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Sökning: WFRF:(McLachlan Michael S.) > (2010-2014)

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1.
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2.
  • Krogseth, Ingjerd S., et al. (författare)
  • Occurrence and seasonality of cyclic volatile methyl siloxanes in arctic air
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:1, s. 502-509
  • Tidskriftsartikel (refereegranskat)abstract
    • Cyclic volatile methyl siloxanes (cVMS) are present in technical applications and personal care products. They are predicted to undergo long-range atmospheric transport, but measurements of cVMS in remote areas remain scarce. An active air sampling method for decamethylcyclopentasiloxane (D5) was further evaluated to include hexamethylcyclotrisiloxane (D3), octamethylcyclotetrasiloxane (D4), and dodecamethylcyclohexasiloxane (D6). Air samples were collected at the Zeppelin observatory in the remote Arctic (79 degrees N, 12 degrees E) with an average sampling time of 81 +/- 23 h in late summer (August-October) and 25 +/- 10 h in early winter (November-December) 2011. The average concentrations of D5 and D6 in late summer were 0.73 +/- 0.31 and 0.23 +/- 0.17 ng/m(3), respectively, and 2.94 +/- 0.46 and 0.45 +/- 0.18 ng/m(3) in early winter, respectively. Detection of D5 and D6 in the Arctic atmosphere confirms their long-range atmospheric transport. The D5 measurements agreed well with predictions from a Eulerian atmospheric chemistry-transport model, and seasonal variability was explained by the seasonality in the OH radical concentrations. These results extend our understanding of the atmospheric fate of D5 to high latitudes, but question the levels of D3 and D4 that have previously been measured at Zeppelin with passive air samplers.
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3.
  • McLachlan, Michael S., et al. (författare)
  • Using Model-Based Screening to Help Discover Unknown Environmental Contaminants
  • 2014
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 48:13, s. 7264-7271
  • Tidskriftsartikel (refereegranskat)abstract
    • Of the tens of thousands of chemicals in use, only a small fraction have been analyzed in environmental samples. To effectively identify environmental contaminants, methods to prioritize chemicals for analytical method development are required. We used a high-throughput model of chemical emissions, fate, and bioaccumulation to identify chemicals likely to have high concentrations in specific environmental media, and we prioritized these for target analysis. This model-based screening was applied to 215 organosilicon chemicals culled from industrial chemical production statistics. The model-based screening prioritized several recognized organosilicon contaminants and generated hypotheses leading to the selection of three chemicals that have not previously been identified as potential environmental contaminants for target analysis. Trace analytical methods were developed, and the chemicals were analyzed in air, sewage sludge, and sediment. All three substances were found to be environmental contaminants. Phenyl-tris(trimethylsiloxy)silane was present in all samples analyzed, with concentrations of similar to 50 pg m(-3) in Stockholm air and similar to 0.5 ng g(-1) dw in sediment from the Stockholm archipelago. Tris(trifluoropropyl)trimethyl-cyclotrisiloxane and tetrakis(trifluoropropyl)tetramethyl-cyclotetrasiloxane were found in sediments from Lake Mjosa at similar to 1 ng g(-1) dw. The discovery of three novel environmental contaminants shows that models can be useful for prioritizing chemicals for exploratory assessment.
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4.
  • Norström, Karin, et al. (författare)
  • External exposure and bioaccumulation of PCBs in humans living in a contaminated urban environment.
  • 2010
  • Ingår i: Environment International. - : Elsevier BV. - 0160-4120 .- 1873-6750. ; 36:8, s. 855-861
  • Tidskriftsartikel (refereegranskat)abstract
    • Humans are exposed to different mixtures of PCBs depending on the route of exposure. In this study we investigated the potential contribution of inhalation to the overall human exposure to PCBs in an urban area. For this purpose, the mechanistically based, non-steady state bioaccumulation model ACC-HUMAN was applied to predict the PCB body burden in an adult living in the Midwestern United States who eats a typical North American diet and inhales air contaminated with PCBs. Dietary exposure was estimated using measured data for eighteen PCB congeners in different food groups (fish, meat and egg, dairy products). Two scenarios for inhalation exposure were evaluated: one using air concentrations measured in Chicago, and a second using air measurements in a remote area on Lake Michigan, Sleeping Bear Dunes. The model predicted that exposure via inhalation increases the accumulated mass of PCBs in the body by up to 30% for lower chlorinated congeners, while diet is by far the dominant source of exposure for those PCB congeners that accumulate most in humans.
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5.
  • Adolfsson-Erici, Margaretha, et al. (författare)
  • A flow-through passive dosing system for continuously supplying aqueous solutions of hydrophobic chemicals to bioconcentration and aquatic toxicity tests
  • 2012
  • Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 86:6, s. 593-599
  • Tidskriftsartikel (refereegranskat)abstract
    • A continuous supply of water with defined stable concentrations of hydrophobic chemicals is a requirement in a range of laboratory tests such as the OECD 305 protocol for determining the bioconcentration factor in fish. Satisfying this requirement continues to be a challenge, particularly for hydrophobic chemicals. Here we present a novel solution based on equilibrium passive dosing. It employs a commercially available unit consisting of similar to 16000 polydimethylsiloxane (PDMS) tubes connected to two manifolds. The chemicals are loaded into the unit by repeatedly perfusing it with a methanol solution of the substances that is progressively diluted with water. Thereafter the unit is perfused with water and the chemicals partition from the unit into the water. The system was tested with nine chemicals with logK(ow) ranging from 4.1 to 6.3. The aqueous concentrations generated were shown to be largely independent of the water flow rate, and the unit to unit reproducibility was within a factor of similar to 2. In continuous flow experiments the aqueous concentrations of most of the study chemicals remained constant over 8 d. A model was assembled that allows prediction of the operating characteristics of the system from the logKow or PDMS/water partition coefficient of the chemical. The system is a simple, safe, predictable and flexible tool that generates stable aqueous concentrations of hydrophobic chemicals.
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6.
  • Adolfsson-Erici, Margaretha, et al. (författare)
  • In-vivo passive sampling to measure elimination kinetics in bioaccumulation tests
  • 2012
  • Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 88:1, s. 62-68
  • Tidskriftsartikel (refereegranskat)abstract
    • The application of in-tissue passive sampling to quantify chemical kinetics in fish bioconcentration experiments was investigated. A passive sampler consisting of an acupuncture needle covered with a PDMS tube was developed together with a method for its deployment in rainbow trout. The time to steady state for chemical uptake into the passive sampler was >1 d, so it was employed as a kinetically limited sampler with a deployment time of 2 h. The passive sampler was employed in parallel with the established whole tissue extraction method to study the elimination kinetics of 10 diverse chemicals in rainbow trout. 4-n-nonylphenol and 2,4,6-tri-tert-butylphenol were close to or below the limit of quantification in the sampler. For chlorpyrifos, musk xylene, hexachlorobenzene, 2,5-dichlorobiphenyl and p,p'-DDT. the elimination rate constants determined with the passive sampler method and the established method agreed within 18%. Poorer agreement (35%) was observed for 2,3,4-trichloroanisole and p-diisopropylbenzene because fewer data were obtained with the passive sampling method due to its lower sensitivity. The work shows that in-tissue passive sampling can be employed to measure contaminant elimination kinetics in fish. This opens up the possibility of studying contaminant kinetics in individual fish, thereby reducing the fish requirements and analytical costs for the determination of bioconcentration factors.
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7.
  • Adolfsson-Erici, Margaretha, et al. (författare)
  • Internal Benchmarking Improves Precision and Reduces Animal Requirements for Determination of Fish Bioconcentration Factors
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:15, s. 8205-8211
  • Tidskriftsartikel (refereegranskat)abstract
    • The enactment of new chemical regulations has generated a large need for the measurement of the fish bioconcentration factor (BCF). Past experience shows that the BCF determination lacks precision, requires large numbers of fish, and is costly. A new protocol was tested that shortens the experiment from up to 12 weeks for existing protocols to 2 weeks and reduces the number of fish by a factor of 5, while introducing internal benchmarking for the BCF determination. Rainbow trout were simultaneously exposed to 11 chemicals. The BCFs were quantified using one of the test chemicals, musk xylene, as a benchmark. These were compared with BCFs measured in a parallel experiment based on the OECD 305 guideline. The agreement was <20% for five chemicals and between 20%-25% for two further, while two chemicals lay outside the BCF operating window of the experiment and one was lost due to analytical difficulties. This agreement is better than that observed in a BCF Gold Standard Database. Internal benchmarking allows the improvement of the precision of BCF determination in parallel to large reduction in costs and fish requirements.
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8.
  • Adolfsson-Erici, Margaretha, et al. (författare)
  • Measuring bioconcentration factors in fish using exposure to multiple chemicals and internal benchmarking to correct for growth dilution
  • 2012
  • Ingår i: Environmental Toxicology and Chemistry. - : Wiley. - 0730-7268 .- 1552-8618. ; 31:8, s. 1853-1860
  • Tidskriftsartikel (refereegranskat)abstract
    • Modern chemical legislation requires measuring the bioconcentration factor (BCF) of large numbers of chemicals in fish. The BCF must be corrected for growth dilution, because fish growth rates vary between laboratories. Two hypotheses were tested: (1) that BCFs of multiple chemicals can be measured simultaneously in one experiment, and (2) that internal benchmarking using a conservative test substance in the chemical mixture can be used to correct for growth dilution. Bioconcentration experiments were conducted following major elements of the OECD 305 guideline. Fish were simultaneously exposed to 11 chemicals selected to cover a range of BCFs and susceptibility to biotransformation. A method was developed to calculate the growth-corrected elimination rate constant from the concentration ratio of the analyte and a benchmarking chemical for which growth dilution dominated other elimination mechanisms. This method was applied to the experimental data using hexachlorobenzene as the benchmarking chemical. The growth dilution correction lowered the apparent elimination rate constants by between 5% and a factor of four for eight chemicals, while for two chemicals the growth-corrected elimination rate constant was not significantly different from zero. The benchmarking method reduced the uncertainty in the elimination rate constant compared to the existing method for growth dilution correction. The BCFs from exposing fish to 10 chemicals at once were consistent with BCF values from single-chemical exposures from the literature, supporting hypothesis 1. Environ. Toxicol. Chem. 2012; 31: 18531860. (c) 2012 SETAC
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9.
  • Arnot, Jon A., et al. (författare)
  • Prioritizing Chemicals and Data Requirements for Screening-Level Exposure and Risk Assessment
  • 2012
  • Ingår i: Journal of Environmental Health Perspectives. - : Environmental Health Perspectives. - 0091-6765 .- 1552-9924. ; 120:11, s. 1565-1570
  • Tidskriftsartikel (refereegranskat)abstract
    • BACKGROUND: Scientists and regulatory agencies strive to identify chemicals that may cause harmful effects to humans and the environment; however, prioritization is challenging because of the large number of chemicals requiring evaluation and limited data and resources. OBJECTIVES: We aimed to prioritize chemicals for exposure and exposure potential and obtain a quantitative perspective on research needs to better address uncertainty in screening assessments. METHODS: We used a multimedia mass balance model to prioritize > 12,000 organic chemicals using four far-field human exposure metrics. The propagation of variance (uncertainty) in key chemical information used as model input for calculating exposure metrics was quantified. RESULTS: Modeled human concentrations and intake rates span approximately 17 and 15 orders of magnitude, respectively. Estimates of exposure potential using human concentrations and a unit emission rate span approximately 13 orders of magnitude, and intake fractions span 7 orders of magnitude. The actual chemical emission rate contributes the greatest variance (uncertainty) in exposure estimates. The human biotransformation half-life is the second greatest source of uncertainty in estimated concentrations. In general, biotransformation and biodegradation half-lives are greater sources of uncertainty in modeled exposure and exposure potential than chemical partition coefficients. CONCLUSIONS: Mechanistic exposure modeling is suitable for screening and prioritizing large numbers of chemicals. By including uncertainty analysis and uncertainty in chemical information in the exposure estimates, these methods can help identify and address the important sources of uncertainty in human exposure and risk assessment in a systematic manner.
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10.
  • Binnington, Matthew J., et al. (författare)
  • Evaluating the Effectiveness of Fish Consumption Advisories : Modeling Prenatal, Postnatal, and Childhood Exposures to Persistent Organic Pollutants
  • 2014
  • Ingår i: Journal of Environmental Health Perspectives. - : Environmental Health Perspectives. - 0091-6765 .- 1552-9924. ; 122:2, s. 178-186
  • Tidskriftsartikel (refereegranskat)abstract
    • Background: Because human exposure to persistent organic pollutants (POPs) occurs mainly through ingestion of contaminated food, regulatory bodies issue dietary consumption advisories to describe safe intake levels for food items of concern, particularly fish. Objectives: Our study goal was to estimate the effectiveness of fish consumption advisories in reducing exposure of infants and children to POPs. Methods: We used the time-variant mechanistic model CoZMoMAN to estimate and compare prenatal, postnatal, and childhood exposure to polychlorinated biphenyl congener PCB-153 under different scenarios of maternal guideline adherence for both hypothetical constant and realistic time-variant chemical emissions. The scenarios differed in terms of length of compliance (1 vs. 5 years), extent of fish substitution (all vs. half), and replacement diet (uncontaminated produce vs. beef). We also estimated potential exposure reductions for a range of theoretical chemicals to explore how guideline effectiveness varies with a chemical's partitioning and degradation properties. Results: When assuming realistic time periods of advisory compliance, our findings suggest that temporarily eliminating or reducing maternal fish consumption is largely ineffective in reducing pre-and postnatal exposure to substances with long elimination half-lives in humans, especially during periods of decreasing environmental emissions. Substituting fish with beef may actually result in higher exposure to certain groups of environmental contaminants. On the other hand, advisories may be highly effective in reducing exposure to substances with elimination half-lives in humans shorter than the length of compliance. Conclusions: Our model estimates suggest that fish consumption advisories are unlikely to be effective in reducing prenatal, postnatal, and childhood exposures to compounds with long elimination half-lives in humans.
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11.
  • Borga, Katrine, et al. (författare)
  • Consistency in Trophic Magnification Factors of Cyclic Methyl Siloxanes in Pelagic Freshwater Food Webs Leading to Brown Trout
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:24, s. 14394-14402
  • Tidskriftsartikel (refereegranskat)abstract
    • Cyclic volatile methyl siloxanes (cVMS) concentrations were analyzed in the pelagic food web of two Norwegian lakes (Mjosa, Randsfjorden), and in brown trout (Salmo trutta) and Arctic char (Salvelinus alpinus) collected in a reference lake (Femunden), in 2012. Lakes receiving discharge from wastewater treatment plants (Mjosa and Randsfjorden) had cVMS concentrations in trout that were up to 2 orders of magnitude higher than those in Femunden, where most samples were close to the limit of quantification (LOO). Food web biomagnification of cVMS in Mjosa and Randsfjorden was quantified by estimation of trophic magnification factors (TMFs). TMF for legacy persistent organic pollutants (POPs) were analyzed for comparison. Both decamethylcyclopentasiloxane (DS) and dodecamethylcyclohexasiloxane (D6) biomagnified with TMFs of 2.9 (2.1-4.0) and 2.3 (1.8-3.0), respectively. Octamethylcyclotetrasiloxane (D4) was below the LOQ in the majority of samples and had substantially lower biomagnification than for D5 and D6. The cVMS TMFs did not differ between the lakes, whereas the legacy POP TMFs were higher in Mjosa than inRandsfjorden. Whitefish had lower cVMS bioaccumulation compared to legacy POPs, and affected the TMF significance for cVMS, but not for POPs. TMFs of D5 and legacy contaminants in Lake Mjosa were consistent with those previously measured in Mjosa.
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12.
  • Borga, Katrine, et al. (författare)
  • Food Web Accumulation of Cyclic Siloxanes in Lake Mjosa, Norway
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:11, s. 6347-6354
  • Tidskriftsartikel (refereegranskat)abstract
    • The biomagnification of the cyclic volatile methyl siloxanes octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexatetrasiloxane (D6) was analyzed in the Lake Mjosa food web in Norway from zooplankton and Mysis to planktivorous and piscivorous fish. The trophic magnification factor (TMF) for D5 was determined and compared with TMFs of several legacy contaminants: polychlorinated biphenyl (PCB) congeners 153 and 180, polybrominated diphenyl ether (PBDE) congeners 47 and 99, and p,p'-DDE. D5 showed TMF significantly greater than 1, implying food web biomagnification (TMF = 2.28, CI: 1.22-4.29). This contrasts with two studies that reported TMF < 1, which may reflect variability in TMF between food webs. The Lake Mjosa D5 TMF was sensitive to the species included at the higher trophic level; whole food web TMF differed from TMF excluding smelt (Osmerus eperlanus) or brown trout (Salmo trutta) (TMF-SMELT = 1.62, CI: 0.96-2.72; TMF-TROUT = 3.58, CI: 1.82-7.03). For legacy contaminants (e.g., PCB-153 and PCB-180), the TMFs were less sensitive to the food web composition, and a better model fit was obtained compared to D5. The differences in biomagnification behavior between D5 and the legacy contaminants suggest that the biomagnification of D5 is being governed by species-specific properties such as biotransformation rate or tissue distribution that differ from those of legacy contaminants.
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13.
  • Breivik, Knut, et al. (författare)
  • Screening organic chemicals in commerce for emissions in the context of environmental and human exposure
  • 2012
  • Ingår i: Journal of Environmental Monitoring. - : Royal Society of Chemistry (RSC). - 1464-0325 .- 1464-0333. ; 14:8, s. 2028-2037
  • Tidskriftsartikel (refereegranskat)abstract
    • Quantitative knowledge of organic chemical release into the environment is essential to understand and predict human exposure as well as to develop rational control strategies for any substances of concern. While significant efforts have been invested to characterize and screen organic chemicals for hazardous properties, relatively less effort has been directed toward estimating emissions and hence also risks. Here, a rapid throughput method to estimate emissions of discrete organic chemicals in commerce has been developed, applied and evaluated to support screening studies aimed at ranking and identifying chemicals of potential concern. The method builds upon information in the European Union Technical Guidance Document and utilizes information on quantities in commerce (production and/or import rates), chemical function (use patterns) and physical-chemical properties to estimate emissions to air, soil and water within the OECD for five stages of the chemical life-cycle. The method is applied to 16 029 discrete substances (identified by CAS numbers) from five national and international high production volume lists. As access to consistent input data remains fragmented or even impossible, particular attention is given to estimating, evaluating and discussing uncertainties in the resulting emission scenarios. The uncertainty for individual substances typically spans 3 to 4 orders of magnitude for this initial tier screening method. Information on uncertainties in emissions is useful as any screening or categorization methods which solely rely on threshold values are at risk of leading to a significant number of either false positives or false negatives. A limited evaluation of the screening method's estimates for a sub-set of about 100 substances, compared against independent and more detailed emission scenarios presented in various European Risk Assessment Reports, highlights that up-to-date and accurate information on quantities in commerce as well as a detailed breakdown on chemical function are critically needed for developing more realistic emission scenarios.
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14.
  • Egebäck, Anna-Lena, et al. (författare)
  • Decabromodiphenyl ethane and decabromodiphenyl ether in Swedish background air
  • 2012
  • Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 86:3, s. 264-269
  • Tidskriftsartikel (refereegranskat)abstract
    • Decabromodiphenyl ethane (DPDPE) is a flame retardant that has been on the market for more than 20 years and is used as a replacement for decabromodiphenyl ether (BDE-209). Environmental data on DPDPE are scarce but for BDE-209, studies have shown that long-range transport in the atmosphere leads to contamination of remote regions. Given their similar physical-chemical properties, we hypothesized that this is also true for DPDPE. In this study we explored the European continent as a source for DBDPE by collecting air samples at a back-ground location in southern Sweden. Twelve samples with stable air mass back trajectories over the 24 h sampling period were analysed. BDE-209 and 5 polycyclic aromatic hydrocarbons (PAHs) were also included in the study. The concentration ranges of DBDPE and BDE-209 were similar, 0.077-7.9 and 0.093-1.8 pg m(-3) air, respectively. The highest concentrations were detected when the air originated from the European continent and the lowest during periods with rather stagnant air over southern Scandinavia. The concentrations of DBDPE and BDE-209 did not co-vary, indicating that there are different major sources of the two compounds. In air, the compounds measured in this study are predominantly associated with particles. PAHs in the atmosphere are known to originate primarily from combustion processes and their concentrations were highly correlated with several measures of atmospheric particle concentration, i.e. PM 10, PM 2.5, soot, and N 450 (number of particles in the size range approximately 420-450 nm). No clear correlations were found between the concentrations of DBDPE or BDE-209 and any of the measures of particle concentrations, indicating that the emissions of these are not related to the major sources of emissions of soot or small particles.
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15.
  • Felizeter, Sebastian, et al. (författare)
  • Root Uptake and Trans location of Perfluorinated Alkyl Acids by Three Hydroponically Grown Crops
  • 2014
  • Ingår i: Journal of Agricultural and Food Chemistry. - : American Chemical Society (ACS). - 0021-8561 .- 1520-5118. ; 62:15, s. 3334-3342
  • Tidskriftsartikel (refereegranskat)abstract
    • Tomato, cabbage, and zucchini plants were grown hydroponically in a greenhouse. They were exposed to 14 perfluorinated alkyl acids (PFAAs) at four different concentrations via the nutrient solution. At maturity the plants were harvested, and the roots, stems, leaves, twigs (where applicable), and edible parts (tomatoes, cabbage head, zucchinis) were analyzed separately. Uptake and transfer factors were calculated for all plant parts to assess PFAA translocation and distribution within the plants. Root concentration factors were highest for long-chain PFAAs (>C11) in all three plant species, but these chemicals were not found in the edible parts. All other PFAAs were present in all above-ground plant parts, with transpiration stream concentration factors (sTSCFs) of 0.05-0.25. These PFAAs are taken up with the transpiration stream and accumulate primarily in the leaves. Although some systematic differences were observed, overall their uptake from nutrient solution to roots and their further distribution within the plants were similar between plant species and among PFAAs.
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16.
  • Felizeter, Sebastian, et al. (författare)
  • Uptake of Perfluorinated Alkyl Acids by Hydroponically Grown Lettuce (Lactuca sativa)
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:21, s. 11735-11743
  • Tidskriftsartikel (refereegranskat)abstract
    • An uptake study was carried out to assess the potential human exposure to perfluorinated alkyl acids (PFAAs) through the ingestion of vegetables. Lettuce (Lactuca sativa) was grown in PFAA-spiked nutrient solutions at four different concentrations, ranging from 10 ng/L to 10 mu g/L. Eleven perfluorinated carboxylic acids (PFCAs) and three perfluorinated sulfonic acids (PFSAs) were analyzed by HPLC-MS/MS. At the end of the experiment, the major part of the total mass of each of the PFAAs (except the short-chain, C4-C7, PFCAs) taken up by plants appeared to be retained in the nonedible part, viz, the roots. Root concentration factors (RCF), foliage/root concentration factors (FRCF), and transpiration stream concentration factors (TSCF) were calculated. For the long chained PFAAs, RCF values were highest, whereas FRCF were lowest. This indicates that uptake by roots is likely governed by sorption of PFAAs to lipid-rich root solids. Translocation from roots to shoots is restricted and highly depending on the hydrophobicity of the compounds. Although the TSCF show that longer chain PFCAs (e g, perfluorododecanoic acid) get better transferred from the nutrient solution to the foliage than shorter-chain PFCAs (e.g., perfluoroheptanoic acid), the major fraction of longer-chain PFCAs is found in roots due to additional adsorption from the spiked solution. Due to the strong electron-withdrawing effect of the fluorine atoms the role of the negative charge of the dissociated PFAAs is likely insignificant.
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17.
  • Filipovic, Marko, 1985-, et al. (författare)
  • Mass Balance of Perfluoroalkyl Acids in the Baltic Sea
  • 2013
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:9, s. 4088-4095
  • Tidskriftsartikel (refereegranskat)abstract
    • A mass balance was assembled for perfluorohexanoic acid (PFHxA), perfluorooctanoic acid (PFOA), perfluorodecanoic acid (PFDA), and perfluorooctanesulfonic acid (PFOS) in the Baltic Sea. Inputs (from riverine discharge, atmospheric deposition, coastal wastewater discharges, and the North Sea) and outputs (to sediment burial, transformation of the chemical, and the North Sea), as well as the inventory in the Baltic Sea, were estimated from recently published monitoring data. Formation of the chemicals in the water column from precursors was not considered. River inflow and atmospheric deposition were the dominant inputs, while wastewater treatment plant (WWTP) effluents made a minor contribution (<5%). A mass balance of the Oder River watershed was assembled to explore the sources of the perfluoroalkyl acids (PFAAs) in the river inflow. It indicated that WWTP effluents made only a moderate contribution to riverine discharge (21% for PFOA, 6% for PFOS), while atmospheric deposition to the watershed was 1-2 orders of magnitude greater than WWTP discharges. The input to the Baltic Sea exceeded the output for all four PFAAs, suggesting that inputs were higher during 2005-2010 than during the previous 20 years despite efforts to reduce emissions of PFAAs. One possible explanation is the retention and delayed release of PFAAs from atmospheric deposition in the soils and groundwater of the watershed.
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18.
  • Fridén, Ulrika E., et al. (författare)
  • Chlorinated paraffins in indoor air and dust : Concentrations, congener patterns, and human exposure
  • 2011
  • Ingår i: Environment International. - : Elsevier BV. - 0160-4120 .- 1873-6750. ; 37:7, s. 1169-1174
  • Tidskriftsartikel (refereegranskat)abstract
    • Chlorinated paraffins (CPs) are large production volume chemicals used in a wide variety of commercial applications. They are ubiquitous in the environment and humans. Human exposure via the indoor environment has, however, been barely investigated. In the present study 44 indoor air and six dust samples from apartments in Stockholm, Sweden, were analyzed for CPs. and indoor air concentrations are reported for the first time. The sumCP concentration (short chain CPs (SCCPs) and medium chain CPs (MCCPs)) in air ranged from <5-210 ng m(-3) as quantified by gas chromatography coupled to electron ionization tandem mass spectrometry (GC/EI-MS/MS). Congener group patterns were studied using GC with electron capture negative ionization MS (GC/ECNI-MS). The air samples were dominated by the more volatile SCCPs compared to MCCPs. SumCPs were quantified by GC/EI-MS/MS in the dust samples at low mu g g(-1) levels, with a chromatographic pattern suggesting the prevalence of longer chain CPs compared to air. The median exposure to sumCPs via the indoor environment was estimated to be similar to 1 mu g day(-1) for both adults and toddlers. Adult exposure was dominated by inhalation, while dust ingestion was suggested to be more important for toddlers. Comparing these results to literature data on dietary intake indicates that human exposure to CPs from the indoor environment is not negligible.
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19.
  • Fridén, Ulrika E., 1973- (författare)
  • Sources, emissions, and occurrence of chlorinated paraffins in Stockholm, Sweden
  • 2010
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • Chlorinated paraffins (CPs) are ubiquitous environmental contaminants. They fulfill all of the criteria (persistent, toxic, and subject to long-range transport) for persistent organic pollutants (POPs) according to the United Nations Economic Commission for Europe (UNECE). CPs are also under consideration for inclusion in the Stockholm Convention on POPs. Their presence has been shown in various environmental matrices in the industrialized parts of the world, as well as in remote regions such as the Arctic. The aim of this thesis was to increase the limited knowledge of the presence of CPs in the environment, their sources to the environment, and the resulting human exposure. An analytical procedure for the determination of CPs in environmental samples based on gas chromatography coupled to electron capture detection (GC-ECD) has been developed. GC-ECD is a relatively inexpensive instrument that is fast and easy to operate. These advantages open up the possibility for a comprehensive screening of the occurrence of CPs in the environment, including developing countries. Furthermore, the occurrence of CPs in ambient air and in indoor air and dust was studied. Elevated CP concentrations in indoor air (<5-210 ng/m3) were observed compared to ambient air (0.7-33 ng/m3), which is indicative of the presence of indoor emission sources. Indoor air and dust concentrations were used to estimate the human exposure to CPs via the indoor environment. Comparison of the estimates to available dietary intake estimates indicated that the indoor exposure pathways are not negligible. CP concentrations in ambient air from urban Stockholm were higher than in rural Aspvreten, Sweden. This indicates the presence of additional (emission) sources in urban areas compared to rural sites. Additionally, a seasonal variation of air concentrations was observed at both locations, suggesting temperature dependent emission sources for CPs. These observations were supported by a substance flow analysis of CPs performed for Stockholm. This study estimated the major emission sources of CPs to the Stockholm environment to be emissions from painted surfaces and in-place sealants.
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20.
  • Jahnke, Annika, et al. (författare)
  • EQUILIBRIUM SAMPLING OF ENVIRONMENTAL POLLUTANTS IN FISH : COMPARISON WITH LIPID-NORMALIZED CONCENTRATIONS AND HOMOGENIZATION EFFECTS ON CHEMICAL ACTIVITY
  • 2011
  • Ingår i: Environmental Toxicology and Chemistry. - : Wiley. - 0730-7268 .- 1552-8618. ; 30:7, s. 1515-1521
  • Tidskriftsartikel (refereegranskat)abstract
    • Equilibrium sampling of organic pollutants into the silicone polydimethylsiloxane (PDMS) has recently been applied in biological tissues including fish. Pollutant concentrations in PDMS can then be multiplied with lipid/PDMS distribution coefficients (D(Lipid.PDMS)) to obtain concentrations in fish lipids. In the present study, PDMS thin films were used for equilibrium sampling of polychlorinated biphenyls (PCBs) in intact tissue of two eels and one salmon. A classical exhaustive extraction technique to determine lipid-normalized PCB concentrations, which assigns the body burden of the chemical to the lipid fraction of the fish, was additionally applied. Lipid-based PCB concentrations obtained by equilibrium sampling were 85 to 106% (Norwegian Atlantic salmon), 108 to 128% (Baltic Sea eel), and 51 to 83% (Finnish lake eel) of those determined using total extraction. This supports the validity of the equilibrium sampling technique, while at the same time confirming that the fugacity capacity of these lipid-rich tissues for PCBs was dominated by the lipid fraction. Equilibrium sampling was also applied to homogenates of the same fish tissues. The PCB concentrations in the PDMS were 1.2 to 2.0 times higher in the homogenates (statistically significant in 18 of 21 cases, p < 0.05), indicating that homogenization increased the chemical activity of the PCBs and decreased the fugacity capacity of the tissue. This observation has implications for equilibrium sampling and partition coefficients determined using tissue homogenates.
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21.
  • Jahnke, Annika, et al. (författare)
  • Sensitive equilibrium sampling to study polychlorinated biphenyl disposition in Baltic Sea sediment
  • 2012
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:18, s. 10114-10122
  • Tidskriftsartikel (refereegranskat)abstract
    • An equilibrium sampling approach using glass jars with pm thin coatings of the silicone polydimethylsiloxane (PDMS) was validated and applied to background sediment samples from a >50 km transect in the Stockholm Archipelago. Equilibrium between the sediment and the PDMS was demonstrated using different coating thicknesses. From the concentrations of polychlorinated biphenyls (PCBs) in the PDMS, we assessed (i) freely dissolved concentrations in the sediment interstitial porewater (C-Sediment_free); (ii) the equilibrium brium status between sediment and water; (iii) the equilibrium status between sediment and biota; and (iv) site-specific sediment/water distribution ratios (K-D). The results showed that (i) Stockholm was a source of PCBs to the Baltic Sea as evidenced by significantly higher C-Sediment_free in Stockholm Harbor; (ii) the fugacity in sediment exceeded that in water (monitoring samples collected in February) by an average factor of 4.0; (iii) the fugacity in sediment exceeded that in herring by an average factor of 5.2; and (iv) K-D near Stockholm Harbor was 0.3-1.7 log units greater than in the outer archipelago. The coated glass jar method with its high precision and built-in QA/QC opens new possibilities to study the disposition of hydrophobic chemicals at trace levels (C-Sediment_free down to 1.06 fg/L) in background environments.
  •  
22.
  • Jahnke, Annika, et al. (författare)
  • Silicone passive equilibrium samplers as 'chemometers' in eels and sediments of a Swedish lake
  • 2014
  • Ingår i: Environmental Science Processes and Impacts. - : Royal Society of Chemistry (RSC). - 2050-7887 .- 2050-7895. ; 16:3, s. 464-472
  • Tidskriftsartikel (refereegranskat)abstract
    • Passive equilibrium samplers deployed in two or more media of a system and allowed to come to equilibrium can be viewed as 'chemometers' that reflect the difference in chemical activities of contaminants between the media. We applied silicone-based equilibrium samplers to measure relative chemical activities of seven 'indicator' polychlorinated biphenyls (PCBs) and hexachlorobenzene in eels and sediments from a Swedish lake. Chemical concentrations in eels and sediments were also measured using exhaustive extraction methods. Lipid-normalized concentrations in eels were higher than organic carbon-normalized concentrations in sediments, with biota-sediment accumulation factors (BSAFs) of five PCBs ranging from 2.7 to 12.7. In contrast, chemical activities of the same pollutants inferred by passive sampling were 3.5 to 31.3 times tower in eels than in sediments. The apparent contradiction between BSAFs and activity ratios is consistent with the sorptive capacity of lipids exceeding that of sediment organic carbon from this ecosystem by up to 50-fold. Factors that may contribute to the elevated activity in sediments are discussed, including slower response of sediments than water to reduced emissions, sediment diagenesis and sorption to phytoplankton. The 'chemometer' approach has the potential to become a powerful tool to study the thermodynamic controls on persistent organic chemicals in the environment and should be extended to other environmental compartments.
  •  
23.
  • Kierkegaard, Amelie, et al. (författare)
  • Bioaccumulation of decamethylcyclopentasiloxane in perch in Swedish lakes
  • 2013
  • Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 93:5, s. 789-793
  • Tidskriftsartikel (refereegranskat)abstract
    • Decamethylcyclopentasiloxane (D5), a high production volume chemical used in personal care products, enters the environment both via air and sewage treatment plant (STP) recipients. It has been found in fish, and there is concern that it may be a bioaccumulative substance. In this work D5 was analyzed in perch from six Swedish lakes that did not receive STP effluent, and in perch and sediment from six lakes that received STP effluent. In the lakes receiving the STP effluent, the D5 concentrations in sediment varied over three orders of magnitude and were correlated with the number of persons connected to the STP normalized to the surface area of the receiving body. In the lakes not receiving effluent, the D5 levels in perch were all below the LOQ while D5 was above the LOQ in almost all perch from lakes that received effluent. The D5 concentrations in perch and sediment from the lakes receiving STP effluent were correlated. This shows that STP effluent is a much more important source of D5 to aquatic ecosystems than atmospheric deposition, and that the risk of adverse effects of D5 on aquatic life will be greatest in small recipients receiving large amounts of STP effluent. The bioaccumulation of D5 was compared to that of PCB 180 on the basis of multimedia bioaccumulation factors (mmBAFs), which describe the fraction of the contaminant present in the whole aquatic environment (i.e. water and surface sediment) that is transferred to the fish. In four of the six lakes the mmBAF of D5 was >0.3 of the mmBAF of PCB 180. Given that PCB 180 is a known highly bioaccumulative chemical, this indicates that the bioaccumulation of D5 in perch is considerable.
  •  
24.
  • Kierkegaard, Amelie, et al. (författare)
  • Cyclic Volatile Methylsiloxane Bioaccumulation in Flounder and Ragworm in the Humber Estuary
  • 2011
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 45:14, s. 5936-5942
  • Tidskriftsartikel (refereegranskat)abstract
    • Cyclic volatile methylsiloxanes are being subjected to regulatory scrutiny as possible PET chemicals. The investigation of bioaccumulation has yielded apparently contradictory results, with high laboratory fish bioconcentration factors on the one hand and low field trophic magnification factors on the other. In this study, octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6) were studied along with polychlorinated biphenyls (PCBs) in sediments, ragworm, and flounder from six sites in the Humber Estuary. Bioaccumulation was evaluated using multimedia bioaccumulation factors (mmBAFs) which quantified the fraction of the contaminant present in the aquatic environment that is transferred to the biota. PCB 180, a known strongly bioaccumulative chemical, was used as a benchmark. The mean mmBAF of D5 was about twice that of PCB 180 in both polycheates and flounder, while for D4 it was 6 and 14 times higher, respectively. The mmBAF of D6 was a factor 5-10 lower than that of PCB180. The comparatively strong multimedia bioaccumulation of D4 and D5, even in the absence of biomagnification, was explained by both compounds having a >100 times stronger tendency to partition into lipid rather than into organic carbon, while PCB 180 partitions to a similar extent into both matrices.
  •  
25.
  • Kierkegaard, Amelie, et al. (författare)
  • Cyclic volatile methylsiloxanes in fish from the Baltic Sea
  • 2013
  • Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 93:5, s. 774-778
  • Tidskriftsartikel (refereegranskat)abstract
    • Laboratory studies suggest that the cyclic volatile methylsiloxanes (cVMS) octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (05) and dodecamethylcyclohexasiloxane (D6) will persist in the aquatic environment and bioaccumulate in fish. Here these cVMS were measured in herring collected in the Swedish waters of the Baltic Sea and the North Sea and in grey seals from the Baltic Proper. D4, D5, and D6 were present in herring muscle at concentrations around 10, 200, and 40 ng g(-1) lipid weight, respectively. The ratio of these concentrations was similar to the relative magnitude of estimated emissions to water, suggesting that the efficiency of overall transfer through the environment and food web was similar (within a factor 2-3) for the three chemicals. The concentrations of D5 and D6 were similar in herring caught in the highly populated Baltic Proper and in the less populated Bothnian Sea and Bothnian Bay. The D4 concentrations were lower at the most remote northern station, suggesting that D4 is less persistent than D5 and D6. Herring from the North Sea had lower levels of all three chemicals. The concentrations of D4, D5 and D6 in grey seal blubber were lower than the lipid normalized concentrations in herring, indicating that they do not biomagnify in grey seals.
  •  
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