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Supporting Information
Spatial Distribution and Source Tracing of Per- and Polyfluoroalkyl Substances (PFASs) in Surface Water in Northern
Europe
Minh A. Nguyen*, Karin Wiberg, Erik Ribeli, Sarah Josefsson, Martyn Futter, Jakob Gustavsson, Lutz Ahrens
Department of Aquatic Sciences and Assessment, Swedish University of Agricultural Sciences (SLU),
Box 7050, SE-75007, Uppsala, Sweden
Corresponding author
* Email: [email protected]
Pages: 30
Tables: 17
Figures: 4
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Table of Contents:
Table S1. Information for sampling sites at Swedish rivers S3
Table S2. Information for sampling sites at the Baltic Sea and the Kattegat S6
Table S3. List of analyzed PFASs and their octanol water partition coefficient (log KOW) S7
Table S4. Blank concentrations, MDLs, MQLs of PFASs for the aqueous phase S9
Table S5. Blank concentrations, MDLs and MQLs of PFASs for the particulate phase S9
Table S6. Recovery of internal standards in the field samples S10
Table S7. Standard deviation of duplicate river samples S10
Table S8. Standard deviation of duplicate samples from the Baltic Sea and the Kattegat S11
Table S9. Levels (ng L-1) of detected PFASs (aqueous phase) in Swedish river surface water S12
Table S10. Levels (ng L-1) of detected PFASs (aqueous phase) in the Baltic Sea and the Kattegat surface water S15
Table S11. Levels (ng L-1) of detected PFASs (particulate phase) in Swedish river surface water S16
Table S12. Levels (ng L-1) of detected PFASs (particulate phase) in the Baltic Sea and the Kattegat surface water S18
Table S13. Discharges Q (m3 s-1) of water and loads (kg yr-1) of ∑PFASs from Swedish rivers into the receiving sea S19
Table S14. Variations (R2X and R2Y) given by SIMCA® software for PFASs and water chemistry, demographic, geographic and hydrological factors in Swedish rivers S21
Table S15. Variations (R2X and R2Y) given by SIMCA® software for PFASs and water chemistry, geographic and hydrological factors in the Baltic Sea and the Kattegat S22
Table S16. Coefficients of determination (R2) and p-values of Pearson correlation of PFCAs, PFSAs and DOC (log10-transformed data) in rivers and the recipient seas......................................................S23
Table S17. Monthly DOC levels (mg L-1) for Swedish rivers (n = 40) during August to October, 2013 .....................................................................................................................................S24
Figure S1. Potential PFASs sources of ten rivers with elevated PFASs concentrations......................S27
Figure S2. PFOS concentrations (ng L-1) of 44 river sites along Swedish coast..................................S28
Figure S3. PFOS concentrations (ng L-1) of 18 sites in the Baltic Sea and the Kattegat......................S29
Figure S4. Biplot of principal component analysis (PCA) of PFAS concentrations (log10-transformed), latitude, and DOC of the river (n = 44) and seawater samples (n = 18)........................S30
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Table S1. Detailed information on the river sampling sites
Sample ID River names
Coordinates
(WGS 84) Discha-rge (Q)(m³ s-1)
Catchment size (km2)d
Water temperature
(°C)
Total population
in the catchment(persons)d
DOC(mg L-1)d
Run off(m³ s-1
km -2)
Population density
(person km -2)
Suspended particulate
matter (mg)Latitude
(degree)Longitude(degree)
R1 Torne älv 65.847 24.156 420e 45297 5.7c 38 952 4.6 0.0093 0.86 3.6R2 Kalix älv 65.853 23.129 311e 19128 7.6c 32 540 5.0 0.016 1.70 3.1R3 Råne älv 66.022 21.968 43e 3778 10c 914 8.6 0.011 0.24 2.6R4b
Lule älv 65.589 22.032 522e 27901 9.4c 40 350 2.8 0.019 1.4 1.3R5 Alterälven 65.420 21.486 4.5e 458 6.0d 1 813 11 0.010 4.0 4.6R6 Pite älv 65.380 21.299 173e 11933 10c 9 815 3.3 0.014 0.82 1.4R7b
Skellefte älv 64.740 20.769 164e 11916 10c 14 010 2.6 0.014 1.2 1.3R8 Rickleån 64.087 20.941 16e 1648 6.7d 3 296 12 0.010 2.0 2.0
R9 Ume älv [Umeå]
64.198 19.869 440e 30502 7.9c 89 241 3.8 0.014 2.9 2.1
R9A Ume älv [Gubböle]
64.090 19.936 NAa 30245 8.2c 34 776 NA NA 1.22.4
R9B Vindelälven [Rödånäs]
63.886 19.917 NA 14114 9.1c 8 752 3.2 NA 0.62 2.0
R9C Vindelälven [Krycklan]
63.825 20.249 NA 85 7.2c 49 NA NA 0.57 1.5
R10 Öre älv 63.605 19.663 35e 2971 8.5c 3 629 15 0.012 1.2 1.9R11 Lögde älv 63.552 19.415 20e 1608 6.1d 913 9.8 0.013 0.57 1.9R12 Gide älv 63.346 19.116 39e 3439 NA 2 808 13 0.011 0.82 2.3R13 Ångermanälven 63.170 17.271 485e 33250 9.6c 39 426 6.0 0.015 1.2 2.0R14 Indalsälven 62.516 17.375 438e 28633 9.6c 100 711 4.3 0.015 3.5 0.8R15b
Ljungan 62.364 16.962 120e 12769 11c 25 025 9.5 0.0094 2.0 0.97
S3
52
Sample ID
River namesCoordinates
(WGS 84) Discha-rge (Q)(m³ s-1)
Catchment size (km2)d
Water temperature
(°C)
Total population
in the catchment(persons)d
DOC(mg L-1)d
Run off(m³ s-1
km -2)
Population density
(person km -2)
Suspended particulate
matter (mg)Latitude
(degree)Longitude(degree)
R16 Delångersån 61.638 17.086 16e 12 10c 1 299 6.4 1.3 104 1.4R17b
Ljusnan 61.214 17.083 216e 21106 12c 69 779 1.6 0.010 3.3 1.3R18 Gavleån 60.672 17.136 20e 2458 9.8c 92 562 12 0.0079 38 4.0R19 Dalälven 60.564 17.441 353e 29958 10c 253 417 5.6 0.012 8.5 5.1R20 Fyrisån 59.832 17.661 10e 1254 NA 133 186 14 0.0080 106 6.4R21 Norrström 59.328 18.067 166e 22620 13c 1 808 903 20 0.0073 80 2.0R22 Nyköpingsån 58.824 16.929 237e 3588 9.9c 68 331 13 0.066 19 5.0R23b
Motala ström 58.595 16.122 101e 15379 12c 519 322 7.1 0.0065 34 1.1R24 Botorpsström 57.664 16.496 6.7e 975 11d 5 021 11 0.0069 5.2 0.73R25 Emån 57.141 16.453 34e 4443 11c 74 200 10 0.0075 17 1.1R26 Alsterån 57.009 16.162 11e 1332 10d 6 544 13 0.0083 4.9 3.1R27 Ljungbyån 56.632 16.173 4.1e 757 9.5d 21 771 11 0.0055 29 2.6R28 Lyckebyån 56.199 15.663 6.0e 806 11d 14 692 14 0.0074 18 1.7R29 Mörrumsån 56.194 14.749 31e 3366 11c 11 4916 11 0.0092 34 2.5R30 Helge Å 55.944 14.219 42e 4140 11c 14 7971 9.0 0.010 36 2.6R31 Kävlingeån 55.780 13.077 11e 1183 9.7d 69 230 8.6 0.0096 58 2.0R32 Rönneån 56.122 13.145 11e 969 11d 39 170 10 0.011 40 8.5R33 Lagan 56.516 13.052 81e 6127 8.5d 105 825 10 0.013 17 3.2R34 Nissan 56.691 12.874 47e 2674 11d 66 999 10 0.018 25 2.4R35 Ätran 56.903 12.495 57e 3339 12d 61 109 9.2 0.017 18 2.6R36 Viskan 57.239 12.309 43e 2162 7.9d 128 880 7.3 0.020 60 4.1
R37 Göta älv [Alelyckan]
57.764 12.002 355e 48365 NA 780 439 4.9 0.0073 16 4.0
S4
Sample ID
River namesCoordinates
(WGS 84) Discha-rge (Q)(m³ s-1)
Catchment size (km2)d
Water temperature
(°C)
Total population
in the catchment(persons)d
DOC(mg L-1)d
Run off(m³ s-1
km -2)
Population density
(person km -2)
Suspended particulate
matter (mg)Latitude
(degree)Longitude(degree)
R37A Göta älv [Trollhättan]
57.846 11.914 554e 47206 11d 675 547 NA 0.012 14 3.4
R38 Nordre älv 58.284 12.281 540e 63 11d 22 792 NA 8.6 364 3.9R39 Örekilsälven 58.460 11.686 24e 1338 NA 13 454 12 0.018 10 3.1R40 Enningdalsälven 58.877 11.537 12e 5.7 12d 22 9.0 2.1 3.9 1.2
a NA = not available. b Duplicate for the sampling site. c measured data. d data from SLU database. e data from Swedish meteorological institute (URL1)
S5
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Table S2. Detailed information on the sampling sites in the Baltic Sea and the Kattegat
Sample ID
Coordinates
(WGS 84)Water
temperature
(°C)b
Salinity
(‰)b
DOC
(mg L-1)b
Suspended
particulate
matter
(mg)
Latitude
(degree)
Longitude
(degree)
S1 65.660 24.510 15 1.2 6.5 1.0S2 65.320 23.930 14 2.3 4.9 0.33S3 64.770 22.990 15 2.8 4.6 0.39S4 64.220 22.076 16 3.0 4.6 0.52S5 63.460 20.640 16 3.0 4.5 0.60S6 62.710 20.110 16 4.7 4.4 0.48S6a 61.700 19.630 16 4.7 4.4 0.26S7 60.370 19.300 17 5.3 4.2 0.50S8 59.860 19.640 17 5.4 4.2 0.20S9 58.757 19.297 17 5.4 4.3 0.46S10 58.050 18.500 18 6.1 4.6 0.53S11 57.260 17.680 19 6.3 4.6 0.66S12 56.050 16.700 19 6.5 4.6 0.64S13 55.180 14.044 18 7.1 4.4 0.67S13a 55.585 12.701 18 7.1 4.4 1.6S14 56.180 12.370 19 7.2 4.4 0.65S15 56.935 12.039 17 9.1 4.2 1.0S16 57.325 11.782 18 16 3.4 1.0S17 65.660 24.510 19 20 2.9 0.98S18 65.320 23.930 19 22 2.9 2.8
a Duplicate for the sampling site. b measured data
S6
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55
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57
58
59
60
61
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Table S3. The selected PFASs and their octanol-water partition coefficients (log KOW)
Abbreviation Name Molecular formula CAS No. Log Kowb
PFBA Perfluorobutanoic acid CF3(CF2)2COOH 375-22-4 2.82
PFPeA Perfluoropentanoic acid CF3(CF2)3COOH 2706-90-3 3.43
PFHxA Perfluorohexanoic acid CF3(CF2)4COOH 307-24-4 4.06
PFHpA Perfluoroheptanoic acid CF3(CF2)5COOH 375-85-9 4.67
PFOA Perfluorooctanoic acid CF3(CF2)6COOH 335-67-1 5.30
PFNA Perfluorononanoic acid CF3(CF2)7COOH 375-95-1 5.92
PFDA Perfluorodecanoic acid CF3(CF2)8COOH 335-76-2 6.50
PFUnDA Perfluoroundecanoic acid CF3(CF2)9COOH 2058-94-8 7.15
PFDoDA Perfluorododecanoic acid CF3(CF2)10COOH 307-55-1 7.77
PFTriDA Perfluorotridecanoic acid CF3(CF2)11COOH 72629-94-8 8.25
PFTeDA Perfluorotetradecanoic acid CF3(CF2)12COOH 376-06-7 8.90
PFHxDA Perfluorohexadecanoic acid CF3(CF2)14COOH 67905-19-5 NAa
PFOcDA Perfluorooctadecanoic acid CF3(CF2)16COOH 16517-11-6 NA
Abbreviation Name Molecular formula CAS No. Log Kowb
S7
63
PFBS Perfluorobutanesulfonic acid CF3(CF2)3SO3H 375-73-5 3.90
PFHxS Perfluorohexanesulfonic acid CF3(CF2)5SO3H 355-46-4 5.17
PFOS Perfluorooctanesulfonic acid CF3(CF2)7SO3H 1763-23-1 6.43
PFDS Perfluorodecanesulfonic acid CF3(CF2)9SO3H 335-77-3 7.66
6:2 FTS 6:2 fluorotelomer sulfonate F(CF2)6CH2CH2SO3- 27619-97-2 4.44
FOSA Perfluorooctanesulfonamide CF3(CF2)7SO2NH2 754-91-6 5.62
MeFOSA N-methyl perfluorooctane sulfonamide CF3(CF2)7SO2NH(CH3) 31506-32-8 6.07
EtFOSA N-ethylperfluoro-1-octanesulfonamide CF3(CF2)7SO2NHC2H5 4151-50-2 6.71
MeFOSE N-methyl perfluorooctanesulfonamidoethanol CF3(CF2)7SO2N(CH3)C2H4OH 24448-09-7 6.00
EtFOSE N-ethyl perfluorooctanesulfonamidoethanol CF3(CF2)7SO2N(C2H5)C2H4OH 1691-99-2 6.52
FOSAA Perfluoro-1-octanesulfonamidoacetic acid CF3(CF2)7SO2NHCOOH 2806-24-8 NA
MeFOSAA N-methyl perfluorooctanesulfonamidoacetic acid CF3(CF2)7SO2N(CH3)CH2COOH 2355-31-9 NA
EtFOSAA N-ethylperfluoro-1-octanesulfonamidoacetic acid CF3(CF2)7SO2N(C2H5)COOH 2991-50-6 NA
a NA = not available. b Kow = octanol-water partitioning coefficient (Wang et al., 2011)
S8
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Table S4. Blank concentrations (n = 5), MDLs and MQLs of PFASs for the aqueous phase samples
Compound Mean blank (ng L-1) MDLs (ng L-1) MQLs (ng L-1)PFBA 0.029 0.12 0.32PFPeA 0.12 0.76 2.3PFHxA 0.083 0.49 1.4PFHpA 0.051 0.27 0.77PFOA 0.025 0.087 0.23PFNA NDa 0.030 0.10PFDA ND 0.030 0.10PFUnDA ND 0.030 0.10PFDoDA ND 0.030 0.10PFTeDA ND 0.030 0.10PFOcDA ND 0.030 0.10PFBS ND 0.030 0.10PFHxS ND 0.030 0.10PFOS ND 0.030 0.106:2 FTS ND 0.030 0.10FOSA ND 0.030 0.10MeFOSA ND 0.030 0.10MeFOSE 0.061 0.15 0.37EtFOSE 0.058 0.17 0.45FOSAA ND 0.030 0.10MeFOSAA ND 0.030 0.10EtFOSAA ND 0.030 0.10
a ND = not detected.
Table S5. Blank concentrations (n = 6), MDLs and MQLs of PFASs for the particulate phase samples (GF/F) a
Compound Mean blank (ng L-1) MDLs (ng L-1) MQLs (ng L-1)PFBA NDa 0.030 0.10PFPeA ND 0.030 0.10PFHxA ND 0.030 0.10PFHpA ND 0.030 0.10PFOA ND 0.030 0.10PFNA ND 0.030 0.10PFDA ND 0.030 0.10PFUnDA ND 0.030 0.10PFDoDA ND 0.030 0.10PFTeDA ND 0.030 0.10PFOcDA ND 0.030 0.10PFBS ND 0.030 0.10PFHxS ND 0.030 0.10PFOS ND 0.030 0.106:2 FTS ND 0.030 0.10Compound Mean blank (ng L-1) MDLs (ng L-1) MQLs (ng L-1)
S9
6566
67
6869
FOSA ND 0.030 0.10MeFOSA ND 0.030 0.10MeFOSE ND 0.030 0.10EtFOSE ND 0.030 0.10MeFOSAA ND 0.030 0.10EtFOSAA ND 0.030 0.10
a ND = not detected.
Table S6. Average recoveries (%) of internal standards ± standard deviation (SD) for the field aqueous phase samples)for rivers and seas (n = 56)
Internal standard Recovery ± SD[13C4]-PFBA 111 ± 29 %[13C6]-PFHxA 87 ± 21 %[13C4]-PFOA 102 ± 23 %[13C9]-PFNA 102 ± 24 %[13C10]-PFDA 100 ± 24 %[13C11]-PFUnDA 97 ± 24 %[13C12]-PFDoDA 85 ± 23 %[18O2]-PFHxS 91 ± 25 %[13C4]-PFOS 102 ± 23 %[13C8]-FOSA 90 ± 21 %[d7]-MeFOSE 61 ± 21 %[d9]-EtFOSE 56 ± 20 %[d3]-MeFOSAA 107 ± 31 %[d5]-EtFOSAA 102 ± 30 %
Table S7. Standard deviation (%) of duplicate river samples (n = 5) (ID R4, R7, R15, R17 and R23)
SD (%) Average SD
(%) for all
PFASsPFBA PFOA PFNA PFDA PFUnDA PFDoDA FOS
A PFOS
Average SD (%)
for PFAS11 16 30 49 38 44 42 56 36
S10
70
7172
73
7475
76
77
78
79
80
81
Table S8. Standard deviation (%) of duplicate samples from the Baltic Sea and the Kattegat (n = 2) (ID S6 and S23)
SD (%) Average SD
(%) for all
PFASsPFB
APFHp
A PFOA PFNA PFDA FOSA PFBS PFHx
SPFO
S
Average SD (%) for
PFAS13 20 20 45 90 26 96 29 61 44
S11
8283
Table S9. Levels (ng L-1) of detected PFASs (aqueous phase) in Swedish river surface water
Sample ID PFBA PFHxA PFHpA PFOA PFNA PFDA PFUnDA PFDoDA PFTeDA PFBS PFHxS PFOS FOSA ƩPFASs
R1 0.94 <0.49 <0.27 0.26 0.15 0.13 0.077 0.053 <0.030 0.39 0.069 0.082 0.15 2.3
R2 0.76 <0.49 <0.27 0.23 0.23 <0.030 0.10 0.10 0.14 <0.030 <0.030 0.053 <0.030 1.6
R3 1.2 <0.49 <0.27 0.21 1.3 0.28 0.16 0.19 0.15 <0.030 0.15 0.34 <0.030 4.0
R4a 0.60± 0.00
<0.49 <0.27 0.39± 0.074
0.23± 0.057
0.14± 0.069
0.073± 0.022
0.033 <0.030 <0.030 0.051 0.058±0.018
0.12±0.023
1.7
R5 0.60 <0.49 0.61 <0.087 0.18 0.11 0.044 <0.030 <0.030 <0.030 <0.030 0.12 <0.030 1.7
R6 0.97 <0.49 0.54 0.44 0.40 0.22 0.081 0.069 <0.030 4.1 0.31 0.28 0.056 7.5
R7a 0.91±0.26
<0.49 <0.27 0.39±0.026
0.36±0.12
0.27±0.20
0.17±0.15
0.12±0.10
<0.030 5.1 0.19 0.30±0.31
0.37±0.12
8.2
R8 0.99 <0.49 <0.27 <0.09 0.09 <0.030 0.04 <0.030 <0.030 0.03 <0.030 0.04 0.10 1.3
R9 0.63 <0.49 <0.27 0.26 0.32 0.064 0.058 <0.030 <0.030 0.048 0.14 0.25 0.093 1.9
R9A 0.57 <0.49 1.0 3.3 5.8 4.4 1.6 0.77 0.46 16 18 6.9 <0.030 60
R9B 0.47 <0.49 <0.27 <0.087 0.26 <0.030 0.074 0.067 0.094 <0.030 <0.030 0.074 <0.030 1.0
R9C 0.99 <0.49 <0.27 <0.087 0.091 <0.030 0.041 <0.030 <0.030 0.030 <0.030 0.042 0.075 1.3
R10 0.62 <0.49 <0.27 0.39 0.36 0.14 0.084 0.043 <0.030 0.17 0.12 0.18 0.064 2.2
R11 0.96 <0.49 <0.27 <0.087 0.16 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 0.060 0.18 1.4
R12 0.79 <0.49 <0.27 <0.087 0.12 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 0.052 1.0
S12
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Sample ID PFBA PFHxA PFHpA PFOA PFNA PFDA PFUnDA PFDoDA PFTeDA PFBS PFHxS PFOS FOSA ƩPFASs
R13 0.96 <0.49 <0.27 <0.087 0.40 0.12 0.10 <0.030 <0.030 <0.030 <0.030 0.16 <0.030 1.8
R14 1.0 <0.49 0.36 1.5 2.8 1.9 0.84 0.40 0.84 6.9 7.6 3.1 <0.030 27
R15a 1.2±0.056
<0.49 <0.27 <0.087 0.21±0.00
0.024 0.044±0.00
<0.030 <0.030 <0.030 <0.030 0.12±0.090
0.032±0.059
1.6
R16 1.9 <0.49 1.4 3.6 5.6 4.3 1.8 0.82 0.41 17 16 6.8 <0.030 60
R17a 1.1± 0.19 <0.49 <0.27 0.34
±0.070.33
±0.070.092±0.00
0.087±0.02
0.035±0.00 <0.02 0.44 0.10 0.046 0.061
±0.03 2.8
R18 2.1 1.1 0.82 0.92 0.41 0.17 0.078 <0.030 <0.030 4.9 0.38 0.29 0.052 11
R19 1.2 1.1 0.56 0.40 0.37 0.15 0.16 0.046 0.42 0.42 0.13 0.61 0.053 5.5
R20 2.5 4.2 1.4 4.2 0.63 0.34 0.092 0.034 <0.030 2.2 12 5.3 0.094 33
R21 2.9 1.9 1.3 1.6 0.51 0.22 0.075 0.061 <0.030 0.83 1.2 2.4 0.46 13
R22 3.7 1.5 1.4 1.1 0.44 0.18 0.093 <0.030 0.093 0.61 0.64 0.71 0.076 10
R23a 2.1± 0.07
<0.49 <0.27 0.61± 0.08
0.32± 0.09
<0.02 0.047 <0.030 <0.030 <0.030 0.29 0.63± 0.04
0.098± 0.04
4.1
R24 2.0 <0.49 <0.27 0.22 0.19 <0.030 0.057 <0.030 <0.030 <0.030 <0.030 0.11 <0.030 2.5
R25 2.3 0.51 1.7 3.8 5.4 3.7 1.5 0.70 1.5 12 14 5.1 <0.030 52
R26 1.6 <0.49 <0.27 0.42 0.38 0.038 0.097 <0.030 <0.030 <0.030 <0.030 0.25 <0.030 2.8
R27 1.5 1.3 0.74 0.91 0.19 0.065 0.051 <0.030 <0.030 0.042 0.46 0.28 <0.030 5.6
S13
Sample ID PFBA PFHxA PFHpA PFOA PFNA PFDA PFUnDA PFDoDA PFTeDA PFBS PFHxS PFOS FOSA ƩPFASs
R28 1.9 <0.49 0.89 0.64 0.45 0.17 0.12 0.031 <0.030 <0.030 0.47 1.1 <0.030 5.7
R29 1.8 <0.49 0.85 0.98 0.60 0.22 0.14 0.080 <0.030 0.51 0.42 0.60 0.20 6.4
R30 1.8 1.5 1.0 1.2 0.61 0.30 0.18 0.095 <0.030 19 1.9 0.54 0.10 28
R31 1.8 2.6 0.96 1.1 0.12 0.088 0.037 <0.030 <0.030 0.15 0.73 0.50 0.16 8.3
R32 2.3 1.6 0.93 1.3 0.26 <0.030 <0.030 <0.030 <0.030 0.87 3.0 3.9 0.072 14
R33 1.8 <0.49 <0.27 1.0 0.36 0.058 0.018 0.016 <0.030 0.083 0.34 0.56 <0.030 4.2
R34 2.7 1.1 0.85 1.2 0.52 0.11 0.050 0.030 <0.030 0.44 0.41 0.81 0.072 8.3
R35 1.5 <0.49 <0.27 0.69 0.33 0.045 <0.030 <0.030 <0.030 <0.030 0.20 0.35 <0.030 3.1
R36 1.4 1.3 0.95 1.6 0.54 0.19 0.081 <0.030 <0.030 <0.030 0.39 0.79 0.079 7.3
R37 1.3 <0.49 0.55 1.1 0.41 0.11 0.039 <0.030 <0.030 0.041 0.34 0.79 0.037 4.7
R37A 1.4 <0.49 <0.27 0.75 0.26 0.047 0.062 <0.030 <0.030 0.035 0.28 0.35 <0.030 3.2
R38 0.88 <0.49 <0.27 0.98 0.38 0.060 <0.030 <0.030 <0.030 0.098 0.26 0.57 0.14 3.4
R39 2.1 <0.49 <0.27 0.87 0.27 0.049 <0.030 <0.030 <0.030 <0.030 0.11 0.40 0.041 3.9
R40 2.0 <0.49 <0.27 0.90 0.36 0.042 0.046 <0.030 <0.030 <0.030 0.24 0.25 <0.030 3.8
a duplicate samples.
S14
85
Table S10. Levels (ng L-1) of detected PFASs (aqueous phase) in the Baltic Sea and the Kattegat surface water
Sample ID PFBA PFHpA PFOA PFNA PFDA PFDoDA PFTeDA PFBS PFHxS PFOS FOSAA FOSA ƩPFASsS1 0.62 <0.27 0.24 0.41 <0.030 <0.030 <0.030 <0.030 0.15 0.17 <0.030 0.038 1.6S2 0.48 <0.27 0.21 0.20 <0.030 <0.030 <0.030 <0.030 0.11 0.11 <0.030 0.041 1.2S3 0.58 <0.27 0.24 0.14 <0.030 <0.030 0.053 <0.030 0.12 0.28 <0.030 0.043 1.5S4 0.55 0.61 0.51 1.54 <0.030 <0.030 <0.030 0.12 0.49 0.89 <0.030 0.032 4.7S5 0.39 <0.27 0.41 1.1 <0.030 <0.030 0.072 <0.030 0.37 0.63 0.061 0.035 3.1S6a 0.44 <0.27 0.38 0.66 <0.030 <0.030 0.016 <0.030 0.24 0.39 <0.030 0.019 2.1S7 0.45 <0.27 0.51 1.1 <0.030 <0.030 <0.030 0.14 0.44 0.72 <0.030 <0.030 3.3S8 0.41 <0.27 0.41 0.96 <0.030 <0.030 <0.030 <0.030 0.37 0.61 <0.030 <0.030 2.8S9 0.43 <0.27 0.53 1.4 <0.030 <0.030 <0.030 0.096 0.47 0.74 <0.030 <0.030 3.6S10 0.34 <0.27 0.57 1.2 0.045 <0.030 0.031 0.11 0.49 0.75 <0.030 0.046 3.5S11 0.40 <0.27 0.42 0.57 <0.030 <0.030 <0.030 0.062 0.25 0.50 <0.030 0.050 2.3S12 0.65 1.0 0.99 3.8 0.58 <0.030 0.053 0.16 1.2 2.0 <0.030 0.035 11S13a 0.41 0.71 0.71 2.1 0.25 0.045 0.024 0.15 0.60 1.3 <0.030 0.043 6.3S14 0.49 <0.27 0.60 1.2 0.075 <0.030 <0.030 0.13 0.40 0.71 <0.030 0.051 3.6S15 0.42 <0.27 0.65 1.1 <0.030 <0.030 <0.030 0.089 0.39 0.76 <0.030 0.040 3.5S16 0.49 0.61 0.82 2.2 0.21 <0.030 <0.030 0.12 1.7 0.92 <0.030 0.034 7.2S17 0.59 <0.27 0.86 1.6 0.28 <0.030 0.041 0.22 0.59 1.2 <0.030 <0.030 5.4S18 0.67 1.00 1.3 5.7 0.83 <0.030 0.048 0.57 1.5 2.5 <0.030 0.032 14
a duplicate samples.
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Table S11. Levels (ng L-1) of detected PFASs (particulate phase) in Swedish river surface water
PFNA PFDA PFUnDA PFDoDA PFTeDA PFOS FOSA ƩPFASsR1 <0.030 <0.030 0.031 0.031 <0.030 <0.030 <0.030 0.062R2 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAa
R3 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR4b <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR5 <0.030 <0.030 <0.030 0.29 <0.030 <0.030 <0.030 0.29R6 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR7b <0.030 <0.030 <0.030 0.036 0.037 <0.030 <0.030 0.073R8 <0.030 <0.030 <0.030 0.110 <0.030 <0.030 <0.030 0.11R9 0.28 0.35 0.19 0.21 0.049 0.070 <0.030 1.2R9A <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR9B <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR9C <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR10 <0.030 <0.030 <0.030 0.050 <0.030 <0.030 <0.030 0.050R11 <0.030 <0.030 <0.030 0.036 <0.030 <0.030 <0.030 0.036R12 <0.030 <0.030 <0.030 0.14 <0.030 <0.030 <0.030 0.14R13 <0.030 <0.030 <0.030 0.074 <0.030 <0.030 <0.030 0.074R14 <0.030 <0.030 <0.030 0.089 <0.030 <0.030 <0.030 0.089
R15b <0.030 <0.030 <0.030 0.064± 0.045 <0.030 <0.030 <0.030 0.064
R16 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NA
R17b <0.030 <0.030 <0.030 0.33± 0.21 <0.030 <0.030 <0.030 0.33
R18 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR19 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR20 <0.030 <0.030 <0.030 0.16 <0.030 <0.030 <0.030 0.16R21 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR22 <0.030 <0.030 <0.030 0.35 <0.030 <0.030 <0.030 0.35
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PFNA PFDA PFUnDA PFDoDA PFTeDA PFOS FOSA ƩPFASs
R23b <0.030 <0.030 <0.030 0.086± 0.079 <0.030 <0.030 <0.030 0.086
R24 <0.030 <0.030 <0.030 0.14 <0.030 <0.030 <0.030 0.14R25 <0.030 <0.030 <0.030 0.039 <0.030 <0.030 <0.030 0.039R26 <0.030 <0.030 <0.030 0.097 <0.030 <0.030 <0.030 0.097R27 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR28 <0.030 <0.030 <0.030 0.099 <0.030 <0.030 <0.030 0.099R29 <0.030 <0.030 <0.030 0.038 <0.030 <0.030 <0.030 0.038R30 <0.030 <0.030 <0.030 0.046 <0.030 <0.030 <0.030 0.046R31 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR32 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR33 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR34 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR35 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR36 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR37 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR37A <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR38 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR39 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NAR40 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 <0.030 NA
a NA = not available. b duplicate samples.
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Table S12. Levels (ng L-1) of detected PFASs (particulate phase) in the Baltic Sea and the Kattegat surface water
PFDoDA PFTeDA FOSA ƩPFASsS1 <0.030 <0.030 <0.030 NAa
S2 <0.030 <0.030 <0.030 NAS3 <0.030 <0.030 <0.030 NAS4 0.71 <0.030 <0.030 0.71S5 <0.030 <0.030 <0.030 NAS6b <0.030 <0.030 <0.030 NAS7 <0.030 <0.030 <0.030 NAS8 <0.030 <0.030 <0.030 NAS9 <0.030 <0.030 <0.030 NAS10 <0.030 <0.030 0.068 0.068S11 <0.030 <0.030 <0.030 NAS12 <0.030 <0.030 <0.030 NA
S13b <0.030 0.044± 0.035 <0.030 0.044
S14 <0.030 <0.030 <0.030 NAS15 <0.030 <0.030 <0.030 NAS16 <0.030 <0.030 <0.030 NAS17 <0.030 <0.030 <0.030 NAS18 <0.030 <0.030 <0.030 NA
a NA = not available. b duplicate samples.
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Table S13. Discharges of water and loads of ∑PFASs from Swedish rivers into the receiving sea
Sample ID River Discharge (Q) (m3 s-1) ƩPFASs (kg yr-1) Basin
R1 Torne älv 419a 30
Bothnian Bay
R2 Kalix älv 311a 16R3 Råne älv 43a 5.4R4 Lule älv 522a 28R5 Alterälven 4.5a 0.23R6 Pite älv 172a 40R7 Skellefte älv 164a 42R8 Rickleån 16a 0.65R9 Ume älv [Umeå] 440a 30
R10 Öre älv 35a 1.5R11 Lögde älv 20a 0.61R12 Gide älv 39a 2.2R13 Ångermanälven 485a 418
Bothnian Sea
R14 Indalsälven 438a 17R15 Ljungan 120a 6.1R16 Delångersån 16a 30R17 Ljusnan 216a 19R18 Gavleån 20a 6.8R19 Dalälven 353a 62R21 Norrström 166a 70R22 Nyköpingsån 237a 78
Baltic ProperR23 Motala ström 100a 13
R24 Botorpsström 6.7a 0.54
Sample ID River Discharge (Q) (m3 s-1) ƩPFASs (kg yr-1) Basin
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R25 Emån 34a 55R26 Alsterån 11a 0.98
R27 Ljungbyån 4.1a 0.72 Baltic Proper
R28 Lyckebyån 6.0a 1.1R29 Mörrumsån 31a 6.2R30 Helge Å 42a 36R31 Kävlingeån 11a 3.0
Kattegat
R32 Rönneån 11a 4.8R33 Lagan 81a 11R34 Nissan 47a 12R35 Ätran 57a 5.6R36 Viskan 43a 9.9R37 Göta älv [Alelyckan] 554a 82R38 Nordre älv 355a 38R39 Örekilsälven 24a 2.9R40 Enningdalsälven 12a 1.5
a data from Swedish meteorological institute (SMHI)2
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Table S14. Explained nariation (R2X and R2Y) from SIMCA® (Umetrics AB) modeling for PFASs and water chemistry, demographic, geographic and hydrological factors in Swedish rivers
Factor Number of components R2X (cumulative) R2Y (cumulative)
Catchment size 5 0.90 0.18
DOC 5 0.91 0.49
Flow 5 0.91 0.32
Latitude 5 0.92 0.72
Population density 5 0.92 0.67
Run-off 5 0.91 0.21
Total population 5 0.92 0.38
Water temperature 5 0.93 0.46
Latitude & population density 5 0.92 0.69
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100
Table S15. Explained variation (R2X and R2Y) from by SIMCA® (Umetrics AB) modeling for PFASs and water chemistry, geographic and hydrological factors in the Baltic Sea and the Kattegat
Factor Number of components R2X (cumulative) R2Y (cumulative)
DOC 5 0.98 0.75
Latitude 4 0.98 0.85
Salinity 5 0.98 0.93
Water temperature 5 0.98 0.67
DOC, latitude, salinity and
water temperature5 0.98 0.78
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Table S16. Coefficients of determination (R2) and p-values of Pearson correlation of PFCAs, PFSAs and DOC (log10-transformed data) in rivers and the recipient seas
Log DOC
Log PFBA
Log PFHxA
Log PFHpA
Log PFOA
Log PFNA
Log PFDA
Log PFUnDA
LogPFDoDA
Log PFBS
Log PFHxS
LogPFOS
Log DOC
R2 - 0.49 <0.1 0.44 0.30 <0.1 <0.1 <0.1 <0.1 0.11 0.24 <0.1p-value - <0.00001 0.32 <0.001 <0.0001 0.26 0.78 0.65 0.81 <0.05 <0.001 <0.05
Log PFBA
R2 0.49 - <0.1 0.21 0.27 <0.1 <0.1 <0.1 <0.1 0.21 <0.1 <0.1p-value <0.00001 - 0.59 <0.05 <0.0001 0.13 0.72 0.59 0.63 <0.05 0.060 0.18
Log PFHxA
R2 <0.1 <0.1 - <0.1 <0.1 0.31 0.18 0.38 0.46 <0.1 <0.1 <0.1p-value 0.32 0.59 - 0.77 0.57 0.062 0.16 <0.05 <0.05 0.97 0.70 0.61
Log PFHpA
R2 0.44 0.21 <0.1 - 0.52 <0.1 0.14 <0.1 <0.1 <0.1 <0.1 <0.1p-value <0.001 <0.05 0.77 - <0.0001 0.26 0.068 0.40 0.22 0.45 0.77 0.17
Log PFOA
R2 0.30 0.27 <0.1 0.52 - 0.20 0.30 0.16 0.13 <0.1 0.10 0.16p-value <0.0001 <0.0001 0.57 <0.0001 - <0.001 <0.001 <0.05 0.11 0.12 <0.05 <0.05
Log PFNA
R2 <0.1 <0.1 0.31 <0.1 0.20 - 0.58 0.74 0.53 <0.1 <0.1 <0.1p-value 0.26 0.13 0.062 0.26 <0.001 - <0.00001 <0.00001 <0.001 0.080 0.89 <0.05
Log PFDA
R2 <0.1 <0.1 0.18 0.14 0.30 0.58 - 0.81 0.87 <0.1 <0.1 <0.1p-value 0.78 0.72 0.16 0.068 <0.001 <0.00001 - <0.00001 <0.00001 0.67 0.21 1.00
Log PFUnDA
R2 <0.1 <0.1 0.38 <0.1 0.16 0.74 0.81 - 0.85 <0.1 0.12 <0.1p-value 0.65 0.59 <0.05 0.40 <0.05 <0.00001 <0.00001 - <0.00001 0.33 <0.05 0.33
Log PFDoDA
R2 <0.1 <0.1 0.46 <0.1 0.13 0.53 0.87 0.85 - <0.1 <0.1 <0.1p-value 0.81 0.63 <0.05 0.22 0.11 <0.001 <0.00001 <0.00001 - 0.30 0.21 0.72
Log PFBS
R2 0.11 0.21 <0.1 <0.1 <0.1 <0.1 <0.1 <0.1 <0.1 - 0.37 0.21p-value <0.05 <0.05 0.97 0.45 0.12 0.08 0.67 0.33 0.30 - <0.0001 <0.05
Log PFHxS
R2 0.24 <0.1 <0.1 <0.1 0.10 <0.1 <0.1 0.12 <0.1 0.37 - 0.82p-value <0.001 0.06 0.70 0.77 <0.05 0.89 0.21 <0.05 0.21 <0.0001 - <0.00001
LogPFOS
R2 <0.1 <0.1 <0.1 <0.1 0.16 <0.1 <0.1 <0.1 <0.1 0.21 0.82 -p-value <0.05 0.18 0.61 0.17 <0.05 <0.05 1.0 0.33 0.72 <0.05 <0.00001 -
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Table S17. Monthly DOC levels (mg L-1) for Swedish rivers (n = 40) during August to October, 2013
ID River Sampling date
Minimum sampling depth (m)
Maximum sampling depth (m)
DOC (mg L-1)
R1 Torne älv2013-08-14 0.5 1.1 4.52013-09-10 0.2 0.1 4.42013-10-17 0.5 1.1 4.6
R2 Kalix älv2013-08-14 0.5 1.1 3.72013-09-16 0.5 1.1 3.22013-10-14 0.5 1.1 5.0
R3 Råne älv2013-08-11 0.5 1.1 8.92013-09-15 0.5 1.1 8.22013-10-12 0.5 1.1 8.6
R4 Lule älv2013-08-19 0.5 1.1 2.92013-09-18 0.5 1.1 2.32013-10-21 0.0 0.1 2.8
R5 Alterälven2013-08-10 0.5 1.1 132013-09-15 0.5 1.1 112013-10-12 0.5 1.1 11
R6 Pite älv2013-08-10 0.5 1.1 3.02013-09-15 0.5 1.1 2.42013-10-12 0.5 1.1 3.3
R7 Skellefte älv2013-08-11 0.5 1.1 2.82013-09-16 0.5 1.1 3.32013-10-15 0.5 1.1 2.6
R8 Rickleån2013-08-18 0.5 1.1 122013-09-13 0.5 1.1 112013-10-14 0.5 1.1 12
R9 Ume älv2013-08-12 0.5 1.1 4.02013-09-18 0.5 1.1 3.32013-10-14 0.5 1.1 3.8
R9B Vindelälven2013-08-13 0.5 1.1 3.22013-09-16 0.5 1.1 3.22013-10-14 0.5 1.1 3.2
R10 Öre älv2013-08-19 0.5 1.1 122013-09-16 0.5 1.1 102013-10-14 0.5 1.1 15
R11 Lögde älv2013-08-14 0.5 1.1 8.32013-09-11 0.5 1.1 8.52013-10-16 0.5 1.1 9.8
R12 Gide älv2013-08-19 0.5 1.1 8.72013-09-16 0.5 1.1 8.32013-10-14 0.5 1.1 13
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ID River names Sampling date
Minimum sampling depth (m)
Maximum sampling depth (m)
DOC/TOC (mg/l)
R13 Ångermanälven2013-08-16 0.3 0.1 5.52013-09-16 0.3 0.1 4.12013-10-15 0.2 0.1 6.0
R14 Indalsälven2013-08-04 0.5 1.1 4.02013-09-05 0.5 1.1 3.92013-10-14 0.5 1.1 4.3
R15 Ljungaån2013-08-14 0.5 1.1 152013-09-18 0.1 0.1 102013-10-16 0.1 0.1 9.5
R16 Delångersån2013-08-12 0.5 1.1 6.92013-09-16 0.5 1.1 6.52013-10-14 0.5 1.1 6.4
R17 Ljusnan2013-08-16 0.5 1.1 2.92013-09-17 0.5 1.1 3.62013-10-16 0.5 1.1 1.6
R18 Gavleån2013-08-14 0.5 1.1 132013-09-15 0.5 1.1 132013-10-15 0.5 1.1 12
R19 Dalälven2013-08-13 0.5 1.1 7.42013-09-17 0.5 1.1 6.62013-10-16 0.5 1.1 5.6
R20 Fyrisån2013-08-12 0.5 1.1 162013-09-17 0.5 1.1 152013-10-16 0.5 1.1 14
R21 Norrström2013-08-19 0.1 0.1 242013-09-17 0.1 0.1 222013-10-15 0.1 0.1 20
R22 Nyköpingsån2013-08-14 0.5 1.1 142013-09-17 0.3 0.1 152013-10-15 0.1 0.1 13
R23 Motala Ström2013-08-19 0.5 1.1 8.12013-09-16 0.5 1.1 7.42013-10-17 0.5 1.1 7.1
R24 Botorpström2013-08-13 0.5 1.1 122013-09-16 0.5 1.1 122013-10-15 0.5 1.1 11
R25 Emån2013-08-15 0.5 1.1 132013-09-15 0.5 1.1 112013-10-14 0.5 1.1 10
R26 Alsterån2013-08-18 0.5 1.1 152013-09-15 0.5 1.1 132013-10-13 0.5 1.1 13
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ID River names Sampling date
Minimum sampling depth (m)
Maximum sampling depth (m)
DOC/TOC (mg/l)
R27 Ljungbyån2013-08-15 0.5 1.1 112013-09-18 0.5 1.1 9.72013-10-15 0.5 1.1 11
R28 Lyckebyån2013-08-19 0.5 1.1 162013-09-17 0.5 1.1 152013-10-14 0.5 1.1 14
R29 Mörrumsån2013-08-20 0.5 0.5 132013-09-18 0.5 0.5 122013-10-17 0.2 0.2 11
R30 Helgeån2013-08-22 0.5 1.1 142013-09-24 0.5 1.1 6.02013-10-17 0.5 1.1 9.0
R31 Kävlingeån2013-08-20 0.5 1.1 7.82013-09-18 0.5 1.1 7.52013-10-21 0.5 1.1 8.6
R32 Rönneån2013-08-20 0.5 1.1 112013-09-11 0.5 1.1 112013-10-17 0.5 1.1 10
R33 Lagan2013-08-14 0.1 0.1 132013-09-16 0.1 0.1 122013-10-15 0.1 0.1 10
R34 Nissan2013-08-13 0.2 0.1 122013-09-16 0.1 0.1 112013-10-14 0.1 0.1 10
R35 Ätran2013-08-13 0.2 0.1 8.62013-09-17 0.1 0.1 7.92013-10-14 0.1 0.1 9.2
R36 Viskan2013-08-19 0.5 1.1 8.32013-09-16 0.5 1.1 6.82013-10-21 0.5 1.1 7.3
R37 Göta Älv2013-08-15 0.5 1.1 4.72013-09-17 0.5 1.1 4.92013-10-15 0.5 1.1 4.9
R39 Örekilsälven2013-08-13 0.2 0.1 122013-09-10 0.2 0.1 122013-10-08 0.2 0.1 12
R40 Enningdalsälv2013-08-14 0.5 0.1 9.22013-09-17 0.3 0.1 9.32013-10-14 0.1 0.1 9.0
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Figure S1. Potential PFASs sources (red square, ■) of ten rivers with elevated PFASs
concentrations (black dots, ●)
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112
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Figure S2. PFOS concentrations of 44 river sites along Swedish coast. The dotted line represents the European annual average environmental standard (AA-EQS) value for inland surface water
(0.65 ng L-1)
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115116117
Figure S3. PFOS concentrations of 18 sites in the Baltic Sea and the Kattegat. The dotted line represents the European annual average environmental standard (AA-EQS) value for sea water
(0.13 ng L-1)
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119120121
Figure S4. Biplot of principal component analysis (PCA) of PFAS concentrations (log10-transformed, orange diamonds), latitude (not log10-
transformed, green squares), and DOC (not log10-transformed, green squares) of the river (n = 44) and seawater samples (n = 18) (black round
dots).
References
URL1, Swedish meteorological and hydrological institute, website; http://vattenwebb.smhi.se/, 2016 September 20
Wang Z, MacLeod M, Cousins I, Scheringer M and Hungerbühler K., 2011. Using COSMOtherm to predict physicochemical properties of poly- and perfluorinated alkyl substances (PFASs). Environmental Chemistry 8, 389-398.
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