| 1. |
- Benskin, Jonathan, et al.
(författare)
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Manufacturing Origin of Perfluorooctanoate (PFOA) in Atlantic and Canadian Arctic Seawater
- 2012
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:2, s. 677-685
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Tidskriftsartikel (refereegranskat)abstract
- 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 ∼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.
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| 2. |
- Benskin, Jonathan P., et al.
(författare)
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Perfluoroalkyl Acids in the Atlantic and Canadian Arctic Oceans
- 2012
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Ingår i: Environmental Science and Technology. - : American Chemical Society. - 0013-936X .- 1520-5851. ; 46:11, s. 5815-5823
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Tidskriftsartikel (refereegranskat)abstract
- 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 less than210 pg/L. PFOA/PFOS ratios were typically greater than= 1 in the northern hemisphere, similar to 1 near the equator, and less than= 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 greater thangreater than1) 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.
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| 3. |
- Bidleman, Terry Frank, et al.
(författare)
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Scavenging amphipods : sentinels for penetration of mercury and persistent organic chemicals into food webs of the deep arctic ocean
- 2013
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Ingår i: Environmental Science and Technology. - Washington : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:11, s. 5553-5561
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Tidskriftsartikel (refereegranskat)abstract
- Archived specimens of the scavenging amphipod Eurythenes gryllus, collected from 2075 to 4250 m below the surface on five expeditions to the western and central Arctic Ocean between 1983 and 1998, were analyzed for total mercury (∑Hg), methyl mercury (MeHg), polychlorinated biphenyls (PCBs) and other industrial or byproduct organochlorines (chlorobenzenes, pentachloroanisole, octachlorostyrene), organochlorine pesticides (OCPs), and polybrominated diphenyl ethers (PBDEs). Median ∑Hg concentrations ranged from 70 to 366 ng g(-1) wet weight (ww). MeHg concentrations (3.55 to 23.5 ng g(-1) ww) accounted for 1.7 to 20.1% (median 3.7%) of ∑Hg. ∑Hg and MeHg were positively and significantly correlated with ww (∑Hg r(2) = 0.18, p = 0.0004, n = 63; MeHg r(2) = 0.42, p = 0.0004, n = 25), but not significantly with δ(13)C nor δ(15)N. Median concentrations of total persistent organic pollutants (POPs) ranged from 9750 to 156 000 ng g(-1) lipid weight, with order of abundance: ∑TOX (chlorobornanes quantified as technical toxaphene) > ∑PCBs > ∑DDTs > ∑chlordanes > ∑mirex compounds > ∑BDEs ∼ ∑chlorobenzenes ∼ octachlorostyrene > α-hexachlorocyclohexane ∼ hexachlorobenzene ∼ pentachloroanisole. Enantioselective accumulation was found for the chiral OCPs o,p'-DDT, cis- and trans-chlordane, nonachlor MC6 and oxychlordane. Lipid-normalized POPs concentrations were elevated in amphipods with lipid percentages ≤10%, suggesting that utilization of lipids resulted in concentration of POPs in the remaining lipid pool. Multidimensional Scaling (MDS) analysis using log-transformed physiological variables and lipid-normalized organochlorine concentrations distinguished amphipods from the central vs western arctic stations. This distinction was also seen for PCB homologues, whereas profiles of other compound classes were more related to specific stations rather than central-west differences.
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| 4. |
- Butt, Craig M., et al.
(författare)
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Levels and trends of poly- and perfluorinated compounds in the arctic environment
- 2010
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Ingår i: Science of the Total Environment. - : Elsevier BV. - 0048-9697 .- 1879-1026. ; 408:15, s. 2936-2965
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Tidskriftsartikel (refereegranskat)abstract
- Poly- and perfluorinated organic compounds (PFCs) are ubiquitous in the Arctic environment. Several modeling studies have been conducted in attempt to resolve the dominant transport pathway of PFCs to the arctic-atmospheric transport of precursors versus direct transport via ocean currents. These studies are generally limited by their focus on perfluorooctanoate (PFOA) fluxes to arctic seawater and thus far have only used fluorotelomer alcohols (FTOHs) and sulfonamide alcohols as inputs for volatile precursors. There have been many monitoring studies from the North American and European Arctic, however, almost nothing is known about PFC levels from the Russian Arctic. In general, there are very few measurements of PFCs from the abiotic environment. Atmospheric measurements show the widespread occurrence of PFC precursors, FTOHs and perfluorinated sulfonamide alcohols. Further, PFCAs and PFSAs have been detected on atmospheric particles. The detection of PFCAs and PFSAs in snow deposition is consistent with the volatile precursor transport hypothesis. There are very limited measurements of PFCs in seawater. PFOA is generally detected in the greatest concentrations. Additional seawater measurements are needed to validate existing model predications. The bulk of the monitoring efforts in biological samples have focused on the perfluorinated carboxylates (PFCAs) and sulfonates (PFSAs), although there are very few measurements of PFC precursors. The marine food web has been well studied, particularly the top predators. In contrast, freshwater and terrestrial ecosystems have been poorly studied. Studies show that in wildlife perfluorooctane sulfonate (PFOS) is generally measured in the highest concentration, followed by either perfluorononanoate (PFNA) or perfluoroundecanoate (PFUnA). However, some whale species show relatively high levels of perfluorooctane sulfonamide (PFOSA) and seabirds are typically characterized by high proportions of the C-11-C-15 PFCAs. PFOA is generally infrequently detected and is present in low concentrations in arctic biota. Food web studies show high bioaccumulation in the upper trophic-level animals, although the mechanism of PFC biomagnification is not understood. Spatial trend studies show some differences between populations, although there are inconsistencies between PFC trends. The majority of temporal trend studies are from the Northern American Arctic and Greenland. Studies show generally increasing levels of PFCs from the 1970s, although some studies from the Canadian Arctic show recent declines in PFOS levels. In contrast, ringed seals and polar bears from Greenland continue to show increasing PFOS concentrations. The inconsistent temporal trends between regions may be representative of differences in emissions from source regions.
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| 5. |
- Holmström, Katrin, 1975-
(författare)
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Analysis of Perfluoroalkyl Acids in Swedish Biota : Temporal trends, tissue distribution and toxicity
- 2010
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Perfluorinated alkyl acids (PFAS) are ubiquitous environmental contaminants. They are found in high concentrations in top predators worldwide, with perfluorooctane sulfonate (PFOS) as the predominant compound. Due to concerns regarding toxicity and persistence of PFOS, this compound was included in the Stockholm convention of persistent organic pollutants in 2009. PFAS differ from other persistent organic pollutants in their physicochemical properties and as a result their environmental fate is insufficiently understood. The focus of this thesis was to learn more on the environmental fate of PFAS by analysis of 15 different PFAS in Swedish biota. Analytes included perfluorinated carboxylates (PFCAs; carbon chain lengths C6-C15), perfluorinated sulfonates (PFSAs; C4, C6, C8, C10), and perfluorooctane sulfonamide (PFOSA). Elevated concentrations of PFAS were found in the marine, terrestrial and limnic Swedish environment, exemplified by Baltic common guillemot (Uria aalge), peregrine falcon (Falco peregrinus), and the amphipod Monoporeia affinis. PFOS was the predominant PFAS in the species. Analysis of archived material showed that PFOS concentration had increased 30-fold in guillemot eggs since 1968. PFOS concentration in peregrine falcon eggs had increased from 1974 to the mid 1980s and then leveled off, while PFCA in the falcon eggs showed an exponential increase until recent years. The relation between PFAS concentrations in egg and in tissue from adult guillemot showed that PFAS had different potentials for transfer to the egg, depending on chain length and functional group. The toxicological implications of PFAS pollution in the Swedish environment are not known but the high concentrations of PFOS in the Baltic guillemot eggs are of concern. Recent toxicological studies show toxic effects of PFOS in concentrations close to, or below the concentrations reported in this thesis. The margins of safety seem to be higher for the PFCAs, although toxicity data are scarce.
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| 6. |
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| 7. |
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| 8. |
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| 9. |
- Löfstrand, Karin, et al.
(författare)
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Spatial trends of polyfluorinated compounds in guillemot (Uria aalge) eggs from North-Western Europe
- 2008
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Ingår i: Chemosphere. - : Elsevier BV. - 0045-6535 .- 1879-1298. ; 72:10, s. 1475-1480
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Tidskriftsartikel (refereegranskat)abstract
- Polyfluorinated alkyl compounds (PFCs) are a group of chemicals of growing concern that have been detected in biological and abiotic samples worldwide. This study reports the concentrations of a suite of PFCs: perfluorooctyl sulfonate (PFOS), perfluorooctyl sulfonamide (PFOSA) and perfluorinated carboxylic acids (PFCAs) in guillemot (Uria aalge) eggs, collected in North-Western Europe, from Iceland, the Faroe Islands, Sweden and two locations in Norway. The highest concentrations of PFOS were found in samples from Sweden (mean 400 ng g(-1) wet weight (w.w.)), which were almost five times higher than concentrations found in Norwegian samples (mean 85 ng g(-1) w.w. from both sample sites). The concentrations found in Icelandic and Faroe samples were lowest (mean 16 and 15 ng g(-1) w.w., respectively). Only Swedish samples differed signiflcantly from the other locations. In general, PFCAs show a different spatial trend than PFOS. Perfluorooctanoic acid (PFOA) was not detected in any sample and perfluorononanoic acid (PFNA) was only detected in samples from Sweden. The most abundant PFCA was perfluoroundecanoic acid (PFUA) with highest concentrations in samples from Sweden (mean 82 ng g(-1) w.w.), samples from the Faroe Islands had the second highest concentration (mean 57 ng g(-1) w.w.) and samples from Iceland and Norway had concentrations ranging between 18 and 30 ng g(-1) w.w. The original hypothesis was based on the idea that PFC concentrations are the highest close to more densely populated and industrialized areas and lower levels in remote areas. However, the geographic pattern is more complicated than predicted and varies among different PFCs.
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| 10. |
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