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  • 1.
    Benskin, Jonathan P.
    et al.
    Univ Alberta, Dept Lab Med & Pathol, Edmonton, AB, Canada..
    Ahrens, Lutz
    Helmholtz Zentrum Geesthacht, Inst Coastal Res, Geesthacht, Germany..
    Muir, Derek C. G.
    Environm Canada, Aquat Ecosyst Protect Res Div, Water Sci & Technol Directorate, Burlington, ON L7R 4A6, Canada..
    Scott, Brian F.
    Environm Canada, Aquat Ecosyst Protect Res Div, Water Sci & Technol Directorate, Burlington, ON L7R 4A6, Canada..
    Spencer, Christine
    Environm Canada, Aquat Ecosyst Protect Res Div, Water Sci & Technol Directorate, Burlington, ON L7R 4A6, Canada..
    Rosenberg, Bruno
    Fisheries & Oceans Canada, Arctic Aquat Res Div, Winnipeg, MB, Canada..
    Tomy, Gregg
    Fisheries & Oceans Canada, Arctic Aquat Res Div, Winnipeg, MB, Canada..
    Kylin, Henrik
    Linkoping Univ, Dept Water & Environm Studies, S-58183 Linkoping, Sweden..
    Lohmann, Rainer
    Univ Rhode Isl, Grad Sch Oceanog, Narragansett, RI 02882 USA..
    Martin, Jonathan W.
    Univ Alberta, Dept Lab Med & Pathol, Edmonton, AB, Canada..
    Manufacturing Origin of Perfluorooctanoate (PFOA) in Atlantic and Canadian Arctic Seawater2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 2, p. 677-685Article in journal (Refereed)
    Abstract [en]

    The extent to which different manufacturing sources and long-range transport pathways contribute to perfluorooctanoate (PFOA) in the world's oceans, particularly in remote locations, is widely debated. Here, the relative contribution of historic (i.e., electrochemically fluorinated) and contemporary (i.e., telomer) manufacturing sources was assessed for PFOA, in various seawater samples by an established isomer profiling technique. The ratios of individual branched PFOA isomers were indistinguishable from those in authentic historic standards in 93% of the samples examined, indicating that marine processes had little influence on isomer profiles, and that isomer profiling is a valid source apportionment tool for seawater. Eastern Atlantic PFOA was largely (83-98%) of historic origin, but this decreased to only 33% close to the Eastern U.S. seaboard. Similarly, PFOA in the Norwegian Sea was near exclusively historic, but the relative contribution decreased to similar to 50% near the Baltic Sea. Such observations of contemporary PFOA in coastal source regions coincided with elevated concentrations, suggesting that the continued production and use of PFOA is currently adding to the marine burden of this contaminant. In the Arctic, a spatial trend was observed whereby PFOA in seawater originating from the Atlantic was predominantly historic (up to 99%), whereas water in the Archipelago (i.e., from the Pacific) was predominantly of contemporary origin (as little as 17% historic). These data help to explain reported temporal and spatial trends from Arctic wildlife biomonitoring, and suggest that the dominant PFOA source(s) to the Pacific and Canadian Arctic Archipelago are either (a) from direct emissions of contemporary PFOA via manufacturing or use in Asia, or (b) from atmospheric transport and oxidation of contemporary PFOA-precursors.,

  • 2.
    Benskin, Jonathan P.
    et al.
    Univ Alberta, Dept Lab Med & Pathol, Edmonton, AB T6G 2G3, Canada..
    Muir, Derek C. G.
    Environm Canada, Aquat Contaminants Res Div, Burlington, ON L7R 4A6, Canada..
    Scott, Brian F.
    Environm Canada, Aquat Contaminants Res Div, Burlington, ON L7R 4A6, Canada..
    Spencer, Christine
    Environm Canada, Aquat Contaminants Res Div, Burlington, ON L7R 4A6, Canada..
    De Silva, Amila O.
    Environm Canada, Aquat Contaminants Res Div, Burlington, ON L7R 4A6, Canada..
    Kylin, Henrik
    Linkoping Univ, Dept Water & Environm Studies, SE-58183 Linkoping, Sweden..
    Martin, Jonathan W.
    Univ Alberta, Dept Lab Med & Pathol, Edmonton, AB T6G 2G3, Canada..
    Morris, Adam
    Univ Guelph, Dept Environm Biol, Guelph, ON N1G 2W1, Canada..
    Lohmann, Rainer
    Univ Rhode Isl, Grad Sch Oceanog, Narragansett, RI 02882 USA..
    Tomy, Gregg
    Dept Fisheries & Oceans Canada, Arctic Aquat Res Div, Winnipeg, MB R3T 2N6, Canada..
    Rosenberg, Bruno
    Dept Fisheries & Oceans Canada, Arctic Aquat Res Div, Winnipeg, MB R3T 2N6, Canada..
    Taniyasu, Sachi
    Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058569, Japan..
    Yamashita, Nobuyoshi
    Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058569, Japan..
    Perfluoroalkyl Acids in the Atlantic and Canadian Arctic Oceans2012In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 46, no 11, p. 5815-5823Article in journal (Refereed)
    Abstract [en]

    We report here on the spatial distribution of C-4, C-6, and C-8 perfluoroalkyl sulfonates, C-6-C-14 perfluoroalkyl carboxylates, and perfluorooctanesulfonamide in the Atlantic and Arctic Oceans, including previously unstudied coastal waters of North and South America, and the Canadian Arctic Archipelago. Perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS) were typically the dominant perfluoroalkyl acids (PFAAs) in Atlantic water. In the midnorthwest Atlantic/Gulf Stream, sum PFAA concentrations (Sigma PFAAs) were low (77-190 pg/L) but increased rapidly upon crossing into U.S. coastal water (up to 5800 pg/L near Rhode Island). Sigma PFAAs in the northeast Atlantic were highest north of the Canary Islands (280-980 pg/L) and decreased with latitude. In the South Atlantic, concentrations increased near Rio de la Plata (Argentina/Uruguay; 350-540 pg/L Sigma PFAAs), possibly attributable to insecticides containing N-ethyl perfluorooctanesulfonamide, or proximity to Montevideo and Buenos Aires. In all other southern hemisphere locations, Sigma PFAAs were <210 pg/L. PFOA/PFOS ratios were typically >= 1 in the northern hemisphere, similar to 1 near the equator, and <= 1 in the southern hemisphere. In the Canadian Arctic, Sigma PFAAs ranged from 40 to 250 pg/L, with perfluoroheptanoate, PFOA, and PFOS among the PFAAs detected at the highest concentrations. PFOA/PFOS ratios (typically >>1) decreased from Baffin Bay to the Amundsen Gulf; possibly attributable to increased atmospheric inputs. These data help validate global emissions models and contribute to understanding of long-range transport pathways and sources of PFAAs to remote regions.

  • 3.
    Jantunen, Liisa M.
    et al.
    Environm Canada, Ctr Atmospher Res Expt, Egbert, ON L0L 1N0, Canada..
    Helm, Paul A.
    Univ Toronto, Toronto, ON M5S 3E5, Canada..
    Kylin, Henrik
    Norwegian Inst Air Res, Polar Environm Ctr, NO-9296 Tromso, Norway.;Swedish Univ Agr Sci, Dept Environm Assessment, SE-70507 Uppsala, Sweden..
    Bidlemant, Terry F.
    Environm Canada, Ctr Atmospher Res Expt, Egbert, ON L0L 1N0, Canada..
    Hexachlorocyclohexanes (HCHs) in the Canadian archipelago. 2. Air-water gas exchange of alpha- and gamma-HCH2008In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 42, no 2, p. 465-470Article in journal (Refereed)
    Abstract [en]

    Air and water were sampled in the Canadian Archipelago during summer on the Tundra Northwest 1999 (TNW-99) expedition and air was sampled at Resolute Bay (1313), Nunavut, to determine the gas exchange of a-and gamma-hexachlorocyclohexanes (HCHs) and the enantiomers of alpha-HCH. Air concentrations of Sigma HCH during TNW-99 and at RB were similar, averaging 55 and. 53 pg m(-3), respectively. The net gas exchange direction was volatilization for alpha-HCH and near equilibrium or deposition for gamma-HCH, whereas actual fluxes depended on the fraction of open water. Enantiomer fractions, EF = (+)/[(+) + (-)] of alpha-HCH in air sampled from shipboard were significantly correlated to those in surface water for events with >90% open water, but were closer to racemic and not correlated to EFs in water for events with 0-50% open water. Levels of alpha-HCH in air at RB averaged 37 9 pg m(-3) from June to early July, and EFs were close to racemic (0.496 +/- 0.004). In mid-July the ice pack broke up around RB. From this point through August, air concentrations increased significantly to 53 +/- 5 pg m(-3), and the mean EF decreased significantly to 0.483 +/- 0.009. Air concentrations of gamma-HCH at RB did not differ significantly before (8.0 +/- 3.7 pg m(-3)) and after (6.6 +/- 0.76 pg m(-3)) ice breakup. Results show that a-HCH enantiomers are sensitive tracers for following the impact of ice cover loss on gas exchange in the Arctic.

  • 4.
    Jantunen, Liisa
    et al.
    Environment Canada, Canada.
    Wong, Fiona
    Stockholm University.
    Gawor, Anya
    Environment Canada.
    Kylin, Henrik
    Linköpings universitet, Tema Miljöförändring.
    Helm, Paul
    Ontario Ministry of the Environment, Canada.
    Stern, Gary
    University of Manitoba, Canada.
    Strachan, William
    Environment Canada, Canada.
    Burniston, Deborah
    Environment Canada, Canada.
    Bidleman, Terry
    Umeå University.
    20 Years of Air-Water Gas Exchange Observations for Pesticides in the Western Arctic Ocean2015In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 23, p. 13844-13852Article in journal (Refereed)
    Abstract [en]

    The Arctic has been contaminated by legacy organochlorine pesticides (OCPs) and currently used pesticides (CUPs) through atmospheric transport and oceanic currents. Here we report the time trends and air−water exchange of OCPs and CUPs from research expeditions conducted between 1993 and 2013. Compounds determined in both air and water were trans- and cis-chlordanes (TC, CC), trans- and cis-nonachlors (TN, CN), heptachlor exo-epoxide (HEPX), dieldrin (DIEL), chlorobornanes (ΣCHBs and toxaphene), dacthal (DAC), endosulfans and metabolite endosulfan sulfate (ENDO-I, ENDO-II, and ENDO SUL), chlorothalonil (CHT), chlorpyrifos (CPF), and trifluralin (TFN). Pentachloronitrobenzene (PCNB and quintozene) and its soil metabolite pentachlorothianisole (PCTA) were also found in air. Concentrations of most OCPs declined in surface water, whereas some CUPs increased (ENDO-I, CHT, and TFN) or showed no significant change (CPF and DAC), and most compounds declined in air. Chlordane compound fractions TC/(TC + CC) and TC/(TC + CC + TN) decreased in water and air, while CC/(TC + CC + TN) increased. TN/(TC + CC + TN) also increased in air and slightly, but not significantly, in water. These changes suggest selective removal of more labile TC and/or a shift in chlordane sources. Water−air fugacity ratios indicated net volatilization (FR > 1.0) or near equilibrium (FR not significantly different from 1.0) for most OCPs but net deposition (FR < 1.0) for ΣCHBs. Net deposition was shown for ENDO-I on all expeditions, while the net exchange direction of other CUPs varied. Understanding the processes and current state of air−surface exchange helps to interpret environmental exposure and evaluate the effectiveness of international protocols and provides insights for the environmental fate of new and emerging chemicals.

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