDLINE | ID: mdl-20600211

ABSTRACT

The persistent organochlorine pesticide lindane is still abundantly found in the environment and in human and animal tissue samples. Lindane induces a wide range of adverse health effects, which are at least partially mediated via the known inhibition of GABA(A) and glycine receptors. Additionally, lindane has been reported to increase the basal intracellular Ca(2+) concentration ([Ca(2+)](i)). As Ca(2+) triggers many cellular processes, including cell death and vesicular neurotransmitter release (exocytosis), we investigated whether lindane affects exocytosis, Ca(2+) homeostasis, production of reactive oxygen species (ROS) and cytotoxicity in neuroendocrine PC12 cells. Amperometric recordings and [Ca(2+)](i) imaging experiments with fura-2 demonstrated that lindane (≥ 10 µM) rapidly increases basal exocytosis and basal [Ca(2+)](i). Additional imaging and electrophysiological recordings revealed that this increase was largely due to a lindane-induced membrane depolarization and subsequent opening of N- and P/Q-type voltage-gated Ca(2+) channels (VGCC). On the other hand, lindane (≥ 3 µM) induced a concentration-dependent but non-specific inhibition of VGCCs, thereby limiting the lindane-induced increase in basal [Ca(2+)](i) and exocytosis. Importantly, the non-specific inhibition of VGCCs also reduced stimulation-evoked exocytosis and Ca(2+) influx. Though lindane exposure concentration-dependently increased ROS production, cell viability was not affected indicating that the used concentrations were not acute cytotoxic. These combined findings indicate that lindane has two, partly counteracting effects. Lindane causes membrane depolarization, thereby increasing basal [Ca(2+)](i) and exocytosis. In parallel, lindane inhibits VGCCs, thereby limiting the basal effects and reducing stimulation-evoked [Ca(2+)](i) and exocytosis. This study further underlines the need to consider presynaptic, non-receptor-mediated effects in human risk assessment.


Subject(s)
Calcium/metabolism , Exocytosis/drug effects , Hexachlorocyclohexane/toxicity , Insecticides/toxicity , Animals , Calcium Channels, N-Type/drug effects , Calcium Channels, N-Type/metabolism , Calcium Channels, P-Type/drug effects , Calcium Channels, P-Type/metabolism , Calcium Channels, Q-Type/drug effects , Calcium Channels, Q-Type/metabolism , Dose-Response Relationship, Drug , Electrophysiology , Hexachlorocyclohexane/administration & dosage , Homeostasis/drug effects , Insecticides/administration & dosage , PC12 Cells , Rats , Reactive Oxygen Species/metabolism
3.
Environ Sci Technol ; 43(16): 6364-9, 2009 Aug 15.
Article in English | MEDLINE | ID: mdl-19746738

ABSTRACT

Many studies have demonstrated that persistent organic pollutants are transferred from mother to pup during lactation in phocid seals, but none have been able to determine the significance of these findings for survivorship. The aim of this study was to investigate the relationship between blubber contaminant concentrations and first-year survival in gray seal pups. A mark-recapture framework was used to estimate survival probabilities and animals were "marked" using novel mobile phone tags. Individual and group covariates (sex, condition, and blubber contaminants) were embedded within a live-resighting model. The most significant covariates remained condition at weaning and sex (males in poor condition had the lowest survival probability), as was found previously, but there was also evidence indicating that higher blubber contaminants additionally decreased survivorship. The models' Akaike's Information Criteria (AICs) and their associated weights, point toward the tetrapolybrominated diphenyl ether congeners (dominated by BDE-47) as being the most important group of contaminants affecting survival probability, followed by the total dichlorodiphenyltrichloroethanes (DDTs) and pentapolychlorinated biphenyl congeners. These compounds were not the most abundant in the blubber, suggesting further studies into their toxicological effects in this species are necessary. The specific mechanisms driving the reduction in survivorship remain unknown.


Subject(s)
Environmental Exposure/analysis , Environmental Monitoring , Environmental Pollutants/analysis , Organic Chemicals/analysis , Seals, Earless/metabolism , Animals , Confidence Intervals , Environmental Exposure/adverse effects , Environmental Pollutants/poisoning , Likelihood Functions , Organic Chemicals/poisoning , Probability , Survival Analysis , Weaning
4.
Environ Sci Technol ; 43(9): 3356-64, 2009 May 01.
Article in English | MEDLINE | ID: mdl-19534158

ABSTRACT

Whether polybrominated diphenyl ethers (PBDEs) induce effects in target cells is increasingly important given that their environmental burdens are rising. Attenuated total reflection Fourier-transform infrared (ATR-FTIR) spectroscopy can be used to biochemically signature cells based on the notion that a detailed "biochemical-cell fingerprint" in the form of an infrared (IR) spectrum is derived. By employing subsequent computational approaches such as principal component analysis (PCA) and/or linear discriminant analysis (LDA), data reduction is achieved to allow for the identification of wavenumber-related biomarkers of effect Clustering of similar spectra (or scores) away from dissimilar ones highlights the variance responsible for discriminating classes. Discriminating biomarkers might include protein conformational changes, structural alterations to DNA/RNA, glycogen content, or protein phosphorylation. Employing this approach, we investigated in MCF-7 cells the dose-related effects of PBDEs (congeners 47, 153, 183, and 209), benzo[a]pyrene (B[a]P), 2-amino-1-methyl-6-phenylimidazo[4,5-b]pyridine (PHIP), 17beta-Oestradiol (E2), or lindane (gamma-hexachlorocyclohexane). Cultures concentrated in G0/G1- or S-phases were treated for 24 h. Following treatment MCF-7 cells were fixed and applied to IR reflective Low-E windows for interrogation using ATR-FTIR spectroscopy. At concentrations as low as 10(-12) M in culture, significant separation (P < or = 0.05) of PBDE-treated and vehicle control cell populations was noted. In some cases this was associated with alterations in lipid or the secondary structure of proteins; with DNA-reactive compounds (e.g., B[a]P), variance was primarily noted in the DNA/RNA region. This study points to a novel nondestructive approach capable of identifying contaminant effects at environmental concentrations in target cells.


Subject(s)
Benzo(a)pyrene/toxicity , Biochemical Phenomena/drug effects , DNA/metabolism , Endocrine Disruptors/toxicity , Halogenated Diphenyl Ethers/toxicity , Imidazoles/toxicity , Cell Line, Tumor , Humans , Principal Component Analysis , Spectroscopy, Fourier Transform Infrared
5.
Environ Sci Technol ; 43(7): 2602-7, 2009 Apr 01.
Article in English | MEDLINE | ID: mdl-19452923

ABSTRACT

Beef and dairy products can be important vectors of human exposure to polybrominated diphenylethers (BDEs), and hence an understanding of BDE transfer from feed to cows' milk and tissue is important for BDE exposure assessment The fate of tri- to hexaBDEs in lactating cows exposed to a naturally contaminated diet was studied by analyzing feed, feces, and milk samples from a mass balance study. Tissue distribution was studied in one cowslaughtered afterthe experiment The carryover rates from feed to milk ranged from 0.15 to 0.35 for the major congeners. Lower values were observed for several of the tetrabrominated congeners, and this was attributed to metabolism. The dietary absorption efficiency decreased with increasing octanol-water partition coefficient of the BDE congener. The absorption behavior was consistent with a model based on chemical lipophilicity, but agreed less well with a model based on effective molecular diameter, and it violated Lipinski's "rule of 5". The lipid normalized concentrations were similar in all tissues analyzed including liver and milk, suggesting that tissue distribution is governed by partitioning into lipids. Overall, the behavior of the tri- to hexaBDEs was consistent with that observed for other classes of halogenated aromatic contaminants such as PCBs and PCDD/Fs, but it differed markedly from the behavior of the hepta- decaBDEs.


Subject(s)
Lactation , Milk/chemistry , Polybrominated Biphenyls/analysis , Animal Feed/analysis , Animals , Cattle , Female , Intestinal Absorption , Mass Spectrometry , Polybrominated Biphenyls/pharmacokinetics , Tissue Distribution
6.
Environ Sci Technol ; 42(1): 100-5, 2008 Jan 01.
Article in English | MEDLINE | ID: mdl-18350882

ABSTRACT

The uptake kinetics and storage of PCBs by isolated cuticles and cuticular waxes from Hedera helix, Prunus laurocerasus, and Ilex aquifolium were studied. Small chambers were used, allowing variation in plant uptake parameters to be studied by having the same air boundary layer in each chamber. During the 64 day study tri- and tetrachlorinated biphenyls generally reached equilibrium in waxes but not in whole cuticles. Differences between species were observed. Higher chlorinated PCB congeners did not approach equilibrium in either sample type. Although PCBs showed higher affinity for waxes than whole cuticles, the latter dominated the total uptake capacity on a surface area basis, because of the large amount of nonwax cuticular components. Mass transfer coefficients (MTCs) for PCB uptake (into both cuticles and waxes) indicated partition dependence up to log octanol/air partition coefficients (K(OA)) of 8.5-10, depending on species and sample type. For cuticles, higher MTCs occurred at the beginning of the experiment than later. This was not seen in reconstituted waxes, a difference which may be explained by the dispersion of intracuticular waxes within cuticles. For more lipophilic compounds, uptake appeared to be limited by diffusion processes, which may be influenced by plant physiology. Leaf surface area is, therefore, likely to control the ability of vegetation to scavenge these compounds from the air in many field situations.


Subject(s)
Air Pollutants/analysis , Hedera/chemistry , Ilex/chemistry , Polychlorinated Biphenyls/analysis , Prunus/chemistry , Waxes/chemistry , Kinetics , Plant Leaves
7.
Environ Int ; 34(3): 412-9, 2008 Apr.
Article in English | MEDLINE | ID: mdl-17961649

ABSTRACT

The occurrence of the major components of the decabromodiphenyl ether (deca-BDE) flame retardant and other PBDEs was investigated in daily air particulate samples from 17th April to 20th May 2004 at a semi-rural site in north-west England. BDE-209 was found at between <0.49 and 100 pg m(-3) (median 13 pg m(-3)), and other higher-brominated PBDE congeners were also found, particularly the nona-BDEs (e.g. BDE-207: <0.042-79 pg m(-3), median 2.5 pg m(-3)). Deca- and nona-BDEs dominated the median particulate sample congener profile: 60% BDE-209, 16% BDE-207, 6% BDE-208 and 4% BDE-206. Nona-BDEs were greatly enriched, relative to BDE-209, compared to the deca-BDE commercial mixture, which may suggest degradation of BDE-209 between source and sampling site, or release from older deca-BDE commercial mixtures, which may have contained higher proportions of nona-BDEs. The highest PBDE concentrations occurred when air-masses passed over urban and industrial areas to the SSW-SW, though small local influences may also be seen. PBDE concentrations appear to have been influenced mainly by particle levels: 1-3 microm diameter particles for BDE-153, and 3-10 microm particles for BDEs with 7-10 Br atoms. BDE-153 may either be released from combustion sources, or re-condense onto small particles after emission, whereas BDE-209 and nona-BDEs appear to be associated with larger dust particles from industrial or domestic sources.


Subject(s)
Air Pollution , Particulate Matter/chemistry , Phenyl Ethers/analysis , Polybrominated Biphenyls/analysis , Air Movements , England , Environmental Monitoring , Flame Retardants/analysis , Halogenated Diphenyl Ethers
8.
Chemosphere ; 70(9): 1596-602, 2008 Feb.
Article in English | MEDLINE | ID: mdl-17888489

ABSTRACT

The levels and distribution of polynuclear aromatic hydrocarbons (PAHs) were determined in soil samples from background locations in the UK and Norway, to investigate their spatial distribution and the controlling environmental factors. Concentrations ranged between 42 and 11200 microg kg(-1) (geometric mean 640 microg kg(-1)) and 8.6 and 1050 microg kg(-1) (150 microg kg(-1)) dry weight in the UK and Norwegian soil, respectively. Proximity to sources and locations susceptible to high atmospheric depositional inputs resulted in higher concentrations. Statistically significant relationships were observed between PAH and total organic carbon (TOC) in the Norwegian samples. High molecular weight PAHs correlated with black carbon (BC) in UK-woodland soil. These observations support the hypothesis that TOC plays an important role in the retention of PAHs in soil and that PAHs are often combined with BC during combustion emissions. PAHs with 4 and more rings comprised approximately 90% of total PAHs in the UK soil, but only 50% in the Norwegian soil. The mixture of PAHs implied that fractionation occurred during long-range atmospheric transport and deposition. The lighter PAHs with lower K(ow) values more readily reached the most remote sites. The heavier PAHs with higher K(ow) values remained in closer proximity to sources.


Subject(s)
Organic Chemicals/analysis , Polycyclic Aromatic Hydrocarbons/analysis , Soil/analysis , Carbon/analysis , Environmental Monitoring , Europe , Geography , Norway , Organic Chemicals/chemistry , Polycyclic Aromatic Hydrocarbons/chemistry , United Kingdom
9.
Environ Toxicol Chem ; 26(12): 2486-93, 2007 Dec.
Article in English | MEDLINE | ID: mdl-18020674

ABSTRACT

The uptake, transport, storage, and processing of semivolatile organic chemicals (SVOCs) by vegetation plays an important role in their environmental fate. Understanding these processes at the plant cellular level is essential to understanding the fate and behavior of SVOCs within the environment. Traditional analytical methods have relied on destructive analysis of the plant and a level of inference to suggest exactly where within the plant the chemical is residing, how it is getting there, and what its subsequent fate might be. The use of two-photon excitation microscopy to visualize the in situ uptake, transport, storage, compartmentalization, processing, and fate of a number of polycyclic aromatic hydrocarbons (PAHs) in living vegetation is summarized. Using this technique, the uptake of PAHs to leaves and roots via the atmosphere or soil is visualized. Subsequent storage, transport, compartmentalization, and plant processing, including metabolism, can then be monitored. Differences in processing of the same chemical between species are observed, including compartmentalization, transport routes, and degradation pathways. Chemical location within the plant is observed to have a significant effect on PAH fate (e.g., through photodegradation). We highlight a number of key findings and the research areas requiring increased impetus to gain a comprehensive understanding of the complexity involved in SVOC-plant interactions from the cellular to global scales.


Subject(s)
Microscopy, Fluorescence/methods , Plant Structures/chemistry , Plant Structures/metabolism , Polycyclic Aromatic Hydrocarbons/analysis , Air , Fluorescence , Plant Structures/growth & development , Polycyclic Aromatic Hydrocarbons/pharmacokinetics , Sensitivity and Specificity , Soil Pollutants/analysis , Soil Pollutants/pharmacokinetics , Tissue Distribution , Volatilization
10.
J Environ Monit ; 9(11): 1176-82, 2007 Nov.
Article in English | MEDLINE | ID: mdl-17968443

ABSTRACT

An atmospheric deposition sampler was validated with respect to polybrominated diphenyl ethers (PBDEs), a compound group that is widely used as flame retardants in many types of consumer products. The deposition sampler consists of an adsorption cartridge that is connected to a glass funnel. Extraction tests with spiked cartridges using soxhlet extraction with acetone revealed recoveries of >80% for all of the investigated PBDEs. Once adsorbed, PBDEs are stable, as proven by extractions of spiked cartridges that were stored outdoors and collected after different periods of time, up to 84 days. High recoveries indicate that degradation of adsorbed PBDEs does not play a role under realistic field conditions. Bulk deposition rates of PBDEs were determined in a field test with 3 replicates, and a possible breakthrough of target compounds was assessed in the field using a second adsorption cartridge in series. No breakthrough of target compounds could be observed within a sampling period of 61 days, and a bulk deposition rate of approximately 1 ng m(-2) day(-1) for the sum of all analysed PBDEs was measured. The highest deposition rates were measured for octa-brominated congeners, followed by BDEs 99, 183, 153, and 47. Overall, the sampler was successfully validated regarding the atmospheric deposition of PBDEs.


Subject(s)
Air Pollutants/analysis , Polybrominated Biphenyls/analysis , Adsorption , Atmosphere , Chromatography, Gel , Ethers , Gas Chromatography-Mass Spectrometry , Quality Control , Reference Standards
11.
Environ Sci Technol ; 41(16): 5647-53, 2007 Aug 15.
Article in English | MEDLINE | ID: mdl-17874768

ABSTRACT

In P.R. China, electronic waste (e-waste) from across the world is dismantled and discarded. Concentrations of polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs), and organochlorine pesticides (OCPs) were measured in serum from residents of an e-waste dismantling region (Guiyu, South China), where 80% of families work in e-waste recycling, and compared to a matching cohort from a nearby region where the fishing industry dominates (Haojiang). Serum concentrations of PBDEs and OCPs, but not PCBs, were significantly different in the two regions: the median sigmaPBDE concentration was 3 times higher in Guiyu than Haojiang, whereas the opposite was true for dichloro-diphenyl-trichloroethane (DDT). PBDEs typically accounted for 46% of the total organohalogen chemicals in samples from Guiyu, but 8.7% in Haojiang. The median BDE-209 concentration in Guiyu was 50-200 times higher than previously reported in occupationally exposed populations. The highest BDE-209 concentration was 3100 ng/g lipid, the highest yet reported in humans. Serum PBDE concentrations did not correlate with PCBs or OCPs, whereas PCBs and OCPs showed positive correlations, suggesting that sources of PBDEs to humans are different from PCBs and OCPs. The levels of PBDEs in individuals from Haojiang are possibly related to the recycling activity at Guiyu, through atmospheric transport.


Subject(s)
Electronics , Environmental Monitoring , Occupational Exposure , Pesticides/blood , Polybrominated Biphenyls/blood , Polychlorinated Biphenyls/blood , Refuse Disposal/methods , Adolescent , Adult , Aged , Aged, 80 and over , China , Female , Humans , Male , Middle Aged , Polybrominated Biphenyls/administration & dosage , Polychlorinated Biphenyls/administration & dosage , Workforce
12.
Environ Sci Technol ; 41(16): 5915-22, 2007 Aug 15.
Article in English | MEDLINE | ID: mdl-17874806

ABSTRACT

We set out to determine whether infrared (IR) spectra of treated MCF-7 cells derived using attenuated total reflection Fourier-transform IR (ATR) microspectroscopy could be used to signature different exposures. Serum-lipid samples from residents living in an electronics waste (e-waste) dismantling region (Region E, n = 26) in the south of P.R. China or from a nearby region (Region S, n = 20) associated with the fishing industry were obtained. Following extraction, estrogen receptor-positive MCF-7 cells were treated for 24 h with < or = 5-mg lipid equivalent of individual extracts prior to ethanol fixation; subsequently, IR spectra of treated-cell populations were obtained using ATR microspectroscopy. Levels of organochlorinated and brominated compounds in parallel extracts were also determined. Principal component analysis (PCA) was employed to ascertain whether IR-spectral scores would cluster according to particular cohort. Scores plots following PCA highlighted significant clustering dependent on with which set of extracts MCF-7 cells were treated. This suggests marked differences in the cell-biochemical modulating effects induced by either set of extracts. Analysis of contaminant profiles in the extracts showed that polybrominated diphenyl ethers (PBDEs) accounted for 46.0% of total organohalogens and were higher than dichloro-diphenyl-trichloroethanes (DDTs) in Region E; DDTs were the major contaminants (85.2% of total contaminant load) compared to PBDEs (8.7%) in Region S. These results suggest that ATR microspectroscopy can segregate cell-biochemical effects as a consequence of very different exposure paradigms.


Subject(s)
Environmental Monitoring/methods , Flame Retardants/administration & dosage , Hydrocarbons, Brominated/administration & dosage , Hydrocarbons, Chlorinated/administration & dosage , Lipids/blood , Lipids/pharmacology , Occupational Exposure/analysis , Adolescent , Cell Line, Tumor , Cluster Analysis , Electronics , Environmental Pollutants/administration & dosage , Environmental Pollutants/analysis , Female , Humans , Hydrocarbons, Brominated/analysis , Hydrocarbons, Chlorinated/analysis , Male , Middle Aged , Principal Component Analysis , Refuse Disposal , Spectrophotometry, Infrared , Tissue Extracts
13.
Environ Toxicol Chem ; 26(5): 851-61, 2007 May.
Article in English | MEDLINE | ID: mdl-17521129

ABSTRACT

Polychlorinated biphenyls, DDT and its metabolites, polybrominated diphenyl ethers, and selected organochlorine pesticide concentrations were measured in blubber samples from 60 free-living harbor seals in 2003 from five sites around the United Kingdom coast. Significant regional differences among contaminant levels were found, with seals on Islay and Jura (southwest Scotland) having the highest levels of polychlorinated biphenyls and seals in the Wash (eastern England) having the highest polybrominated diphenyl ether levels. Animals from the north and northeast of Scotland (Orkney and the Moray Firth) had the lowest levels of all the contaminant groups studied. Congener-specific profiles of polychlorinated biphenyls and polybrominated diphenyl ethers showed relatively higher levels of the lower chlorinated and brominated compounds at the more northerly sites, with the lowest total levels of both chemical groups. Significant positive relationships between blubber contaminants and total triiodothyronine (TT3) concentrations were found after controlling for the potential effects of confounding because of sex, mass, and season. Increased serum TT3 levels were significantly related to higher blubber contaminant concentrations in the following order: sum of all contaminants > polybrominated diphenyl ethers > polychlorinated biphenyls > DDT. Serum TT3 levels in the harbor seals with the highest exposures might be indicative of a T3 thyrotoxicosis, but without information on free T3 and circulating thyroid-stimulating hormone levels, it is difficult to determine the importance of this observation for the health of the individuals or populations. However, the mixture of contaminants to which United Kingdom harbor seals are exposed has changed over the last few decades, and the toxicological and epidemiological importance of adding the brominated compounds to the classical organochlorine and heavy metal mixture is not known.


Subject(s)
DDT/analysis , Phenyl Ethers/analysis , Polybrominated Biphenyls/analysis , Polychlorinated Biphenyls/analysis , Seals, Earless/metabolism , Triiodothyronine/metabolism , Water Pollutants, Chemical/analysis , Animals , Environmental Monitoring , Geography , Pesticides/analysis , Pesticides/metabolism , Risk Assessment , United Kingdom
14.
Environ Sci Technol ; 41(2): 417-23, 2007 Jan 15.
Article in English | MEDLINE | ID: mdl-17310701

ABSTRACT

Dietary intake studies of lower brominated diphenyl ethers (BDEs) have shown that fish and animal products are important vectors of human exposure, but almost no data exist for higher brominated BDEs. Therefore, the fate of hepta- to decaBDEs was studied in lactating cows exposed to a naturally contaminated diet by analyzing feed, feces, and milk samples from a previous mass balance study of PCB. Tissue distribution was studied in one cow slaughtered after the experiment. BDE-209 was the dominant congener in feed, organs, adipose tissues, and feces, but not in milk. In contrast to PCBs and lower brominated BDEs, concentrations of hepta- to decaBDEs in adipose tissue were 9-80 times higher than in milk fat and the difference increased with degree of bromination/log K(OW). The congener profiles in adipose tissue and feed differed; BDE-207, BDE-196, BDE-197, and BDE-182 accumulated to a surprisingly greater extent in the fat compared to their isomers, suggesting metabolic debromination of BDE-209 to these BDEs. The results indicate that meat rather than dairy product consumption may be an important human exposure route to higher brominated BDEs.


Subject(s)
Cattle/metabolism , Diet , Environmental Monitoring/statistics & numerical data , Environmental Pollutants/pharmacokinetics , Phenyl Ethers/pharmacokinetics , Polybrominated Biphenyls/pharmacokinetics , Adipose Tissue/chemistry , Animal Feed/analysis , Animals , Environmental Pollutants/analysis , Environmental Pollutants/chemistry , Feces/chemistry , Female , Lactation , Mass Spectrometry , Milk/chemistry , Molecular Structure , Phenyl Ethers/analysis , Phenyl Ethers/chemistry , Polybrominated Biphenyls/analysis , Polybrominated Biphenyls/chemistry , Tissue Distribution
15.
J Environ Monit ; 8(7): 700-10, 2006 Jul.
Article in English | MEDLINE | ID: mdl-16826283

ABSTRACT

Data are presented for polynuclear aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), polybrominated diphenyls ethers (PBDEs) and selected organochlorine compounds (OCs) in passive air samplers (PAS) along a rural/remote latitudinal transect from southern UK to northern Norway during 2002-2004. This study is part of an ongoing campaign, using semi-permeable membrane devices (SPMDs) as PAS over two year intervals since 1994. Data for PCBs, selected OCs and PBDEs are compared with that from previous campaigns. Absolute sequestered amounts of selected PCB congeners have decreased in a first order fashion between 1994-2004, with an average atmospheric clearance rate of 4.1 +/- 0.6 years and continue to fractionate with latitude. HCB has also declined between 1998-2004, with a clearance rate of 6 +/- 2.4 years. Data on DDT and its breakdown products indicate little fresh release in Europe. Comparison of PBDEs in 2000-02 and 2002-04 indicates site differences, generally with increases at UK sites and decreases in Norway. BDE-28, 47 and 49 decreased with increasing latitude (p < 0.04), while the other congeners did not show any significant latitudinal dependence. Transect data are presented for PAHs the first time. Three- and 4-ringed compounds dominated the mixture present in the SPMD. The PAH composition of the SPMDs at site 3 was compared to the average composition taken by active sampling at the same site. SPMD performance for sampling PAHs leaves many uncertainties, but they can be successfully used to semiquantitatively detect PAHs in the atmosphere. Fluorene and phenanthrene increased with latitude (p > 0.05), while 1-methylphenanthere, fluoranthene, benzo[b]fluoranthene and indeno[123-cd]pyrene decreased. Results are discussed in terms of sources, long-range atmospheric transport, global fractionation and clearance processes.


Subject(s)
Hydrocarbons, Chlorinated/analysis , Phenyl Ethers/analysis , Polybrominated Biphenyls/analysis , Polychlorinated Biphenyls/analysis , Polycyclic Aromatic Hydrocarbons/analysis , Air Pollutants/analysis , Environmental Monitoring , Geography , Norway , Time Factors , United Kingdom
16.
Environ Int ; 32(7): 915-29, 2006 Sep.
Article in English | MEDLINE | ID: mdl-16814386

ABSTRACT

Chlorinated paraffins (CPs), as technical mixtures of polychlorinated alkanes (PCAs), are ubiquitous in the environment. CPs tend to behave in a similar way to persistent organic pollutants (POPs), leading several countries to impose regulations on the use of CPs. In this article, we review the literature on the properties of CPs, the current analytical tools available to determine CPs in various types of environmental matrices, and concentrations found in the environment. In particular, concentrations of CPs in environmental compartments including air, water, sediments, biota, human food products and human tissues are summarized. Priorities for future research are: improvements in analytical methodologies (reducing the complexity of the analysis, producing reference materials and performing interlaboratory studies); determining background levels of chlorinated paraffins in the environment and human populations (this question should be answered using quality assured analytical tools allowing the intercomparison of data); and investigating the sources of CPs to the environment and to humans.


Subject(s)
Environmental Monitoring/methods , Environmental Pollutants/analysis , Hydrocarbons, Chlorinated/analysis , Paraffin/chemistry , Animals , Biodiversity , Environmental Pollutants/chemistry , Food , Humans , Hydrocarbons, Chlorinated/chemistry , Paraffin/analysis , Principal Component Analysis/methods , Quality Control , Tissue Distribution
17.
Environ Sci Technol ; 40(3): 907-16, 2006 Feb 01.
Article in English | MEDLINE | ID: mdl-16509336

ABSTRACT

Two-photon excitation microscopy (TPEM) was used to monitor the air-to-leaf transfer and within-leaf movement and distribution of phenanthrene in two plant species (maize and spinach) grown within a contaminated atmosphere. Phenanthrene was visualized within the leaf cuticle, epidermis, mesophyll, and vascular system of living maize and spinach plants. No detectable levels of phenanthrene were observed in the roots or stems of either species, suggesting phenanthrene entered the leaves only from the air. Phenanthrene was observed in both the abaxial and adaxial cuticles of both species. Particulate material (aerosols/dust) contaminated with phenanthrene was located at the surface of the cuticle and became encapsulated within the cuticularwaxes. Overtime, diffuse areas of phenanthrene formed within the adjacent cuticle. However, most of the visualized phenanthrene reaching the leaves arrived via gas-phase transfer. Phenanthrene was found within the wax plugs of stomata of both species and on the external surface of the stomatal pore, but not on the internal surface, or within the sub-stomatal cavity. Phenanthrene diffused through the cuticles of both species in 24-48 h, entering the epidermis to reside predominantly within the cell walls of maize (indicative of apoplastic transport) and the cellular cytoplasm of spinach (indicative of symplastic transport). Phenanthrene accumulated within the spinach cytoplasm where it concentrated into the vacuoles of the epidermal cells. Phenanthrene was not observed to accumulate in the cytoplasm of maize cells. Phenanthrene entered the internal mesophyll of both species, and was found within the mesophyll cell walls, at the surface of the chloroplasts, and within the cellular cytoplasm. Phenanthrene was observed within the xylem of maize following 12 days exposure. The cuticle and epidermis at the edges of spinach leaves had a systematically higher concentration of phenanthrene than the cuticle and epidermal cells at the center of the leaf. These results provide important new information about how such compounds enter, move, and distribute within leaves, and suggest that contemporary views of such processes based on data obtained from traditional analytical methods may need to be revised.


Subject(s)
Environmental Pollutants/pharmacokinetics , Phenanthrenes/pharmacokinetics , Plant Leaves , Adsorption , Cytoplasm/chemistry , Diffusion , Microscopy , Photons , Spinacia oleracea/chemistry , Zea mays/chemistry
18.
Environ Int ; 32(1): 34-40, 2006 Jan.
Article in English | MEDLINE | ID: mdl-15979717

ABSTRACT

Chlorinated paraffins (also called polychlorinated n-alkanes -- PCAs) are a class of industrial chemicals comprising chlorinated straight chain hydrocarbons. They have a wide range of applications and are now found in a range of environmental compartments. We analysed a total of 25 human milk-fat samples, donated by 18 individuals from the urban London and more rural Lancaster areas in the UK, for short chain PCAs (C(10)-C(13) sPCAs) and medium chain PCAs (C(14)-C(17) mPCAs), using gas chromatography-ECNI high-resolution mass spectrometry. Our study confirms that trace quantities of PCAs can reach human milk-fat. sPCAs were detected in all but four samples, while mPCAs were detected in all samples. The median sPCA concentration was 180 ng/g fat (range of 49 to 820 ng/g fat -- detected values only) and the median mPCA concentration was 21 ng/g fat (range of 6.2 to 320 ng/g fat). No differences were noted in ranges of observed values for either sPCAs or mPCAs between samples from London and Lancaster. Most samples also exhibited similar patterns of sPCAs and mPCAs. One sample exhibited a different pattern for sPCAs and mPCAs, an observation that may be related to differences in exposure or biological factors for this individual.


Subject(s)
Fats/chemistry , Hydrocarbons, Chlorinated/analysis , Hydrocarbons, Chlorinated/chemistry , Milk, Human/chemistry , Paraffin/analysis , Paraffin/chemistry , Humans , United Kingdom
19.
Environ Pollut ; 141(1): 30-41, 2006 May.
Article in English | MEDLINE | ID: mdl-16236409

ABSTRACT

Blood serum from 154 volunteers at 13 UK locations in 2003 were analysed for a range of PCBs, organochlorine pesticides and PBDEs. HCB, p,p'-DDE and p,p'-DDT and beta-HCH were the dominant organochlorine pesticides in most samples. BDEs 47, 99, 100, 153, 154 and 183 were the most regularly detected PBDEs. This study is the first report of BDE209 in UK human blood (found in 11 samples, range < 15-240 ng/g lipid). Concentration and age correlated for the less easily metabolised PCBs, p,p'-DDT and p,p'-DDE, HCB and HCHs. With increasing age females tended to have lower concentrations of the more chlorinated PCBs than males. Similar PBDE concentrations, and distributions, to those reported in the general population in Sweden in 2002 were found, despite differences in historical PBDE production and usage. There is increasing regulation to control persistent and bioaccumulative chemicals, and establishing human exposure will help to identify substances which should be urgently phased out.


Subject(s)
Environmental Monitoring/methods , Environmental Pollutants/blood , Hydrocarbons, Halogenated/blood , Pesticides/blood , Adult , Age Distribution , Blood Specimen Collection/methods , Environmental Exposure , Female , Flame Retardants/analysis , Geography , Halogenated Diphenyl Ethers , Humans , Hydrocarbons, Chlorinated/blood , Linear Models , Male , Patient Selection , Phenyl Ethers/blood , Polybrominated Biphenyls/blood , Polychlorinated Biphenyls/blood , Sensitivity and Specificity , Sex Distribution , Sweden , United Kingdom , United States , Urban Population
20.
Environ Sci Technol ; 39(13): 4729-38, 2005 Jul 01.
Article in English | MEDLINE | ID: mdl-16053070

ABSTRACT

Atmospheric concentrations of polychlorinated naphthalenes (PCNs) (108 samples in total) were measured at two rural/ semirural sites in England and one remote site on the west coast of Ireland in the years 2001 and 2000, respectively. Detailed analysis of the factors affecting concentrations is performed. At Mace Head (MH) Ireland, concentrations of sigmaPCNs ranged between 1.7 and 55 pg m(-3) with a mean of 15 pg m(-3) and were controlled primarily by advection. sigmaPCNs concentrations at Hazelrigg (HR), northwest England, ranged between 31 and 310 pg m(-3) with a mean of 110 pg m(-3), and at Chilton (CH), southwest England, ranged between 31 and 180 pg m(-3) with a mean of 85 pg m(-3). Data from the HR site shows that PCN concentrations have not declined between the early 1990s and 2001, while PCB concentrations have declined. The ratio of the sigmaPCNs/ sigmaPCBs was close to or greater than 1 at all sites. From air mass back trajectories, it is clear that local/regional sources influenced concentrations of PCNs at all sites, particularly at MH. At the two English sites during the summer, concentrations of PCNs were strongly influenced by temperature, indicating that air-surface exchange processes play an important role. Advection became more influential during winter, particularly at CH, where a different homologue profile was observed in some samples when air masses approached from the southwest and PCN concentrations increased. The average mixture profile of PCNs in air was similar to that observed in other studies and different from that in Halowax 1014.


Subject(s)
Air Pollutants/analysis , Chlorine Compounds/chemistry , Naphthalenes/chemistry , Air Movements , Chlorine Compounds/analysis , England , Environmental Monitoring , Ireland , Naphthalenes/analysis , Rural Population , Seasons , Temperature , Volatilization
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