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  • 1.
    Adolfsson-Erici, Margaretha
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Åkerman, Gun
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Internal Benchmarking Improves Precision and Reduces Animal Requirements for Determination of Fish Bioconcentration Factors2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 15, 8205-8211 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 2.
    Adolfsson-Erici, Margaretha
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Åkerman, Gun
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    In-vivo passive sampling to measure elimination kinetics in bioaccumulation tests2012In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 88, no 1, 62-68 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 3.
    Adolfsson-Erici, Margaretha
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Åkerman, Gun
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Measuring bioconcentration factors in fish using exposure to multiple chemicals and internal benchmarking to correct for growth dilution2012In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 31, no 8, 1853-1860 p.Article in journal (Refereed)
    Abstract [en]

    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

  • 4.
    Allmyr, M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Harden, F.
    Toms, L-ML.
    Mueller, J.F.
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Adolfsson-Erici, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Sandborgh Englund, G.
    The influence of age and gender on triclosan concentrations in Australian human blood serum2008In: Sci. Tot. Environ.Article in journal (Refereed)
  • 5.
    Armitage, James M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, Ian T
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance Model2009In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 43, no 4, 1134-1140 p.Article in journal (Refereed)
    Abstract [en]

    The global-scale fate and transport processes of perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted from direct sources were simulated using a multispecies mass balance model over the period 1950 to 2010. The main goal of this study was to assess the atmospheric and oceanic long-range transport potential of direct source emissions and the implications for the contamination of terrestrial and marine systems worldwide. Consistent with previous modeling studies, ocean transport was found to be the dominant pathway for delivering PFO(A) associated with direct sources to the Arctic marine environment, regardless of model assumptions. The modeled concentrations for surface ocean waters were insensitive to assumptions regarding physical−chemical properties and emission mode of entry and were in reasonable agreement with available monitoring data from the Northern Hemisphere. In contrast, model outputs characterizing atmospheric transport potential were highly sensitive to model assumptions, especially the assumed value of the acid dissociation constant (pKa). However, the complete range of model results for scenarios with different assumptions about partitioning and emissions provide evidence that the atmospheric transport of directly emitted PFO(A) can deliver this substance to terrestrial environments distant from sources. Additional studies in remote or isolated terrestrial systems may provide further insight into the scale of contamination actually attributable to direct sources.

  • 6.
    Armitage, James M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wiberg, Karin
    Jonsson, Per
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    A model assessment of polychlorinated dibenzo-p-dioxin and dibenzofuran sources and fate in the Baltic Sea.2009In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 407, no 12, 3784-3792 p.Article in journal (Refereed)
    Abstract [en]

    The contamination of the Baltic Sea with polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) has resulted in restrictions on the marketing and consumption of Baltic Sea fish, making this a priority environmental issue in the European Union. To date there is no consensus on the relative importance of different sources of PCDD/Fs to the Baltic Sea, and hence no consensus on how to address this issue. In this work we synthesized the available information to create a PCDD/F budget for the Baltic Sea, focusing on the two largest basins, the Bothnian Sea and the Baltic Proper. The non-steady state multimedia fate and transport model POPCYCLING-Baltic was employed, using recent data for PCDD/F concentrations in air and sediment as boundary conditions. The PCDD/F concentrations in water predicted by the model were in good agreement with recent measurements. The budget demonstrated that atmospheric deposition was the dominant source of PCDD/Fs to the basins as a whole. This conclusion was supported by a statistical comparison of the PCDD/F congener patterns in surface sediments from accumulation bottoms with the patterns in ambient air, bulk atmospheric deposition, and a range of potential industrial sources. Prospective model simulations indicated that the PCDD/F concentrations in the water column will continue to decrease in the coming years due to the slow response of the Baltic Sea system to falling PCDD/F inputs in the last decades, but that the decrease would be more pronounced if ambient air concentrations were to drop further in the future, for instance as a result of reduced emissions. The study illustrates the usefulness of using monitoring data and multimedia models in an integrated fashion to address complex organic contaminant issues.

  • 7. Arnot, Jon A.
    et al.
    Brown, Trevor N.
    Wania, Frank
    Breivik, Knut
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Prioritizing Chemicals and Data Requirements for Screening-Level Exposure and Risk Assessment2012In: Journal of Environmental Health Perspectives, ISSN 0091-6765, E-ISSN 1552-9924, Vol. 120, no 11, 1565-1570 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 8. Binnington, Matthew J.
    et al.
    Quinn, Cristina L.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wania, Frank
    Evaluating the Effectiveness of Fish Consumption Advisories: Modeling Prenatal, Postnatal, and Childhood Exposures to Persistent Organic Pollutants2014In: Journal of Environmental Health Perspectives, ISSN 0091-6765, E-ISSN 1552-9924, Vol. 122, no 2, 178-186 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 9. Bopp, S.
    et al.
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Schirmer, K.
    (2007): Passive sampler for combined chemical and toxicological long-term monitoring of water: the Ceramic Toximeter2007In: SETAC 17:th Annual Meeting in Europe, Porto, Portugal: 20-24 May, 2007Conference paper (Other (popular science, discussion, etc.))
  • 10. Bopp, S.K.
    et al.
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Schirmer, K.
    Passive sampler for combined chemical and toxicological long-term monitoring of groundwater: the Ceramic Toximeter2007In: Environ. Sci. Technol., Vol. 41, 6868-6876 p.Article in journal (Refereed)
  • 11. Borga, Katrine
    et al.
    Fjeld, Eirik
    Kierkegaard, Amelie
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Consistency in Trophic Magnification Factors of Cyclic Methyl Siloxanes in Pelagic Freshwater Food Webs Leading to Brown Trout2013In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 47, no 24, 14394-14402 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 12. Borga, Katrine
    et al.
    Fjeld, Eirik
    Kierkegaard, Amelie
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Food Web Accumulation of Cyclic Siloxanes in Lake Mjosa, Norway2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 11, 6347-6354 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 13. Breivik, Knut
    et al.
    Czub, Gertje
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wanja, Frank
    Towards an understanding of the link between environmental emissions and human body burdens of PCBs using CoZMoMAN2010In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 36, no 1, 85-91 p.Article in journal (Refereed)
    Abstract [en]

    Different factors affect how organic contaminants released into the environment over time distribute and accumulate, enter various food-chains, and potentially cause toxic effects in wildlife and humans. A sound chemical risk assessment thus requires the determination of the quantitative relationship between emissions and human exposure. This study aimed to assess the extent of the quantitative and mechanistic understanding of the link between environmental emissions and human body burdens for polychlorinated biphenyls (PCBs) in the western part of the Baltic Sea drainage basin and to identify any remaining knowledge gaps. An integrated, non-steady state model calculating human body burden from environmental emissions (CoZMoMAN) was created by linking the multi-compartment environmental fate model CoZMo-POP 2 with the human food chain bioaccumulation model ACC-HUMAN. CoZMoMAN predicted concentrations of seven PCB congeners in 11 key model compartments to typically within a factor of 2 to 4 of measured values, although larger discrepancies are noted for soils and humans. We conclude that whereas the most important processes which link emissions of PCBs to human body burdens are quite well understood in this region, some critical knowledge gaps related to the time trend of historical emissions remain to be addressed.

  • 14.
    Broman, D
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Jonsson, P
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wiberg, K.
    Persson, Y.
    Why do the PCDD/F in Baltic Fish not Decrease - "Old Sins" in Sediments?2008In: 11th International Symposium on the Interactions between Sediment and Water: Esperance, Australia, 17-22 February, 2008Conference paper (Refereed)
  • 15. Chen, Yiqin
    et al.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Kaserzon, Sarit
    Wang, Xianyu
    Weijs, Liesbeth
    Gallen, Michael
    Toms, Leisa-Maree L.
    Li, Yan
    Aylward, Lesa L.
    Sly, Peter D.
    Mueller, Jochen E.
    Monthly variation in faeces: blood concentration ratio of persistent organic pollutants over the first year of life2016In: Environmental Research, ISSN 0013-9351, E-ISSN 1096-0953, Vol. 147, 259-268 p.Article in journal (Refereed)
    Abstract [en]

    Previous studies have found that the concentrations of a range of persistent organic pollutants (POPs) in faeces is linearly proportional to the POP concentrations in blood of human adults irrespective of age and gender. In order to investigate the correlation between POP concentrations in faeces and blood in infants, the monthly variation of POP concentrations in faeces over the first year of life of one infant was investigated in this study and compared to modelled blood concentrations. Faecal samples were collected from one male infant daily. The samples were pooled by month and analysed for three selected POPs (2,2',4,4',5,5'-Hexachlorobiphenyl (PCB153), p,p'-dichlorodiphenyldichloroethylene (p,p'-DDE) and 2,2',4,4'-tetrabromodiphenyl ether (BDE47)). The POP concentrations in faecal samples increased for the first four months by a factor of 2.9, 4.9 and 1.4 for PCB153, BDE47, and p,p'-DDE, respectively. The faecal concentrations of all POPs decreased rapidly following the introduction of formula and solid food to the diet and subsequent weaning of the infant. Further, a one-compartment model was developed to estimate the daily POP concentrations in the blood of the infant. The POP concentrations in blood were predicted to vary much less over the first year than those observed in faeces. The faeces:blood concentration ratio of selected POPs (K-fb) differed significantly (P < 0.0001) between the period before and after weaning, and observed changes in K-fb are far greater than the uncertainty in the estimated K-fb. A more stable K-fb after weaning indicates the possibility of applying the stable K-fb values for non-invasive assessment of internal exposure in infants after weaning. The intra-individual variation in K-fb in infants is worthy of further investigation.

  • 16. Chen, Yiqin
    et al.
    Sjodin, Andreas
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    English, Karin
    Aylward, Lesa L.
    Toms, Leisa-Maree L.
    Varghese, Julie
    Sly, Peter D.
    Mueller, Jochen F.
    Persistent organic pollutants in infants and toddlers: Relationship between concentrations in matched plasma and faecal samples2017In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 107, 82-88 p.Article in journal (Refereed)
    Abstract [en]

    Early-childhood biomonitoring of persistent organic pollutants (POPs) is challenging due to the logistic and ethical limitations associated with blood sampling. We investigated using faeces as a non-invasive matrix to estimate internal exposure to POPs. The concentrations of selected POPs were measured in matched plasma and faecal samples collected from 20 infants/toddlers (aged 13 +/- 4.8 months), including a repeat sample time point for 13 infants (similar to 5 months apart). We observed higher rates of POP quantification in faeces (2 g dry weight) than in plasma (0.5 mL). Among the five chemicals that had quantification frequencies over 50% in both matrices, except for HCB, log concentration in faeces (C-f) and blood (C-b) were correlated (r > 0.74, P < 0.05) for p.p'-dichlorodiphenyldichloroethylene (p,p'-DDE), 2,3', 4,4', 5-pentachlorobiphenyl (PCB118), 2,2', 3,4,4', 5'-pentachlorobiphenyl (PCB138) and 2,2', 4,4', 5,5'-pentachlorobiphenyl (PCB153). We determined faeces: plasma concentration ratios (K-fb), which can be used to estimate C-b from measurements of C-f for infants/toddlers. For a given chemical, the variation in K-fb across individuals was considerable (CV from 0.46 to 0.70). Between 5% and 50% of this variation was attributed to short-term intra-individual variability between successive faecal samples. This variability could be reduced by pooling faeces samples over several days. Some of the remaining variability was attributed to longer-term intra-individual variability, which was consistent with previously reported observations of a decrease in K-fb over the first year of life. The strong correlations between C-f and C-b demonstrate the promise of using faeces for biomonitoring of these compounds. Future research on the sources of variability in K-fb could improve the precision and utility of this technique.

  • 17. Chen, Yiqin
    et al.
    Wang, Xianyu
    Li, Yan
    Toms, Leisa-Maree L.
    Gallen, Michael
    Hearn, Laurence
    Aylward, Lesa L.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Sly, Peter D.
    Mueller, Jochen F.
    Persistent organic pollutants in matched breast milk and infant faeces samples2015In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 118, 309-314 p.Article in journal (Refereed)
    Abstract [en]

    Assessing blood concentration of persistent organic pollutants (POPs) in infants is difficult due to the ethical and practical difficulties in obtaining sufficient quantities of blood. To determine whether measuring POPs in faeces might reflect blood concentration during infancy, we measured the concentrations of a range of POPs (i.e. polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs)) in a pilot study using matched breast milk and infant faecal samples obtained from ten mother-child pairs. All infants were breast fed, with 8 of them also receiving solid food at the time of faecal sampling. In this small dataset faecal concentrations (range 0.01-41 ng g(-1) lipid) are strongly associated with milk concentrations (range 0.02-230 ng g(-1) lipid). Associations with other factors generally could not be detected in this dataset, with the exception of a small effect of age or growth. Different sources (external or internal) of exposure appeared to directly influence faecal concentrations of different chemicals based on different inter-individual variability in the faeces-to-milk concentration ratio R-fm. Overall, the matrix of faeces as an external measure of internal exposure in infants looks promising for some chemicals and is worth assessing further in larger datasets.

  • 18. Clift, Roland
    et al.
    Sim, Sarah
    King, Henry
    Chenoweth, Jonathan L.
    Christie, Ian
    Clavreul, Julie
    Mueller, Carina
    Posthuma, Leo
    Boulay, Anne-Marie
    Chaplin-Kramer, Rebecca
    Chatterton, Julia
    DeClerck, Fabrice
    Druckman, Angela
    France, Chris
    Franco, Antonio
    Gerten, Dieter
    Goedkoop, Mark
    Hauschild, Michael Z.
    Huijbregts, Mark A. J.
    Koellner, Thomas
    Lambin, Eric F.
    Lee, Jacquetta
    Mair, Simon
    Marshall, Stuart
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mila i Canals, Llorenc
    Mitchell, Cynthia
    Price, Edward
    Rockstrom, Johan
    Stockholm University, Faculty of Science, Stockholm Resilience Centre.
    Suckling, James
    Murphy, Richard
    The Challenges of Applying Planetary Boundaries as a Basis for Strategic Decision-Making in Companies with Global Supply Chains2017In: Sustainability, ISSN 2071-1050, E-ISSN 2071-1050, Vol. 9, no 2, 279Article in journal (Refereed)
    Abstract [en]

    The Planetary Boundaries (PB) framework represents a significant advance in specifying the ecological constraints on human development. However, to enable decision-makers in business and public policy to respect these constraints in strategic planning, the PB framework needs to be developed to generate practical tools. With this objective in mind, we analyse the recent literature and highlight three major scientific and technical challenges in operationalizing the PB approach in decision-making: first, identification of thresholds or boundaries with associated metrics for different geographical scales; second, the need to frame approaches to allocate fair shares in the 'safe operating space' bounded by the PBs across the value chain and; third, the need for international bodies to co-ordinate the implementation of the measures needed to respect the Planetary Boundaries. For the first two of these challenges, we consider how they might be addressed for four PBs: climate change, freshwater use, biosphere integrity and chemical pollution and other novel entities. Four key opportunities are identified: (1) development of a common system of metrics that can be applied consistently at and across different scales; (2) setting 'distance from boundary' measures that can be applied at different scales; (3) development of global, preferably open-source, databases and models; and (4) advancing understanding of the interactions between the different PBs. Addressing the scientific and technical challenges in operationalizing the planetary boundaries needs be complemented with progress in addressing the equity and ethical issues in allocating the safe operating space between companies and sectors.

  • 19.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Wang, Zhanyun
    Scheringer, Martin
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    The precautionary principle and chemicals management: The example of perfluoroalkyl acids in groundwater2016In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 94, 331-340 p.Article, review/survey (Refereed)
    Abstract [en]

    Already in the late 1990s microgram-per-liter levels of perfluorooctane sulfonate (PFOS) were measured in water samples from areas where fire-fighting foams were used or spilled. Despite these early warnings, the problems of groundwater, and thus drinking water, contaminated with perfluoroalkyl and polyfluoroalkyl substances (PFASs) including PFOS are only beginning to be addressed. It is clear that this PFAS contamination is poorly reversible and that the societal costs of clean-up will be high. This inability to reverse exposure in a reasonable timeframe is a major motivation for application of the precautionary principle in chemicals management. We conclude that exposure can be poorly reversible; 1) due to slow elimination kinetics in organisms, or 2) due to poorly reversible environmental contamination that leads to continuous exposure. In the second case, which is relevant for contaminated groundwater, the reversibility of exposure is not related to the magnitude of a chemical's bioaccumulation potential. We argue therefore that all PFASs entering groundwater, irrespective of their perfluoroalkyl chain length and bioaccumulation potential, will result in poorly reversible exposures and risks as well as further clean-up costs for society. To protect groundwater resources for future generations, society should consider a precautionary approach to chemicals management and prevent the use and release of highly persistent and mobile chemicals such as PFASs. (C) 2016 Elsevier Ltd. All rights reserved.

  • 20.
    Czub,
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Are dietary consumption guidelines effective at reducing exposure of nursing infants to POPs?2007In: SETAC 17:th Annual Meeting in Europe, Porto, Portugal: 20-24 May, 2007Conference paper (Other (popular science, discussion, etc.))
  • 21.
    Czub,
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Undeman,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Human exposure to environmental contaminants: Modelling the food chain2007In: Eurotox 2007, Amsterdam, The Netherlands: 7-10 October, 2007, S12-S13 p.Conference paper (Other (popular science, discussion, etc.))
  • 22.
    Czub, G
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wania, F.
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Combining Long-Range Transport and Bioaccumulation Considerations to Identify Potential Arctic Contaminants2008In: Environ. Sci. Technol., Vol. 42, 3704-3709 p.Article in journal (Refereed)
  • 23.
    Czub, Gertje
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Influence of the temperature gradient in blubber on the bioaccumulation of persistent lipophilic organic chemicals in seals2007In: Environ. Toxicol. Chem., Vol. 26, 1600-1605 p.Article in journal (Refereed)
  • 24. de Voogt, P.
    et al.
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    de Coen, W.
    de Wolf, W.
    Helmstad, E.
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    van Leeuwen, S.
    van Roon, A.
    PERFORCE: Perfluorinated Organic Compounds in the European Environment2007In: Organohalogen Compd., Vol. 69, 153-156 p.Article in journal (Refereed)
  • 25.
    Egebäck,
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Sellström,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Particle size distribution of airborne PBDEs2007In: SETAC Europe 17th Annual Meeting: 20-24 May 2007, 2007Conference paper (Other (popular science, discussion, etc.))
  • 26. Felizeter, Sebastian
    et al.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    De Voogt, Pim
    Root Uptake and Trans location of Perfluorinated Alkyl Acids by Three Hydroponically Grown Crops2014In: Journal of Agricultural and Food Chemistry, ISSN 0021-8561, E-ISSN 1520-5118, Vol. 62, no 15, 3334-3342 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 27. Felizeter, Sebastian
    et al.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    de Voogt, Pim
    Uptake of Perfluorinated Alkyl Acids by Hydroponically Grown Lettuce (Lactuca sativa)2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 21, 11735-11743 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 28. Fiedler, H.
    et al.
    Harner, T.
    Kallenborn, R.
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Shibata, Y.
    Wania, F.
    Weiss, P.
    Zhang, M.
    Global monitoring of persistent organic pollutants in air – First observations and future challenges.2008In: Organohalogen. Compd. 70: Dioxin 2008, Birmingham, UK, 2008Conference paper (Refereed)
  • 29.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Laudon, Hjalmar
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mass Balance of Perfluorinated Alkyl Acids (PFAAs) in a Pristine Boreal CatchmentManuscript (preprint) (Other academic)
    Abstract [en]

    Mass balances of ten individual PFAAs in two nested pristine catchments in Northern Sweden with different sizes and hydrological functions were assembled for 2011-2012. Concentrations of PFAAs in rain and snowmelt, as well as in stream water at the outlet of the two watersheds were measured and used to calculate PFAA inputs and outputs to the catchments. The results generally showed a great excess of PFAA inputs for both catchments. During spring flow the stream water showed PFAA patterns resembling the patterns in rain (as opposed to snowmelt) and the mass balances were roughly closed for several PFAAs, suggesting that snowmelt water infiltrating the ground had displaced water from the previous summer. Comparison of PFAA mass balances between the two catchments further suggested that atmospheric inputs of short-chain (replacement) perfluoroalkyl carboxylic acids had increased in the years before sampling, while inputs of the legacy perfluorooctane sulfonic acid had decreased. The overall positive mass balances indicate that a considerable portion of the PFAAs deposited from the atmosphere are stored in soil and may be released to surface and marine water environments in the future.

  • 30.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Laudon, Hjalmar
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Helmholtz Centre for Environmental Research—UFZ, Germany.
    Mass Balance of Perfluorinated Alkyl Acids in a Pristine Boreal Catchment2015In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 20, 12127-12135 p.Article in journal (Refereed)
    Abstract [en]

    Mass balances of ten individual perfluorinated alkyl acids (PFAAs) in two nested pristine catchments in Northern Sweden with different sizes and hydrological functions were assembled for 2011-2012. Concentrations of PFAAs in rain and snowmelt, as well as in streamwater at the outlet of the two watersheds were measured and used to calculate PFAA atmospheric inputs to and riverine outputs from the catchments. The results generally showed a great excess of PFAA inputs for both catchments over the whole study year. However, during the spring flood period, the inputs and outputs were within a factor of 2 for several PFAAs and the streamwater showed PFAA patterns resembling the patterns in rain (as opposed to snowmelt), suggesting that snowmelt water infiltrating the ground had displaced water from the previous summer. Comparison of PFAA mass balances between the two catchments further suggested that atmospheric inputs of short-chain (replacement) perfluoroalkyl carboxylic acids had increased in the years before sampling, while inputs of the legacy perfluorooctane sulfonic acid had decreased. Overall, the mass balances indicate that a considerable portion of the PFAAs deposited from the atmosphere are stored in soil and may be released to surface and marine water environments in the future.

  • 31.
    Fridén, Ulrika E.
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Järnberg, Ulf
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Chlorinated paraffins in the Swedish atmosphere: spatial and seasonal variabilityManuscript (preprint) (Other academic)
    Abstract [en]

    Chlorinated paraffins (CPs) are ubiquitous environmental contaminants of concern, as indicated by the recent addition of the short-chained CPs as a new Persistent Organic Pollutant (POP) in the United Nations Eco-nomic Commission for Europe (UNECE) Convention on Long-Range Transboundary Air Pollution (CLRTAP) (United Nations, 2010). Howev-er, knowledge about the occurrence of CPs in the environment, and in the atmosphere in particular, is limited. To address this, ambient air samples were collected over a 10 month period at an urban site and a rural site in Sweden, and analyzed for the sum of the short-chained, me-dium-chained and long-chained CPs. The CP concentrations ranged from 0.7-33 ng/m3, and they were significantly higher at the urban site. The low volatile CP congeners dominated in the samples, and this domin-ance was more pronounced at the urban site. Particle-bound and ga-seous CPs were determined separately in several samples, and between 50 and 90 % of the CPs were estimated to be in the gas phase. A clear seasonality in the concentrations was observed, with levels in summer that were about 5 times higher than in winter. This indicates that tem-perature dependent emission from urban sources is a major source of the CPs in air. Diffusive emissions from building materials are likely to make a major contribution.

  • 32.
    Fridén, Ulrika E.
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Chlorinated paraffins in indoor air and dust: Concentrations, congener patterns, and human exposure2011In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 37, no 7, 1169-1174 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 33.
    Fridén, Ulrika E.
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Sörme, Louise
    Regions and Environment Department, Statistics Sweden.
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Emissions of chlorinated paraffins in Stockholm: A substance flow analysis studyManuscript (preprint) (Other academic)
    Abstract [en]

    Chlorinated paraffins (CPs) are currently under consideration for classi-fication as persistent organic pollutants. They have been extensively used for many decades in a wide range of applications, particularly in industrial lubricants and building materials. However, very little is known about their levels in the technosphere or about the origins and quantities of their emission into the environment. In this study, sub-stance flow analysis was used to estimate CP emissions from the city of Stockholm, Sweden to different environmental media. The results indi-cate that 16 tonnes of CPs are added to the technosphere in Stockholm annually, and that approximately 0.5 tonnes are emitted to air and wa-ter annually. The estimated emissions to air and water were in reasona-ble agreement with independent emission estimates derived from envi-ronmental monitoring data. The emissions are not directly linked to the annual inflow; instead, they largely originate from the large quantity of CPs that have accumulated in the technosphere over many years. The main sources of the emissions are in-place paints and sealants. The vast majority of the CPs are expected to leave the technosphere as solid waste, but there are uncertainties regarding subsequent CP emissions from solid waste into the environment.

  • 34.
    Fridén, Ulrika
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Substansflödesanalys av klorparaffiner i Stockholms stad 20042007Report (Other (popular science, discussion, etc.))
  • 35.
    Fridén, Ulrika
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Emissions of Chlorinated Paraffins in Stockholm: A Chemical Flow Analysis Study2007In: Organohalogen Compounds, Vol. 69, 2615-2617 p.Article in journal (Refereed)
    Abstract [en]

    Chlorinated paraffins are currently under consideration for classification as POPs. They have been used for many decades, particularly in industrial lubricants and different building materials, but there is very little information available on their inventories in the technosphere and their emissions to the environment. In this study a chemical flow analysis was conducted for the city of Stockholm with the goals of estimating the current emissions of CPs to different environmental media. The results indicate that approximately 0.5 tonnes of CP are released to air and water in Stockholm annually, with paints and sealants being the major sources. The vast majority of the CPs are expected to end as solid waste, but there are uncertainties regarding their ongoing leakage into the environment.

  • 36.
    Jahnke, A
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mayer, P.
    Equilibrium sampling: Partitioning of organochlorine compounds from lipids into polydimethylsiloxane2008In: Chemosphere, Vol. 73, 1575-1581 p.Article in journal (Refereed)
  • 37.
    Jahnke, A
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mayer, P.
    Broman, D
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    In tissue equilibrium sampling of polychlorinated biphenyls in freshwater fish and fish from the Baltic Sea.2008In: 18th Annual Meeting of SETAC-Europe: Warsaw, Poland, 25-29 May, 2008Conference paper (Refereed)
  • 38.
    Jahnke, Annika
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mayer, Philipp
    Adolfsson-Erici, Margaretha
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    EQUILIBRIUM SAMPLING OF ENVIRONMENTAL POLLUTANTS IN FISH: COMPARISON WITH LIPID-NORMALIZED CONCENTRATIONS AND HOMOGENIZATION EFFECTS ON CHEMICAL ACTIVITY2011In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 30, no 7, 1515-1521 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 39.
    Jahnke, Annika
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mayer, Philipp
    Broman, Dag
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Possibilities and limitations of equilibrium sampling using polydimethylsiloxane in fish tissue.2009In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 77, no 6, 764-70 p.Article in journal (Refereed)
    Abstract [en]

    Polydimethylsiloxane (PDMS) has been used for passive equilibrium sampling in numerous abiotic environmental matrices. Recently, this approach was extended to lipid-rich tissue. This work investigated the possibilities and limitations of using PDMS thin-film extraction for in tissue equilibrium sampling in fish species of varying lipid content. Polychlorinated biphenyls (PCBs) were used as model lipophilic organic pollutants. PDMS thin-films were inserted in intact fish tissue for differing time periods (1h up to 1 week). The thin-films were then solvent-extracted and the extracts were analyzed using gas chromatography coupled to mass spectrometry. Whether equilibrium had been established was investigated either by using PDMS thin-films of multiple thicknesses (140-620 microm) or by assessing kinetics by means of time series. Equilibration was found to be rapid (i.e. in the range of hours) in lipid-rich fish whereas equilibrium was not achieved within one week in tissues with low or medium lipid content (i.e. up to 2% lipids). Regarding lipid-rich fish, the newly developed method was found to be sufficiently sensitive to determine equilibrium partitioning concentrations of PCBs in lipids of samples from the Baltic Sea, and it is a promising approach for any kind of fatty tissue.

  • 40.
    Jahnke, Annika
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mayer, Philipp
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Sensitive equilibrium sampling to study polychlorinated biphenyl disposition in Baltic Sea sediment2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 18, 10114-10122 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 41.
    Jahnke, Annika
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mayer, Philipp
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wickström, Håkan
    Gilbert, Dorothea
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Silicone passive equilibrium samplers as 'chemometers' in eels and sediments of a Swedish lake2014In: Environmental Science Processes and Impacts, ISSN 2050-7887, Vol. 16, no 3, 464-472 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 42.
    Kierkegaard, A
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Adolfsson-Erici, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    A Sensitive Method for the Analysis of Decamethylcyclopentasiloxane (D5) in Biota2008In: SETAC North America 29th Annual Meeting: 16-20 November, 2008Conference paper (Refereed)
  • 43.
    Kierkegaard, A
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Adolfsson-Erici, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Decamethylcyclopentasiloxane (D5) Concentrations in Fish from Urban and Remote Lakes in Sweden2008In: SETAC North America 29th Annual Meeting: 16-20 November, 2008Conference paper (Refereed)
  • 44.
    Kierkegaard, Amelie
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Asplund, Lillemor
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    de Wit, Cynthia
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Thomas, G.O.
    Sweetman, A.J.
    Jones, K.C.
    Fate of Higher Brominated PBDEs in Lactating Cows2007In: Environ. Sci. Technol., Vol. 41, 417-423 p.Article in journal (Refereed)
  • 45.
    Kierkegaard, Amelie
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    De Wit, Cynthia A
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Asplund, Lillemor
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Thomas, Gareth O
    Sweetman, Andrew J
    Jones, Kevin C
    A mass balance of tri-hexabrominated diphenyl ethers in lactating cows.2009In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 43, no 7, 2602-2607 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 46.
    Kierkegaard, Amelie
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Determination of decamethylcyclopentasiloxane in air using commercial solid phase extraction cartridges2010In: Journal of Chromatography A, ISSN 0021-9673, E-ISSN 1873-3778, Vol. 1217, no 21, 3557-3560 p.Article in journal (Refereed)
    Abstract [en]

    Decamethylcyclopentasiloxane (D-5), a high production volume chemical used in personal care products. has been designated for regulation in Canada and is under review in the EU because of concerns about its persistence and potential for bioaccumulation in the environment. D-5 is a volatile compound expected to be found primarily in air, but there is little information on atmospheric concentrations due to the lack of sensitive analytical methods. Here a simple and sensitive method to determine D-5 in ambient air is presented. The challenge in the environmental analysis of D-5 is avoiding contamination. Our method is based on the high trapping efficiency of the sorbent [solute ENV+, combined with a comparably high sampling rate. A small amount of sorbent (10 mg) is eluted in a small volume of n-hexane (0.1-0.6 mL). which is injected onto a GC/MS system without further processing. The simplicity of the method enables the use of a field blank for every sample to trace contamination. The method provides low limits of quantification (similar to 0.3 ng/m(3)), good repeatability and limited breakthrough (similar to 1%). By lowering the limit of quantification compared to published work by almost two orders of magnitude, it became possible to quantify D5 in ambient air at locations remote from strong point sources. The concentrations at a rural Swedish site ranged from 0.7 to 8 ng/m(3) over a period of 4 months.

  • 47.
    Kierkegaard, Amelie
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Determination of linear and cyclic volatile methylsiloxanes in air at a regional background site in Sweden2013In: Atmospheric Environment, ISSN 1352-2310, E-ISSN 1873-2844, Vol. 80, 322-329 p.Article in journal (Refereed)
    Abstract [en]

    A number of volatile methylsiloxanes have been identified as environmental contaminants and several are currently the subject of detailed risk assessments due to concerns that they may be persistent, bioaccumulative and toxic in the environment. Once emitted these chemicals reside primarily in the atmosphere. Consequently, knowledge of their concentrations in air is essential to understanding their fate in the environment and any potential adverse impacts. We developed a method to analyse 4 cyclic volatile methylsiloxanes (D3, D4, D5 and D6) and 4 linear volatile methylsiloxanes (L3, L4, L5 and L6) in air at regional background levels. The method showed good repeatability (median difference between sample pairs of 2-8%) and low limits of quantification (from 3.8 pg m(-3) for L3 to 320 pg m(-3) for D4). However, the analysis of D3 and D4 was confounded by the transformation of D5 to these analytes on the sampling cartridge. During a sampling campaign with a daily temporal resolution between November 4 and December 14 2011, all analytes with the exception of L5 and L6 could be quantified in all samples. It was hypothesized that the ratio of the concentrations of different VMS reflected the relative strength of their emissions to the airshed due to the slow phototransformation of the VMS at high latitudes in winter. This was supported by available emissions information.

  • 48.
    Kierkegaard, Amelie
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Sellström, Ulla
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Environmental analysis of higher brominated diphenyl ethers and decabromodiphenyl ethane.2009In: Journal of Chromatography A, ISSN 0021-9673, E-ISSN 1873-3778, Vol. 1216, no 3, 364-375 p.Article in journal (Refereed)
    Abstract [en]

    Methods for environmental analysis of higher brominated diphenyl ethers (PBDEs), in particular decabromodiphenyl ether (BDE209), and the recently discovered environmental contaminant decabromodiphenyl ethane (deBDethane) are reviewed. The extensive literature on analysis of BDE209 has identified several critical issues, including contamination of the sample, degradation of the analyte during sample preparation and GC analysis, and the selection of appropriate detection methods and surrogate standards. The limited experience with the analysis of deBDethane suggests that there are many commonalities with BDE209. The experience garnered from the analysis of BDE209 over the last 15 years will greatly facilitate progress in the analysis of deBDethane.

  • 49.
    Kierkegaard, Amelie
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    van Egmond, Roger
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cyclic Volatile Methylsiloxane Bioaccumulation in Flounder and Ragworm in the Humber Estuary2011In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 45, no 14, 5936-5942 p.Article in journal (Refereed)
    Abstract [en]

    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.

  • 50. MacLeod, M.
    et al.
    Arnot, J.
    McLachlan, M
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wania, F.
    Tracking the sources, transport and fate of persistent pollutants at regional, continental and global scales.2008In: ISEA Special Symposium: Characterizing Global Exposures to POPs: The Role of Models: Pasadena, 12-16 October, 2008Conference paper (Refereed)
123 1 - 50 of 107
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