Re-analysed time series

Additional file 7 Re-analysed time series Supplementary information to What is the effect of phasing out long-chain per- and polyfluoroalkyl substances on the concentrations of perfluoroalkyl acids and their precursors in the environment? A systematic review Magnus Land 1)*, Cynthia A. de Wit 2), Anders Bignert 3), Ian T. Cousins 2), Dorte Herzke 4), Jana H. Johansson 2), Jonathan W. Martin2, 5) 1) Mistra EviEM, Stockholm Environment Institute, Box 24218, SE-104 51 Stockholm, Sweden 2) Department of Environmental Science and Analytical Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden 3) Swedish Museum of Natural History, Box 50007, SE-104 05 Stockholm, Sweden 4) Norwegian Inst Air Res, FRAM High North Res Ctr Climate & Environm, Tromso, Norway 5) Division of Analytical and Environmental Toxicology, University of Alberta, Edmonton, Alberta Canada T6G 2G3 * Corresponding author 1

Reading instructions for figures in this supplementary information The figures in this additional file show calculated time trends for PFASs in human and environmental samples (see example figure below). To the left ( a bar plot shows study periods, and trend directions are indicated by colour codes. Datasets above the thick horizontal line were analysed for change-points. Other data sets provided less than 7 time points and were not analysed for change-points. Insignificant trends are defined as trends with a p-value >0.05 for the calculated slope of a regression line in a log-linear space. The power of insignificant trends refers to the chance of detecting an annual change of at least 10 % (please see main report for calculation methods). To the right ( a dot plot shows the annual relative change (in %). Where change-points occur the relative change is shown before as well as after the change-point. However, where the trend is insignificant on both sides of the change-point the magnitude is shown for the whole period only. Colour codes are the same in panel and, meaning that significance and power are indicated in both panels Bullet points before the dataset label indicate that time trend analysis was also performed in the original study (reference in square brackets) and that the results originally reported by the authors are shown in Additional file 8. For a full list of references see main article. An asterisk (*) after the reference number indicates low risk of bias according to the critical appraisal performed in the systematic review. No asterisk indicates medium risk of bias. Temporal data and interpretations of datasets A, B, C and D are shown on next page. A B C D Example figure. Temporal data for example datasets A, B, C and D are shown on next page. 2

0,3 Blood plasma (F, 20 29), Halle, Germany [88]* Change point ng/g ww 0,2 0,1 0 1994 1996 1998 2000 2002 2004 2006 2008 2010 Dataset A. No detected change point and no significant trend. The power to detect a trend is low which means that a trend may be present, but given the variability the dataset is insufficient to detect that. ng/g ww 0,4 0,3 0,2 0,1 Blood plasma (M, 20 29), Halle, Germany [88]* Change point 0 1994 1996 1998 2000 2002 2004 2006 2008 2010 Dataset B. A significant change point (CP) is detected, but the trends are insignificant with low power to detect a trend both before and after the CP. However, there is a significantly decreasing trend if the entire study period is considered (as indicated by the green marker in the example figure, page 2). Blood plasma (F, 20 29), Munster, Germany [88]* 0,6 Change point ng/g ww 0,4 0,2 0 1980 1985 1990 1995 2000 2005 2010 2015 Dataset C. A significant change point (CP) is detected. Before the CP the trend is insignificant and the power to detect a trend is high. It is therefore unlikely that there is a significant (undetected) trend before the CP. After the CP there is a significant increasing trend. ng/ml 0,15 0,1 0,05 Blood serum (F, 18 52), Busan, Korea [29] Change point 0 1992 1994 1996 1998 2000 2002 2004 2006 2008 2010 Dataset D. No change point analysis was performed (<7 time points). There is no significant trend and the power to detect a trend is low. 3

List of Figures Figure 1. Figure 2. Figure 3. Figure 4. Figure 5. Figure 6. Figure 7. Figure 8. Figure 9. Figure 10. Figure 11. Figure 12. Figure 13. Figure 14. Figure 15. Figure 16. Figure 17. Figure 18. Figure 19. Figure 20. Figure 21. Figure 22. Figure 23. Figure 24. Figure 25. Figure 26. Figure 27. Figure 28. Figure 29. Figure 30. Figure 31. Figure 32. Figure 33. Figure 34. Figure 35. Figure 36. Figure 37. Figure 38. Figure 39. Figure 40. Figure 41. Figure 42. PFBS in all samples PFHxS in human samples PFHxS in terrestrial and freshwater samples PFHxS in coastal and marine mammals PFHxS in coastal and marine biological samples PFHxS in abiotic samples PFOS in human samples PFOS in terrestrial and freshwater samples PFOS in coastal and marine mammals PFOS in coastal and marine biological samples PFOS in abiotic samples PFDS in all samples PFHpA in human samples PFHpA in biological and abiotic samples PFOA in human samples PFOA in all biological samples PFOA in abiotic samples PFNA in human samples PFNA in terrestrial and freshwater samples PFNA in coastal and marine mammals PFNA in coastal and marine biological samples PFNA in abiotic samples PFDA in human samples PFDA in terrestrial and freshwater samples PFDA in coastal and marine mammals PFDA in coastal and marine biological samples PFDA in abiotic samples PFUnDA in human samples PFUnDA in terrestrial and freshwater samples PFUnDA in coastal and marine mammals PFUnDA in coastal and marine biological samples PFUnDA in abiotic samples PFDoDA in human samples PFDoDA in terrestrial and freshwater samples PFDoDA in all coastal and marine biological samples PFDoDA in abiotic samples PFTrDA in human samples PFTrDA in all biological samples PFTrDA in abiotic samples PFTeDA in all samples PFOSA in human samples and terrestrial and freshwater biol. samples PFOSA in all coastal and marine samples 4

PFBS Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Grey seal (Juvenile), Bal c Sea, Sweden [106] Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring (F+M, Young (muscle)), Ka egat, Sweden [139]* Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Sediment, Core 1, China [122]* Blood serum (F, 21-41), Uppsala sub, Sweden [88] Blood serum (F, 21-41), Uppsala 1, Sweden [88] Blood serum (F, 21-41), Uppsala 3, Sweden [88] Herring (F+M, Young (liver)), Ka egat, Sweden [139]* Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] 1960 1970 1980 1990 2000 2010-10 0 10 20 Fig 1. Calculated time trends for PFBS in all samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHxS Blood plasma (F, 20-29), Halle, Germany [145]* Blood plasma (M, 20-29), Halle, Germany [145]* Blood plasma (F+M, 20-29), Munster, Germany [130]* Blood plasma (F, 20-29), Munster, Germany [145]* Blood plasma (M, 20-29), Munster, Germany [145]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 36-56), Lund, Sweden [68] Milk (F, Primiparous), Stockholm, Sweden [137]* Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Milk (F, 19-41), 4 ci es, Sweden [102]* whole blood (F+M, Infants), NY, USA [135]* Cow (F, ), Sweden, Na onwide [99]* Hen (egg), Sweden, Na onwide [99]* Rainbow trout (>1 yr), Sweden, Na onwide [99]* Blood serum (F+M, All), Australia, Na onwide [138] Blood serum (F+M, ), Arnsberg, Germany [143]* Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (M, age n.r.), Tromsö, Norway [115]* Blood serum (F, 21-41), Uppsala sub, Sweden [88] Blood serum (F, 21-41), Uppsala 1, Sweden [88] Blood serum (F, 21-41), Uppsala 3, Sweden [88] Whole blood (M, 53-79), Örebro, Sweden [69] Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Blood serum (M, >12), NHANES, USA [103]* Blood serum (F, >12), NHANES, USA [103]* Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010-10 0 10 20 Fig 2. Calculated time trends for PFHxS in human samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHxS O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Great blue heron (egg), Pig's Eye Colony, USA [76] 1970 1980 1990 2000 2010-10 0 10 20 30 40 Fig 3. Calculated time trends for PFHxS in terrestrial and freshwater samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHxS Polar Bear (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Harbor porpoise (F, <3,5), North Sea, Germany [96]* Ringed seal (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Ringed seal (F+M?, <6 years), Qeqertarsuaq, Greenland [124]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Ringed seal (F+M, 1-8), I oqqortoormiit, Greenland [71]* Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] 118 Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] 59 1965 1975 1985 1995 2005-10 0 10 20 Fig 4. Calculated time trends for PFHxS in coastal and marine mammals. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHxS Double-crested cormorant (egg), Mandarte Island, Canada Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (egg), Heuwiese, Germany [128] Herring gull (egg), Mellum, Germany [128] Herring gull (egg), Trischen, Germany [128] Eelpout (F+M, age n.r.), Meldorf Bay, Germany [128] Eelpout (F+M, age n.r.), Varel-Mellum, Germany [128] Herring (F+M, Young (muscle)), Ka egat, Sweden [139]* Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] Herring (F+M, Young (liver)), Ka egat, Sweden [139]* 1965 1975 1985 1995 2005-20 0 20 40 60 Fig 5. Calculated time trends for PFHxS in coastal and marine biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHxS Sediment, Core A, Japan [66]* Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] 1960 1970 1980 1990 2000 2010-30 -20-10 0 10 Fig 6. Calculated time trends for PFHxS in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOS Insigni cant, Power >0.8 Insigni cant, Power <0.8 Blood plasma (F, 20-29), Halle, Germany [145]* Blood plasma (M, 20-29), Halle, Germany [145]* Blood plasma (F+M, 20-29), Munster, Germany [130]* Blood plasma (F, 20-29), Munster, Germany [145]* Blood plasma (M, 20-29), Munster, Germany [145]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 36-56), Lund, Sweden [68] Milk (F, Primiparous), Stockholm, Sweden [137]* Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Milk (F, 19-41), 4 ci es, Sweden [102]* whole blood (F+M, Infants), NY, USA [135]* Cow (F, ), Sweden, Na onwide [99]* Hen (egg), Sweden, Na onwide [99]* Rainbow trout (>1 yr), Sweden, Na onwide [99]* Blood serum (F+M, All), Australia, Na onwide [138] Blood serum (F+M, ), Shenyang, China [98] Blood serum (F+M, ), Arnsberg, Germany [143]* Blood plasma (F, 20-29), Munster, Germany [130]* Blood plasma (M, 20-29), Munster, Germany [130]* Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (M, 20-59), Kyoto, Japan [89] Blood serum (F, 20-59), Kyoto, Japan [89] Blood serum (M, age n.r.), Tromsö, Norway [115]* Whole blood (M, 53-79), Örebro, Sweden [69] Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Blood serum (F, age n.r.), California, USA [121] Blood serum (M, 12-19), NHANES, USA [144]* Blood serum (M, 20-29), NHANES, USA [144]* Blood serum (M, 30-39), NHANES, USA [144]* Blood serum (M, 40-49), NHANES, USA [144]* Blood serum (M, 50-59), NHANES, USA [144]* Blood serum (M, 60-69), NHANES, USA [144]* Blood serum (M, 70-79), NHANES, USA [144]* Blood serum (M, >80), NHANES, USA [144]* Blood serum (F, 12-19), NHANES, USA [144]* Blood serum (F, 20-29), NHANES, USA [144]* Blood serum (F, 30-39), NHANES, USA [144]* Blood serum (F, 40-49), NHANES, USA [144]* Blood serum (F, 50-59), NHANES, USA [144]* Blood serum (F, 60-69), NHANES, USA [144]* Blood serum (F, 70-79), NHANES, USA [144]* Blood serum (F, >80), NHANES, USA [144]* Blood serum (M, >12), NHANES, USA [103]* Blood serum (F, >12), NHANES, USA [103]* Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010-40 -20 0 20 40 60 Figure 7. Calculated time trends for PFOS in human samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOS Roe Deer (1), ESB sampling sites, Germany [79]* O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Great blue heron (egg), Pig's Eye Colony, USA [76] 1965 1975 1985 1995 2005-10 0 10 20 30 40 Figure 8. Calculated time trends for PFOS in terrestrial and freshwater samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOS Polar Bear (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Polar Bear (3-5), I oqqortoormiit, Greenland [77]* Polar bear (F+M, Liver), Central East Greenland, Greenland [134] Polar bear (F+M, Kidney), Central East Greenland, Greenland [134] Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor porpoise (F+M, 0-21), North Sea, Denmark [82] Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Ringed seal (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Ringed seal (F+M?, <6 years), Qeqertarsuaq, Greenland [124]* Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Northern Sea O ers (M, 1+ yr), South-central Alaska, USA [42] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Harbor Seal (age n.r.), Gulf of Maine, USA [131] Polar Bear (F+M, Mainly adult), Barrow, North American arc c [132] Polar Bear (F+M, Mainly adult), Ba n Island, North American arc c [132] Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Ringed seal (F+M, 1-8), I oqqortoormiit, Greenland [71]* Ringed seal (F+M, 1-3), Qeqertarsuaq, Greenland [71]* Melon-headed Whale (F+M, age n.r.), East coast, Japan [91] Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] 75 Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] 1965 1975 1985 1995 2005-20 -10 0 10 20 30 Figure 9. Calculated time trends for PFOS in coastal and marine mammals. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOS Double-crested cormorant (egg), Mandarte Island, Canada Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (Egg), Heuwiese, Germany [80]* Herring gull (egg), Heuwiese, Germany [128] Herring gull (egg), Heuwiese, Germany [105]* White-tailed sea eagle (age n.r.), Bal c Sea coast, Germany [100] Herring gull (Egg), Mellum, Germany [80]* Herring gull (Egg), Trischen, Germany [80]* Herring gull (egg), Mellum, Germany [128] Herring gull (egg), Trischen, Germany [128] Herring gull (egg), Mellum, Germany [105]* Herring gull (egg), Trischen, Germany [105]* Guillemot (egg), Stora karlsö, Sweden [94] Eelpout (F+M, age n.r.), Darsser Ort, Germany [128] Eelpout (F+M, age n.r.), Meldorf Bay, Germany [128] Eelpout (F+M, age n.r.), Varel-Mellum, Germany [128] Herring (F+M, Young (muscle)), Ka egat, Sweden [139]* Eel (age n.r.), Haringvliet East, The Netherlands [107]* Eel (age n.r.), Hollands Diep, The Netherlands [107]* Eel (age n.r.), Lobith, The Netherlands [107]* Mussel (age n.r.), Seine estuary, France [113]* Bluse mussel (F+M, age n.r.), Darsser Ort, Germany [128] Bluse mussel (F+M, age n.r.), Eckwardershörne, Germany [128] Bluse mussel (F+M, age n.r.), Königshafen, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada Herring (F+M, Young (liver)), Ka egat, Sweden [139]* 1965 1975 1985 1995 2005-20 0 20 40 60 Figure 10. Calculated time trends for PFOS in coastal and marine biological samples samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOS Water, Tokyo Bay, Japan [129]* Ice, Core 1, Svalbard [37] Snow, Mt Muztagata, Tibet [38]* Snow, Devon ice cap, Canada [148] Sediment, Kempenfeldt bay, Canada [93] Sediment, Sta on 1004, Canada/USA [147]* Sediment, Sta on 1034, Canada/USA [147]* Sediment, Sta on 1046, Canada/USA [147]* Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S6, China [149] Sediment, Haihe River, S8, China [149] Sediment, M009, USA [75]* Sediment, M050, USA [75]* Sediment, Core A, Japan [66]* WRRF biosolids, Mid-Antlan c USA, USA [67] Freshwater, West coast, South Korea [95] Surface water, Bohai Bay, China [140] Bo om water, Bohai Bay, China [140] Seawater, West coast, South Korea [95] Sediment, Bohai Bay, China [140] Sewage treatment e uent, Tokyo, Japan [114] Sewage sludge, Die kon, Switzerland [136]* Sewage sludge, Hinwil, Switzerland [136]* Sewage sludge, Horgen, Switzerland [136]* Sewage sludge, Niedergla, Switzerland [136]* Sewage sludge, Winterthur, Switzerland [136]* 1970 1980 1990 2000 2010-40 -30-20 -10 0 10 20 Figure 11. Calculated time trends for PFOS in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDS Blood plasma (F, 20-29), Halle, Germany [145]* Blood plasma (M, 20-29), Halle, Germany [145]* Blood plasma (M, 20-29), Munster, Germany [145]* Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Double-crested cormorant (egg), Mandarte Island, Canada Great blue heron (egg), Fraser River, Canada Herring (F+M, Young (muscle)), Ka egat, Sweden [139]* Sediment, Core 1, China [122]* Sediment, Core A, Japan [66]* WRRF biosolids, Mid-Antlan c USA, USA [67] Great blue heron (egg), Pig's Eye Colony, USA [76] Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] Herring (F+M, Young (liver)), Ka egat, Sweden [139]* Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] 1970 1980 1990 2000 2010 0 20 40 Figure 12. Calculated time trends for PFDS in all samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHpA Blood plasma (F, 20-29), Halle, Germany [146]* Blood plasma (M, 20-29), Halle, Germany [146]* Blood plasma (F, 20-29), Munster, Germany [146]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Cow (F, ), Sweden, Na onwide [99]* Blood serum (F, 18-52), Busan, Korea [90] Blood serum (M, age n.r.), Tromsö, Norway [115]* Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Dietary exposure, Sweden, Na onwide [142]* 1975 1980 1985 1990 1995 2000 2005 2010-20 -10 0 10 20 30 Figure 13. Calculated time trends for PFHpA in human and food samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFHpA Grey seal (Juvenile), Bal c Sea, Sweden [106] Snow, Coll Gnife, Italy [104] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* WRRF biosolids, Mid-Antlan c USA, USA [67] Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] Sewage treatment e uent, Tokyo, Japan [114] Category D, USA, Na onwide [108] Category E, USA, Na onwide [108] Category F, USA, Na onwide [108] Category G, USA, Na onwide [108] Category H, USA, Na onwide [108] Category I, USA, Na onwide [108] 1960 1970 1980 1990 2000 2010-80 -60-40 -20 0 20 40 Figure 14. Calculated time trends for PFHpA in biological and abiotic samples samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3. Product categories in this and other figures are as follows: Category B Commercial carpet/fabric-care liquids Category C Household carpet/fabric-care liquids and foams Category D Treated apparel Category E Treated home textile and upholstery Category F Treated non-woven medical garments Category G Treated floor waxes and stone/wood sealants Category H Treated food contact paper Category I Membranes for apparel Category J Thread-sealant tapes and pastes

PFOA Blood plasma (F, 20-29), Halle, Germany [146]* Blood plasma (M, 20-29), Halle, Germany [146]* Blood plasma (F+M, 20-29), Munster, Germany [130]* Blood plasma (F, 20-29), Munster, Germany [146]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 36-56), Lund, Sweden [68] Milk (F, Primiparous), Stockholm, Sweden [137]* Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* whole blood (F+M, Infants), NY, USA [135]* Hen (egg), Sweden, Na onwide [99]* Blood serum (F+M, All), Australia, Na onwide [138] Blood serum (F+M, ), Shenyang, China [98] Blood serum (F+M, ), Arnsberg, Germany [143]* Blood plasma (F, 20-29), Munster, Germany [130]* Blood plasma (M, 20-29), Munster, Germany [130]* Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (M, 20-59), Kyoto, Japan [89] Blood serum (F, 20-59), Kyoto, Japan [89] Blood serum (F, 18-52), Busan, Korea [90] Blood serum (M, age n.r.), Tromsö, Norway [115]* Whole blood (M, 53-79), Örebro, Sweden [69] Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Blood serum (F, age n.r.), California, USA [121] Blood serum (M, >12), NHANES, USA [103]* Blood serum (F, >12), NHANES, USA [103]* Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010 0 20 40 Figure 15. Calculated time trends for PFOA in human and food samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOA Roe Deer (1), ESB sampling sites, Germany [79]* O er (F+M, Juvenile to adult), Southern, Sweden [125]* Great blue heron (egg), Fraser River, Canada Tawny Owl (egg), Trondheim, Norway [11]* Polar Bear (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Polar Bear (3-5), I oqqortoormiit, Greenland [77]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Ringed seal (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Ringed seal (F+M?, <6 years), Qeqertarsuaq, Greenland [124]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Double-crested cormorant (egg), Mandarte Island, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (Egg), Heuwiese, Germany [80]* Herring gull (egg), Heuwiese, Germany [128] Herring gull (egg), Mellum, Germany [128] Herring gull (egg), Trischen, Germany [128] Eelpout (F+M, age n.r.), Darsser Ort, Germany [128] Eelpout (F+M, age n.r.), Meldorf Bay, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Polar Bear (F+M, Mainly adult), Barrow, North American arc c [132] Polar Bear (F+M, Mainly adult), Ba n Island, North American arc c [132] Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] Herring gull (egg), Röst, Norway [141] 1965 1975 1985 1995 2005-20 -10 0 10 20 30 40 Figure 16. Calculated time trends for PFOA in all biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFOA Water, Tokyo Bay, Japan [129]* Snow, Coll Gnife, Italy [104] Ice, Core 1, Svalbard [37] Snow, Mt Muztagata, Tibet [38]* Snow, Mt. Zuoqiupu, Tibet [38]* Snow, Devon ice cap, Canada [148] Sediment, Kempenfeldt bay, Canada [93] Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Sta on 1004, Canada/USA [147]* Sediment, Sta on 1034, Canada/USA [147]* Sediment, Sta on 1046, Canada/USA [147]* Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S6, China [149] Sediment, Haihe River, S8, China [149] Sediment, Core A, Japan [66]* WRRF biosolids, Mid-Antlan c USA, USA [67] Freshwater, West coast, South Korea [95] Surface water, Bohai Bay, China [140] Bo om water, Bohai Bay, China [140] Seawater, West coast, South Korea [95] Ice, Core 2, Svalbard [37] Sediment, Bohai Bay, China [140] Sewage treatment e uent, Tokyo, Japan [114] Sewage sludge, Die kon, Switzerland [136]* Sewage sludge, Hinwil, Switzerland [136]* Sewage sludge, Horgen, Switzerland [136]* Sewage sludge, Niedergla, Switzerland [136]* Sewage sludge, Winterthur, Switzerland [136]* Category B, USA, Na onwide [108] Category D, USA, Na onwide [108] Category E, USA, Na onwide [108] Category F, USA, Na onwide [108] Category G, USA, Na onwide [108] Category H, USA, Na onwide [108] Category I, USA, Na onwide [108] Category J, USA, Na onwide [108] 291 1960 1970 1980 1990 2000 2010-80 -60-40 -20 0 20 40 60 Figure 17. Calculated time trends for PFOA in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3. For explanation of product categories please see Figure 14.

PFNA Blood plasma (F, 20-29), Halle, Germany [146]* Blood plasma (M, 20-29), Halle, Germany [146]* Blood plasma (F, 20-29), Munster, Germany [146]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 36-56), Lund, Sweden [68] Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Milk (F, 19-41), 4 ci es, Sweden [102]* whole blood (F+M, Infants), NY, USA [135]* Hen (egg), Sweden, Na onwide [99]* Blood serum (F+M, All), Australia, Na onwide [138] Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (F, 18-52), Busan, Korea [90] Blood serum (M, age n.r.), Tromsö, Norway [115]* Whole blood (M, 53-79), Örebro, Sweden [69] Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Blood serum (F+M, >12), NHANES, USA [103]* Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010-10 0 10 20 30 40 Figure 18. Calculated time trends for PFNA in human and food samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFNA Roe Deer (1), ESB sampling sites, Germany [79]* O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Great blue heron (egg), Pig's Eye Colony, USA [76] 1970 1980 1990 2000 2010-5 0 5 10 15 Figure 19. Calculated time trends for PFNA in terrestrial and freshwater samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFNA Polar Bear (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Polar Bear (3-5), I oqqortoormiit, Greenland [77]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Ringed seal (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Ringed seal (F+M?, <6 years), Qeqertarsuaq, Greenland [124]* Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Northern Sea O ers (M, 1+ yr), South-central Alaska, USA [42] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Polar Bear (F+M, Mainly adult), Barrow, North American arc c [132] Polar Bear (F+M, Mainly adult), Ba n Island, North American arc c [132] Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Ringed seal (F+M, 1-8), I oqqortoormiit, Greenland [71]* Ringed seal (F+M, 1-3), Qeqertarsuaq, Greenland [71]* Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] 1960 1970 1980 1990 2000 2010 0 20 40 60 Figure 20. Calculated time trends for PFNA in coastal and marine mammals. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFNA Double-crested cormorant (egg), Mandarte Island, Canada Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (Egg), Heuwiese, Germany [80]* Herring gull (egg), Heuwiese, Germany [128] Herring gull (egg), Mellum, Germany [128] Herring gull (egg), Trischen, Germany [128] Eelpout (F+M, age n.r.), Darsser Ort, Germany [128] Eelpout (F+M, age n.r.), Meldorf Bay, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] 1960 1970 1980 1990 2000 2010-10 0 10 20 30 Figure 21. Calculated time trends for PFNA in coastal and marine biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFNA Snow, Coll Gnife, Italy [104] Ice, Core 1, Svalbard [37] Snow, Mt Muztagata, Tibet [38]* Snow, Mt. Zuoqiupu, Tibet [38]* Snow, Devon ice cap, Canada [148] Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S8, China [149] Sediment, Core A, Japan [66]* WRRF biosolids, Mid-Antlan c USA, USA [67] Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] Ice, Core 2, Svalbard [37] Sewage treatment e uent, Tokyo, Japan [114] Sewage sludge, Die kon, Switzerland [136]* Category B, USA, Na onwide [108] Category D, USA, Na onwide [108] Category E, USA, Na onwide [108] Category F, USA, Na onwide [108] Category G, USA, Na onwide [108] Category I, USA, Na onwide [108] 1960 1970 1980 1990 2000 2010-80 -60-40 -20 0 20 40 Figure 22. Calculated time trends for PFNA in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDA Blood plasma (F, 20-29), Halle, Germany [146]* Blood plasma (M, 20-29), Halle, Germany [146]* Blood plasma (F, 20-29), Munster, Germany [146]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 36-56), Lund, Sweden [68] Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Hen (egg), Sweden, Na onwide [99]* Blood serum (F+M, All), Australia, Na onwide [138] Blood plasma (F, 19-40), Hokkaido, Japan [118]* 108 Blood serum (F, 18-52), Busan, Korea [90] Blood serum (M, age n.r.), Tromsö, Norway [115]* Whole blood (M, 53-79), Örebro, Sweden [69] Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010-40 -20 0 20 Figure 23. Calculated time trends for PFDA in human and food samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDA Roe Deer (1), ESB sampling sites, Germany [79]* O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Great blue heron (egg), Pig's Eye Colony, USA [76] 1970 1980 1990 2000 2010 0 10 20 30 Figure 24. Calculated time trends for PFDA in terrestrial and freshwater samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDA Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor porpoise (F+M, 0-21), North Sea, Denmark [82] Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Ringed seal (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Ringed seal (F+M?, <6 years), Qeqertarsuaq, Greenland [124]* Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Eelpout (F+M, age n.r.), Meldorf Bay, Germany [128] Eelpout (F+M, age n.r.), Darsser Ort, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Polar Bear (F+M, Mainly adult), Barrow, North American arc c [132] Polar Bear (F+M, Mainly adult), Ba n Island, North American arc c [132] Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Ringed seal (F+M, 1-8), I oqqortoormiit, Greenland [71]* Ringed seal (F+M, 1-3), Qeqertarsuaq, Greenland [71]* Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] 1970 1980 1990 2000 2010-10 0 10 20 30 Figure 25. Calculated time trends for PFDA in coastal and marine mammals. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDA Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (Egg), Heuwiese, Germany [80]* Herring gull (egg), Heuwiese, Germany [128] Herring gull (egg), Mellum, Germany [128] Herring gull (egg), Trischen, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada Double-crested cormorant (egg), Mandarte Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] 1970 1980 1990 2000 2010 0 10 20 30 Figure 26. Calculated time trends for PFDA in coastal ansd marine biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDA Snow, Coll Gnife, Italy [104] Snow, Mt Muztagata, Tibet [38]* Snow, Mt. Zuoqiupu, Tibet [38]* Snow, Devon ice cap, Canada [148] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S6, China [149] Sediment, Haihe River, S8, China [149] Sediment, Core A, Japan [66]* Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] Sewage treatment e uent, Tokyo, Japan [114] Sewage sludge, Die kon, Switzerland [136]* Sewage sludge, Hinwil, Switzerland [136]* Sewage sludge, Horgen, Switzerland [136]* Sewage sludge, Niedergla, Switzerland [136]* Sewage sludge, Winterthur, Switzerland [136]* Category D, USA, Na onwide [108] Category E, USA, Na onwide [108] Category F, USA, Na onwide [108] Category G, USA, Na onwide [108] Category I, USA, Na onwide [108] 159 1960 1970 1980 1990 2000 2010-80 -60-40 -20 0 20 40 60 Figure 27. Calculated time trends for PFDA in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFUnDA Blood plasma (F, 20-29), Halle, Germany [146]* Blood plasma (M, 20-29), Halle, Germany [146]* Blood plasma (F, 20-29), Munster, Germany [146]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 36-56), Lund, Sweden [68] Blood serum (F, 19-41), Uppsala, Sweden [62]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Hen (egg), Sweden, Na onwide [99]* Rainbow trout (>1 yr), Sweden, Na onwide [99]* Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (F, 18-52), Busan, Korea [90] Blood serum (M, age n.r.), Tromsö, Norway [115]* Whole blood (M, 53-79), Örebro, Sweden [69] Blood plasma (F, 20-68), 6 ci es, USA [120]* Blood plasma (M, 20-68), 6 ci es, USA [120]* Blood plasma (F+M, 20-68), 6 ci es, USA [120]* Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010 0 20 40 60 Figure 28. Calculated time trends for PFUnDA in human and food samples samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFUnDA O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Great blue heron (egg), Pig's Eye Colony, USA [76] 1970 1980 1990 2000 2010 0 10 20 Figure 29. Calculated time trends for PFUnDA in terrestrial and freshwater samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFUnDA Polar Bear (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Polar Bear (3-5), I oqqortoormiit, Greenland [77]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor porpoise (F+M, 0-21), North Sea, Denmark [82] Ringed seal (F+M?, <6 years), I oqqortoormiit, Greenland [124]* Ringed seal (F+M?, <6 years), Qeqertarsuaq, Greenland [124]* Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Polar Bear (F+M, Mainly adult), Barrow, North American arc c [132] Polar Bear (F+M, Mainly adult), Ba n Island, North American arc c [132] Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Ringed seal (F+M, 1-8), I oqqortoormiit, Greenland [71]* Ringed seal (F+M, 1-3), Qeqertarsuaq, Greenland [71]* Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] 1960 1970 1980 1990 2000 2010 0 20 40 60 Figure 30. Calculated time trends for PFUnDA in coastal and marine mammals. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFUnDA Double-crested cormorant (egg), Mandarte Island, Canada Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (Egg), Heuwiese, Germany [80]* Herring gull (egg), Heuwiese, Germany [128] Herring gull (egg), Mellum, Germany [128] Herring gull (egg), Trischen, Germany [128] Eelpout (F+M, age n.r.), Darsser Ort, Germany [128] Eelpout (F+M, age n.r.), Meldorf Bay, Germany [128] Eelpout (F+M, age n.r.), Varel-Mellum, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] 1970 1980 1990 2000 2010-10 0 10 20 Figure 31. Calculated time trends for PFUnDA in coastal and marine biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFUnDA Snow, Coll Gnife, Italy [104] Snow, Mt Muztagata, Tibet [38]* Snow, Devon ice cap, Canada [148] Sediment, Kempenfeldt bay, Canada [93] Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S6, China [149] Sediment, Haihe River, S8, China [149] Sediment, Core A, Japan [66]* Freshwater, West coast, South Korea [95] Seawater, West coast, South Korea [95] Sewage treatment e uent, Tokyo, Japan [114] 100 Sewage sludge, Die kon, Switzerland [136]* Sewage sludge, Hinwil, Switzerland [136]* Sewage sludge, Horgen, Switzerland [136]* Sewage sludge, Niedergla, Switzerland [136]* Sewage sludge, Winterthur, Switzerland [136]* Category B, USA, Na onwide [108] Category D, USA, Na onwide [108] Category E, USA, Na onwide [108] Category F, USA, Na onwide [108] Category I, USA, Na onwide [108] 1960 1970 1980 1990 2000 2010-80 -60-40 -20 0 20 Figure 32. Calculated time trends for PFUnDA in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3. For explanation of product categories please see Figure 14.

PFDoDA Blood serum (M, 40-50), Norway, Na onwide [92]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Hen (egg), Sweden, Na onwide [99]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (F, 18-52), Busan, Korea [90] Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010-10 0 10 20 30 40 Figure 33. Calculated time trends for PFDoDA in human and food samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDoDA O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Great blue heron (egg), Pig's Eye Colony, USA [76] 1970 1980 1990 2000 2010 0 5 10 15 Figure 34. Calculated time trends for PFDoDA in terrestrial and freshwater samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDoDA Polar Bear (3-5), I oqqortoormiit, Greenland [77]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Herring gull (Egg), Heuwiese, Germany [80]* Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] 1960 1970 1980 1990 2000 2010-40 -20 0 20 40 60 Figure 35. Calculated time trends for PFDoDA in all coastal and marine biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFDoDA Snow, Coll Gnife, Italy [104] Snow, Mt Muztagata, Tibet [38]* Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S6, China [149] Sediment, Haihe River, S8, China [149] Sediment, Core A, Japan [66]* Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Haihe River, S6, China [149] Sediment, Haihe River, S8, China [149] Sewage sludge, Die kon, Switzerland [136]* Sewage sludge, Hinwil, Switzerland [136]* Sewage sludge, Horgen, Switzerland [136]* Sewage sludge, Niedergla, Switzerland [136]* Sewage sludge, Winterthur, Switzerland [136]* Category D, USA, Na onwide [108] Category E, USA, Na onwide [108] Category F, USA, Na onwide [108] Category I, USA, Na onwide [108] 1960 1970 1980 1990 2000 2010-80 -60-40 -20 0 20 40 Figure 36. Calculated time trends for PFDoDA in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFTrDA Blood plasma (F, 20-29), Halle, Germany [146]* Blood plasma (M, 20-29), Halle, Germany [146]* Blood plasma (F, 20-29), Munster, Germany [146]* Blood plasma (M, 20-29), Munster, Germany [146]* Blood serum (M, 40-50), Norway, Na onwide [92]* Hen (egg), Sweden, Na onwide [99]* Blood serum (F, 19-42), Uppsala, Sweden [85]* Blood plasma (F, 19-40), Hokkaido, Japan [118]* Blood serum (F, 18-52), Busan, Korea [90] Dietary exposure, Sweden, Na onwide [142]* 1970 1980 1990 2000 2010 0 20 40 60 80 Figure 37. Calculated time trends for PFTrDA in human and food samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFTrDA O er (F+M, Juvenile to adult), Southern, Sweden [125]* Polar Bear (3-5), I oqqortoormiit, Greenland [77]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Double-crested cormorant (egg), Mandarte Island, Canada Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Lake trout (F+M, age n.r.), Western Lake Ontario, Canada [86]* Eelpout (F+M, age n.r.), Darsser Ort, Germany [128] Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Pilot Whale (M, age n.r.), Faroe Islands, North Atlan c [126] Ringed Seal (F+M, age n.r.), Ba n Bay, Greenland [126] Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada Herring gull (egg), Hornoya, Norway [141] Herring gull (egg), Röst, Norway [141] 1960 1970 1980 1990 2000 2010-20 -10 0 10 20 30 Figure 38. Calculated time trends for PFTrDA in all biological samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFTrDA Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sewage sludge, Winterthur, Switzerland [136]* 1960 1970 1980 1990 2000 2010-10 0 10 20 Figure 39. Calculated time trends for PFTrDA in abiotic samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.

PFTeDA Hen (egg), Sweden, Na onwide [99]* O er (F+M, Juvenile to adult), Southern, Sweden [125]* Tawny Owl (egg), Trondheim, Norway [11]* Peregrine falcon (egg), Sweden, Na onwide [12]* Harbor porpoise (F, <3,5), Bal c Sea, Germany [96]* Harbor Seal (F+M, <7-19 months), German Bight, Germany [65] Harbor porpoise (F, <3,5), North Sea, Germany [96]* Grey seal (Juvenile), Bal c Sea, Sweden [106] Great blue heron (egg), Fraser River, Canada Northern fulmar (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Thick-billed murre (egg), Prince Leopold Island, Lancaster Sound, Canada [40]* Loggerhead sea turtle (F+M?, juvenile), Charleston, SC, USA [116]* Sediment, Lake Oesa, Canada [70] Sediment, Lake Opabin, Canada [70] Sediment, Core 1, China [122]* Sediment, Core 2, China [122]* Sediment, Core 3, China [122]* Sediment, Core A, Japan [66]* Dietary exposure, Sweden, Na onwide [142]* Beluga Whale (F+M, age n.r.), Cook inlet, USA [123]* Beluga Whale (F+M, age n.r.), Eastern Chukchi Sea, USA [123]* Bo lenose Dolphin (F+M, 4-26), IRL, USA [78] Bo lenose Dolphin (F+M, 3-33), CHS, USA [78] Rhinoceros auklet (egg), Cleland Island, Canada Rhinoceros auklet (egg), Lucy Island, Canada Leach s storm petrel (egg), Cleland Island, Canada Leach s storm petrel (egg), Hippa Island, Canada 109 88 1960 1970 1980 1990 2000 2010 0 10 20 Figure 40. Calculated time trends for PFTeDA in all samples. Study period and direction of trend. Magnitude of annual change. For further details please see page 2-3.