Spatial and temporal variability of perfluoroalkyl substances in ...1,2103 3 33,580 ± 9,5603 N/A...
Transcript of Spatial and temporal variability of perfluoroalkyl substances in ...1,2103 3 33,580 ± 9,5603 N/A...
1
Electronic Supplementary Information for
Spatial and temporal variability of perfluoroalkyl
substances in the Laurentian Great Lakes
Christina K. Remucal1,2*
1Environmental Chemistry and Technology Program
University of Wisconsin – Madison
Madison, Wisconsin
2Department of Civil and Environmental Engineering
University of Wisconsin – Madison
Madison, Wisconsin
Submitted to: Environmental Science: Processes & Impacts, May 31, 2019. Contents (18 pages): Figures: S1 – S16, Tables: S1 – S2 * Corresponding author address: 660 N. Park St., Madison, WI 53706; e-mail:
[email protected]; telephone: (608) 262-1820; fax: (608) 262-0454; Twitter: @remucal.
Electronic Supplementary Material (ESI) for Environmental Science: Processes & Impacts.This journal is © The Royal Society of Chemistry 2019
2
Aqueous Concentrations
Figure S1. Mean surface (<10 m depth) concentrations of (a) PFBS and (b) PFHxS in the Great Lakes. Points represent the average value and error bars represent the standard deviation of concentrations within each study. Data is compiled from Furdui et al. 2008,1 Scott et al. 2010,2 and De Silva et al. 2011.3
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Superior Michigan Huron Erie Ontario
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S] (n
g/L)
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Furdui 2008Scott 2010De Silva 2011
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[PFH
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(a) (b)
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Figure S2. Mean surface (<10 m depth) concentrations of (a) PFHxA, (b) PFHpA, (c) PFNA, and (d) PFDA in the Great Lakes. Points represent the average value and error bars represent the standard deviation of concentrations within each study. Data is compiled from Simcik et al. 2005,4 Scott et al. 2006,5 Furdui et al. 2008,1 Scott et al. 2010,2 De Silva et al. 2011,3 and Myers et al. 2012.6
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Surface Sediment Concentrations
Figure S3. Mean surface sediment concentrations of (a) PFBS, (b) PFHxS, and (c) PFDS in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations within each study. Data is compiled from Yeung et al. 2013,7 Codling et al. 2014,8 Guo et al. 2016,9 Codling et al. 2018a,10 and Codling et al. 2018b.11
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Figure S4. Mean surface sediment concentrations of (a) PFBA, (b) PFPeA, (c) PFHxA, and (d) PFHpA in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations within each study. Data is compiled from Yeung et al. 2013,7 Codling et al. 2014,8 Guo et al. 2016,9 Codling et al. 2018a,10 and Codling et al. 2018b.11
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Figure S5. Mean surface sediment concentrations of (a) PFNA, (b) PFDA, (c) PFUnA, and (d) PFDoA in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations within each study. Data is compiled from De Silva et al. 2009,12 Yeung et al. 2013,7 Guo et al. 2016,9 Codling et al. 2018a,10 and Codling et al. 2018b.11
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nA] (
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oA] (
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PFAS in Great Lakes Fish Table S1. Reported KBAF (L/kg) for fish in the Great Lakes and nearby waters (mean ± standard deviation when reported). All values are based on the PFAS concentration in the specified fish tissue divided by the PFAS concentration in the water.
Lake Organism PFOA PFNA PFDA PFUnA PFHxS PFOS Superior Lake trout,
whole 41 ± 41,3 1,99513
8,170 ± 1,870,3 5,00013
5,760 ± 2,410,3 7,940 ± 2,00013
N/A 32013 9,040 ± 2,210,3 19,95013
Michigan Lake trout, whole
2,51013 N/A N/A N/A N/A 6,31013
Huron Lake trout, whole
3,9803 4,400 ± 1,540,3 3,98013
3,310 ± 1,593,3 5,01013
120,900 ± 48,6003
2,180 ± 1,200,3 2,00013
7,690 ± 2,550,3 10,00013
Erie Lake trout, whole
10 ± 7,3 79013
8,900 ± 2,530,3 6,31013
56,600 ± 17,500,3 19,95013
N/A 1,710 ± 820,3 6013
33,700 ± 4,730,3 25,10013
Ontario Lake trout, whole
200 ± 80,3 40013
1,840 ± 240,3 1,26013
11,750 ± 2,860,3 5,00013
156,400 ± 42,1003
750 ± 126,3 1,00013
9,400 ± 1,600,3 7,90013
Erie Walleye, whole
90 ± 203 4,160 ± 1,2103
33,580 ± 9,5603
N/A N/A 18,970 ± 2,6503
Figure S6. Biomagnification factors calculated for lake trout in Lake Ontario versus chain length for (a) PFCAs14 and (b) PFSAs.14, 15 BMF was calculated based on the fish concentration measured in whole fish divided by the concentration measured in their prey. The PFCA values and the highest PFOS value (2.9) are weighted according to different fish species consumed by lake trout,14 whereas the other PFOS values are lake trout concentrations compared directly to alewife (1.6), smelt (0.8), and sculpin (0.2).15
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PFCA Chain Length
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Figure S7. Trophic magnification factors calculated for four species (i.e., Mysis, alewife, smelt, and lake trout) in Lake Ontario versus chain length for (a) PFCAs and (b) PFSAs.14, 15
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PFCA Chain Length
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Figure S8. Mean concentrations of (a) PFHxS, (b) PFDS, (c) PFBA, and (d) PFHpA in fish in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations within each study. Data is presented for whole lake trout,3, 13, 16, 17 skin on lake trout fillets,18 skin off lake trout fillets,19 and whole walleye.3
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LT wholeLT skinLT W wholeLT no skinAlewifewalleye whole
extra
[PFD
S] (n
g/g)
Superior Michigan Huron Erie Ontario
Lake troutLake trout fillet (skin on)Lake trout & walleyeLake trout fillet (skin off)AlewifeWalleye
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A] (
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FHxS
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/g)
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FHpA
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Figure S9. Mean concentrations of (a) PFNA, (b) PFDA, (c) PFUnA, (d) PFDoA, (e) PFTrA, and (f) PFTeA in fish in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations within each study. Data is presented for whole lake trout,3, 13-
17 skin on lake trout fillets,18 combined concentrations for whole lake trout and walleye,16 skin off lake trout fillets,19 whole alewife,14, 15 and whole walleye.3
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PFAS in Herring Gulls and Other Terrestrial Biota Table S2. Reported concentrations of PFAS in less frequently studied biota in or near Lakes Superior (SU), Michigan (MI), Huron (HU), Erie (ER), or Ontario (ON). Values in parentheses are the range of concentrations. Values outside of parentheses correspond to study means ± the standard deviation when available.
Compound Invertebrates Amphibians Reptiles Birds Mammals PFSAs PFHxS N/A Frog liver
(HU): <LOD20
Snapping turtle plasma (HU): <LOD20
Bald eagle plasma (SU): 2.0 (<LOD – 8.6) ng/mL;21 tree swallow plasma (SU): <LOD22
Mink liver (HU): (6.3 – 40) ng/g20
PFOS Mysis (ON): (1.8 – 13) ng/g;12, 14 23 Diporeia (ON): (21 – 280) ng/g;14,
15, 23 zooplankton (ON): (1.4 – 6.5) ng/g15, 23
Frog liver (HU): (<LOD – 285) ng/g20
Snapping turtle plasma (HU): (<LOD – 169) ng/mL20
Bald eagle liver (MI): 394 (27 – 1,740) ng/g;20 bald eagle muscle (MI): 32 (<LOD – 96) ng/g;20 bald eagle plasma (SU): 345 (71 – 830) ng/mL;21 cormorant plasma (HU): 215 (1 – 430) ng/mL;24 tree swallow plasma (SU): 13.1 (5.6 – 30) ng/g22
Mink liver (HU): (64 – 4,870) ng/g20
PFDS N/A N/A N/A Bald eagle plasma (SU): 13.7 (<LOD – 100) ng/mL21
N/A
PFCAs PFBA N/A N/A N/A Bald eagle plasma
(SU): 0.4 (<LOD – 22) ng/mL21
N/A
PFOA Mysis (ON): (2.5 – 3.9) ng/g;12, 14 Diporeia (ON): (67 – 90) ng/g;14 12 zooplankton (ON): 1.3 ng/g12
Frog liver (HU): <LOD20
Snapping turtle plasma (HU): <LOD20
Bald eagle plasma (SU): 0.8 (<LOD – 14) ng/mL;21 tree swallow plasma (SU): 11.9 (1.9 – 31.7) ng/g22
Mink liver (HU): (<LOD – 12) ng/g20
PFNA Mysis (ON): (2.7 – 2.8) ng/g;12, 14 Diporeia (ON): (37 – 57) ng/g;12,
14 zooplankton (ON): 0.4 ng/g12
N/A N/A Bald eagle plasma (SU): 6.5 (4.9 – 160) ng/mL;21 tree swallow plasma (SU): 9.1 (2.2 – 20.8) ng/g22
N/A
PFDA Mysis (ON): (1.2 – 1.3) ng/g;12, 14 Diporeia (ON): (16 – 32) ng/g;12,
14 zooplankton (ON): 0.4 ng/g12
N/A N/A Bald eagle plasma (SU): 12 (0.1 – 77) ng/mL;21 tree swallow plasma (SU): 1.7 (0.5 – 2.9) ng/g22
N/A
12
PFUnA Mysis (ON): (0.8 – 1.3) ng/g;12, 14 Diporeia (ON): (18 – 41) ng/g;12,
14 zooplankton (ON): (0.2 – 0.8) ng/g12
N/A N/A Bald eagle plasma (SU): 14.7 (10.9 – 110) ng/mL;21 tree swallow plasma (SU): 3.4 (1.3 – 5.5) ng/g22
N/A
PFDoA Mysis (ON): (0.4 – 1.8) ng/g;12, 14 Diporeia (ON): (5 – 14) ng/g;12, 14 zooplankton (ON): 0.3 ng/g12
N/A N/A Bald eagle plasma (SU): 6.4 (2.0 – 27) ng/mL; 21 tree swallow plasma (SU): (<LOD – 0.9) ng/g22
N/A
PFTrDA Mysis (ON): 1.5 ± 0.2 ng/g;14 Diporeia (ON): 15 ± 0.8 ng/g14
N/A N/A Bald eagle plasma (SU): 3.5 (3.0 – 63) ng/mL21
N/A
PFTeDA Mysis (ON): <LOD;14 Diporeia (ON): 7.3 ± 0.6 ng/g14
N/A N/A Bald eagle plasma (SU): 1.4 (0.4 – 19) ng/mL21
N/A
Figure S10. (a) Concentration and (b) percent distribution of commonly studied PFAS in female herring gull eggs and tissues collected in 2010 from Chantry Island, Lake Huron.25
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Figure S11. (a) Concentration and (b) percent distribution of commonly studied PFAS in herring gull eggs collected from colonies in the Great Lakes determined based on mean concentrations calculated across all studies shown in Figures 9, S12, and S13.26-29 Colonies are arranged from west to east and include three riverine colonies (i.e., Detroit River, Niagara River, and Strachan Island).
Figure S12. Mean concentrations of (a) PFHxS and (b) PFDS in herring gull eggs collected from 17 colonies in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations within each study.27, 28 Data is compiled from Gebbink et al. 201127 and Letcher et al. 2015.28
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Dis
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PFHxSPFOSPFDSPFHpAPFOAPFNAPFDAPFUnAPFDoAPFTrAPFTeA
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[PFD
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Superior Michigan Huron Erie Ontario0
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Geb10 mean
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Let15 mean
extra
[PFH
xS] (
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Superior Michigan Huron Erie Ontario
Gebbink 2011Letcher 2015
(a)
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Figure S13. Mean concentrations of (a) PFNA, (b) PFDA, (c) PFUnA, (d) PFDoA, (e), PFTrA, and (f) PFTeA in herring gull eggs collected from 17 colonies in the Great Lakes. Points represent the average value and error bars represent the reported range of concentrations27, 28 or standard deviation29 within each study. Data is compiled from Gebbink et al. 2009,29 Gebbink et al. 2011,27 and Letcher et al. 2015.28
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Gebbink 2009Gebbink 2011Letcher 2015
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nA] (
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A] (
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eA] (
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Temporal Trends in PFAS
Figure S14. Temporal variability in the average surface concentrations of (a) PFOS and (b) PFOA in Lake Erie. Error bars correspond to reported standard deviations and are not available for all data points.1, 3, 30
Figure S15. Temporal variability in the average surface concentrations of (a) PFOS and (b) PFOA in Lake Ontario. Error bars correspond to reported standard deviations and are not available for all data points.1, 3, 6, 15, 30
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y = 227.93 - 0.112x R= 0.19056
[PFO
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PFOS
extra
y = 560.51 - 0.27667x R= 0.39201
[PFO
S] (n
g/L)
Year
PFOS
0
2
4
6
8
10
2002 2004 2006 2009 2011
PFOA
extra
y = 365.96 - 0.18056x R= 0.29689
[PFO
A] (
ng/L
)
Year
PFOA
(a) (b)
16
Figure S16. Percentage of total PFAS present at PFOS in whole lake trout collected in Lake Ontario. Data from Furdui (hollow)31 was estimated from figures. All other data was summarized from tabulated data.3, 13, 16, 17 Note that the 2010 data point was averaged for samples collected in 2008 – 2012.16 References 1. Furdui, V. I.; Crozier, P. W.; Reiner, E. J.; Mabury, S. A., Trace level determination of
perfluorinated compounds in water by direct injection. Chemosphere 2008, 73, (1), S24-S30.
2. Scott, B. F.; De Silva, A. O.; Spencer, C.; Lopez, E.; Backus, S. M.; Muir, D. C. G., Perfluoroalkyl acids in Lake Superior water: Trends and sources. J. Great Lakes Res. 2010, 36, (2), 277-284.
3. De Silva, A. O.; Spencer, C.; Scott, B. F.; Backus, S.; Muir, D. C. G., Detection of a cyclic perfluorinated acid, perfluoroethylcyclohexane sulfonate, in the Great Lakes of North America. Environ. Sci. Technol. 2011, 45, (19), 8060-8066.
4. Simcik, M. F.; Dorweiler, K. J., Ratio of perfluorochemical concentrations as a tracer of atmospheric deposition to surface waters. Environ. Sci. Technol. 2005, 39, (22), 8678-8683.
5. Scott, B. F.; Moody, C. A.; Spencer, C.; Small, J. M.; Muir, D. C. G.; Mabury, S. A., Analysis for perfluorocarboxylic acids/anions in surface waters and precipitation using GC-MS and analysis of PFOA from large-volume samples. Environ. Sci. Technol. 2006, 40, (20), 6405-6410.
6. Myers, A. L.; Crozier, P. W.; Helm, P. A.; Brimacombe, C.; Furdui, V. I.; Reiner, E. J.; Burniston, D.; Marvin, C. H., Fate, distribution, and contrasting temporal trends of perfluoroalkyl substances (PFASs) in Lake Ontario, Canada. Environ. Int. 2012, 44, 92-99.
7. Yeung, L. W. Y.; De Silva, A. O.; Loi, E. I. H.; Marvin, C. H.; Taniyasu, S.; Yamashita, N.; Mabury, S. A.; Muir, D. C. G.; Lam, P. K. S., Perfluoroalkyl substances and extractable
0
20
40
60
80
100
PFOS distPFOS dist Furdui
extra
1980 1990 2000 2010
PFO
S D
istr
ibut
ion
(%)
Year
All other dataFurdui 2008
0
50
100
150
200
250 PFOS
PFOS Furdui
PFOS Martin
PFAS total
TOtal Fur
extra
1980 1990 2000 2010
[PFO
S] o
r [To
tal P
FAS]
(ng/
g)
Year
All other dataFurdui 2008Martin 2004
0
50
100
150
200
250 PFOS
PFOS Furdui
PFOS Martin
PFAS total
TOtal Fur
extra
1980 1990 2000 2010
[PFO
S] o
r [To
tal P
FAS]
(ng/
g)
Year
All other dataFurdui 2008Martin 2004
(a)
0
20
40
60
80
100
PFOS distPFOS dist Furdui
extra
1980 1990 2000 2010
PFO
S D
istr
ibut
ion
(%)
Year
All other dataFurdui 2008
(b)
(e) (f)
17
organic fluorine in surface sediments and cores from Lake Ontario. Environ. Int. 2013, 59, 389-397.
8. Codling, G.; Vogt, A.; Jones, P. D.; Wang, T.; Wang, P.; Lu, Y. L.; Corcoran, M.; Bonina, S.; Li, A.; Sturchio, N. C.; Rockne, K. J.; Ji, K.; Khim, J.-S.; Naile, J. E.; Giesy, J. P., Historical trends of inorganic and organic fluorine in sediments of Lake Michigan. Chemosphere 2014, 114, 203-209.
9. Guo, R.; Megson, D.; Myers, A. L.; Helm, P. A.; Marvin, C.; Crozier, P.; Mabury, S.; Bhavsar, S. P.; Tomy, G.; Simcik, M.; McCarry, B.; Reiner, E. J., Application of a comprehensive extraction technique for the determination of poly- and perfluoroalkyl substances (PFASs) in Great Lakes Region sediments. Chemosphere 2016, 164, 535-546.
10. Codling, G.; Hosseini, S.; Corcoran, M. B.; Bonina, S.; Lin, T.; Li, A.; Sturchio, N. C.; Rockne, K. J.; Ji, K.; Peng, H.; Giesy, J. P., Current and historical concentrations of poly and perfluorinated compounds in sediments of the northern Great Lakes - Superior, Huron, and Michigan. Environ. Poll. 2018, 236, 373-381.
11. Codling, G.; Sturchio, N. C.; Rockne, K. J.; Li, A.; Peng, H.; Tse, T. J.; Jones, P. D.; Giesy, J. P., Spatial and temporal trends in poly- and per-fluorinated compounds in the Laurentian Great Lakes Erie, Ontario and St. Clair. Environ. Poll. 2018, 237, 396-405.
12. De Silva, A. O.; Muir, D. C. G.; Mabury, S. A., Distribution of perfluorocarboxylate isomers in select samples from the North American environment. Environ. Toxicol. Chem. 2009, 28, (9), 1801-1814.
13. Furdui, V. I.; Stock, N. L.; Ellis, D. A.; Butt, C. M.; Whittle, D. M.; Crozier, P. W.; Reiner, E. J.; Muir, D. C. G.; Mabury, S. A., Spatial distribution of perfluoroalkyl contaminants in lake trout from the Great Lakes. Environ. Sci. Technol. 2007, 41, (5), 1554-1559.
14. Martin, J. W.; Whittle, D. M.; Muir, D. C. G.; Mabury, S. A., Perfluoroalykl contaminants in a food web from Lake Ontario. Environ. Sci. Technol. 2004, 38, 5379-5385.
15. Houde, M.; Czub, G.; Small, J. M.; Backus, S.; Wang, X.; Alaee, M.; Muir, D. C. G., Fractionation and bioaccumulation of perfluorooctane sulfonate (PFOS) isomers in a Lake Ontario food web. Environ. Sci. Technol. 2008, 42, (24), 9397-9403.
16. McGoldrick, D. J.; Murphy, E. W., Concentration and distribution of contaminants in lake trout and walleye from the Laurentian Great Lakes (2008-2012). Environ. Poll. 2016, 217, 85-96.
17. Gewurtz, S. B.; De Silva, A. O.; Backus, S. M.; McGoldrick, D. J.; Keir, M. J.; Small, J.; Melymuk, L.; Muir, D. C. G., Perfluoroalkyl contaminants in Lake Ontario lake trout: Detailed examination of current status and long-term trends. Environ. Sci. Technol. 2012, 46, (11), 5842-5850.
18. Williams, M. C.; Schrank, C. S., Perfluorinated compounds (PFCs) in fish from Wisconsin’s major rivers and Great Lakes. 2016, Wisconsin Department of Natural Resources, Fisheries Management Administrative Report No. 83, pp. 1-12.
19. Guo, R.; Reiner, E. J.; Bhavsar, S. P.; Helm, P. A.; Mabury, S. A.; Braekevelt, E.; Tittlemier, S. A., Determination of polyfluoroalkyl phosphoric acid diesters, perfluoroalkyl phosphonic acids, perfluoroalkyl phosphinic acids, perfluoroalkyl carboxylic acids, and perfluoroalkane sulfonic acids in lake trout from the Great Lakes region. Anal. Bioanal. Chem. 2012, 404, (9), 2699-2709.
18
20. Kannan, K.; Tao, L.; Sinclair, E.; Pastva, S. D.; Jude, D. J.; Giesy, J. P., Perfluorinated compounds in aquatic organisms at various trophic levels in a Great Lakes food chain. Arch. Environ. Contam. Toxicol. 2005, 48, (4), 559-566.
21. Route, W. T.; Key, R. L.; Russell, R. E.; Lindstrom, A. B.; Strynar, M. J., Spatial and temporal patterns in concentrations of perfluorinated compounds in bald eagle nestlings in the upper midwestern United States. Environ. Sci. Technol. 2014, 48, (12), 6653-6660.
22. Custer, C. M.; Custer, T. W.; Dummer, P. M.; Etterson, M. A.; Thogmartin, W. E.; Wu, Q.; Kannan, K.; Trowbridge, A.; McKann, P. C., Exposure and effects of perfluoroalkyl substances in tree swallows nesting in Minnesota and Wisconsin, USA. Arch. Environ. Contam. Toxicol. 2013, 66, (1), 120-138.
23. Asher, B. J.; Wang, Y.; De Silva, A. O.; Backus, S.; Muir, D. C. G.; Wong, C. S.; Martin, J. W., Enantiospecific perfluorooctane sulfonate (PFOS) analysis reveals evidence for the source contribution of PFOS-precursors to the Lake Ontario foodweb. Environ. Sci. Technol. 2012, 46, (14), 7653-7660.
24. Giesy, J. P.; Kannan, K., Global distribution of perfluorooctane sulfonate in wildlife. Environ. Sci. Technol. 2001, 35, (7), 1339-1342.
25. Gebbink, W. A.; Letcher, R. J., Comparative tissue and body compartment accumulation and maternal transfer to eggs of perfluoroalkyl sulfonates and carboxylates in Great Lakes herring gulls. Environ. Poll. 2012, 162, 40-47.
26. Gebbink, W. A.; Letcher, R. J., Linear and branched perfluorooctane sulfonate isomer patterns in herring gull eggs from colonial sites across the Laurentian Great Lakes. Environ. Sci. Technol. 2010, 44, (10), 3739-3745.
27. Gebbink, W. A.; Letcher, R. J.; Hebert, C. E.; Chip Weseloh, D. V., Twenty years of temporal change in perfluoroalkyl sulfonate and carboxylate contaminants in herring gull eggs from the Laurentian Great Lakes. J. Environ. Monitor. 2011, 13, (12), 3365.
28. Letcher, R. J.; Su, G.; Moore, J. N.; Williams, L. L.; Martin, P. A.; de Solla, S. R.; Bowerman, W. W., Perfluorinated sulfonate and carboxylate compounds and precursors in herring gull eggs from across the Laurentian Great Lakes of North America: Temporal and recent spatial comparisons and exposure implications. Sci. Total Environ. 2015, 538, 468-477.
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31. Furdui, V. I.; Helm, P. A.; Crozier, P. W.; Lucaciu, C.; Reiner, E. J.; Marvin, C. H.; Whittle, D. M.; Mabury, S. A.; Tomy, G. T., Temporal trends of perfluoroalkyl compounds with isomer analysis in lake trout from Lake Ontario (1979−2004). Environ. Sci. Technol. 2008, 42, (13), 4739-4744.