Title: Spatial and Temporal Trends of Metals and Arsenic in German Freshwater Compartments

Electronic Supplementary Material

Title: Spatial and temporal trends of metals and arsenic in German freshwater compartments

Journal: Environmental Science and Pollution Research (ESPR)

Authors: Annette Fliedner*, Heinz Rüdel, Burkhard Knopf, Karlheinz Weinfurtner, Martin Paulus, Mathias Ricking, Jan Koschorreck

*Fraunhofer Institute for Molecular Biology and Applied Ecology (Fraunhofer IME), 57392 Schmallenberg, Germany

Table S1: Metals and arsenic in suspended particulate matter from the German ESB sampling sites, sampling period: 2005 – 2009 (exceptions: Danube: 2009; Saar: 2006-2009). Concentrations are given as µg/g dry weight. The highest mean value of every element is written in bold letters.

Water / Sampling site / Value / Arsenic / Lead / Cadmium / Mercury / Copper / Nickel / Zinc
Danube / D1
UIm / Range / 6.96 / 25.38 / 0.54 / 148.7 / 36.68 / 26.52 / 171.0
Median / 6.96 / 25.38 / 0.54 / 148.7 / 36.68 / 26.52 / 171.0
Mean / n.d. / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
SD / n.d. / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
D2
Kelheim / Range / 9.01 / 23.37 / 0.34 / 222.0 / 41.20 / 28.13 / 180.3
Median / 9.01 / 23.37 / 0.34 / 222.0 / 41.20 / 28.13 / 180.3
Mean / n.d. / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
SD / n.d. / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
D3
Jochenstein / Range / 11.74 / 19.77 / 0.25 / 133.7 / 37.68 / 35.88 / 112.5
Median / 11.74 / 19.77 / 0.25 / 133.7 / 37.68 / 35.88 / 112.5
Mean / n.d. / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
SD / n.d. / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
Elbe / E1
Prossen / Range / 23.48- 38.58 / 68.05-113.3 / 1.66-3.06 / 790.0-1580 / 69.28-124.0 / 33.48-69.50 / 388.0-633.0
Median / 24.60 / 71.18 / 1.90 / 918.7 / 82.62 / 43.82 / 444.5
Mean / 27.38 / 81.05 / 2.06 / 1100 / 89.88 / 46.71 / 464.6
SD / 6.38 / 18.98 / 0.57 / 327.5 / 21.39 / 13.54 / 98.26
E2
Zehren / Range / 16.67-31.12 / 33.92-84.80 / 1.34-6.51 / 212.8-1039 / 29.22-87.32 / 15.65-59.50 / 229.5-773.8
Median / 25.15 / 56.53 / 3.36 / 649.7 / 67.82 / 35.52 / 588.5
Mean / 24.69 / 61.08 / 3.81 / 665.0 / 62.21 / 37.13 / 539.9
SD / 6.37 / 19.75 / 1.90 / 314.2 / 21.80 / 15.61 / 203.1
E3
Barby / Range / 14.82-27.95 / 93.50-122.5 / 3.12-4.90 / 1725-2850 / 80.50-101.3 / 33.78-45.88 / 725.5-1075
Median / 18.36 / 104.5 / 3.35 / 2065 / 86.67 / 36.32 / 867.0
Mean / 20.80 / 106.1 / 3.79 / 2099 / 87.90 / 38.24 / 863.1
SD / 5.48 / 12.38 / 0.82 / 455.6 / 8.02 / 4.93 / 135.2
E4
Cumlosen / Range / 20.30-24.68 / 49.87-71.85 / 2.38-8.63 / 1418-1925 / 62.12-81.05 / 19.62-32.92 / 441.8-640.2
Median / 20.72 / 62.23 / 3.62 / 1512 / 66.26 / 28.94 / 584.4
Mean / 22.09 / 62.15 / 4.39 / 1578 / 68.35 / 28.05 / 548.6
SD / 2.13 / 8.17 / 2.44 / 201.3 / 7.59 / 5.38 / 87.13

Table S1 (cont.): Metals and arsenic in suspended particulate matter from the German ESB sampling sites, sampling period: 2005 – 2009 (exceptions: Danube: 2009; Saar: 2006-2009). Concentrations are given as µg/g dry weight. The highest mean value of every element is written in bold letters.

Water / Sampling site / Value / Arsenic / Lead / Cadmium / Mercury / Copper / Nickel / Zinc
Elbe / E5
Blankenese / Range / 17.65-20.15 / 39.82-52.60 / 0.24-5.49 / 785.2-996.5 / 40.92-49.80 / 22.13-27.33 / 244.3-341.5
Median / 19.45 / 44.00 / 1.47 / 929.0 / 42.00 / 23.35 / 290.3
Mean / 19.26 / 45.77 / 2.10 / 903.1 / 44.01 / 24.47 / 297.3
SD / 0.97 / 5.29 / 1.99 / 80.06 / 3.68 / 2.60 / 43.44
Mulde / MU
Dessau / Range / 91.48-111.5 / 125.8-150.5 / 9.13-12.33 / 956.0-1393 / 61.03-73.72 / 51.52-82.45 / 391.5-1043
Median / 106.3 / 137.0 / 10.21 / 1258 / 65.45 / 69.93 / 739.2
Mean / 101.9 / 138.5 / 10.61 / 1205 / 66.09 / 68.87 / 760.3
SD / 9.42 / 9.56 / 1.37 / 186.5 / 5.13 / 13.32 / 265.4
Saale / SA
Wettin / Range / 11.60-19.13 / 66.82-90.97 / 0.63-10.05 / 2078-4095 / 76.78-105.0 / 42.43-62.08 / 457.0-712.7
Median / 12.83 / 77.63 / 2.81 / 2342 / 86.03 / 53.88 / 555.3
Mean / 14.04 / 78.02 / 3.74 / 2674 / 89.58 / 53.13 / 563.1
SD / 3.02 / 8.67 / 3.65 / 812.0 / 11.21 / 7.18 / 106.9
Rhine / R1
Weil / Range / 6.70-8.33 / 19.23-25.48 / 0.09-0.35 / 84.07-169.5 / 28.37-33.07 / 19.07-28.93 / 90.75-112.7
Median / 7.56 / 24.82 / 0.16 / 158.3 / 31.00 / 25.08 / 95.52
Mean / 7.45 / 23.37 / 0.19 / 135.7 / 30.81 / 24.31 / 98.87
SD / 0.61 / 2.59 / 0.10 / 39.49 / 2.24 / 3.95 / 8.41
R2
Iffezheim / Range / 8.07-9.66 / 24.13-29.03 / 0.23-0.45 / 212.7-275.5 / 40.10-45.37 / 24.17-34.00 / 120.3-133.8
Median / 9.15 / 28.53 / 0.29 / 243.8 / 42.53 / 33.30 / 129.5
Mean / 9.01 / 27.35 / 0.31 / 243.0 / 42.73 / 30.53 / 127.3
SD / 0.61 / 2.18 / 0.08 / 24.29 / 2.02 / 4.45 / 5.53
R3
Koblenz / Range / 7.80-9.63 / 22.10-29.72 / 0.19-0.48 / 199.8-258.3 / 30.87-38.83 / 19.52-28.92 / 117.2-153.0
Median / 7.99 / 24.80 / 0.25 / 210.7 / 35.13 / 22.55 / 139.0
Mean / 8.42 / 25.21 / 0.29 / 219.4 / 35.46 / 23.76 / 136.8
SD / 0.79 / 2.85 / 0.11 / 22.66 / 3.32 / 3.58 / 12.98
R4
Bimmen / Range / 11.70-12.45 / 47.05-57.33 / 0.67-1.70 / 353.5-552.0 / 46.47-59.10 / 26.98-37.15 / 281.0-588.5
Median / 11.97 / 51.12 / 0.85 / 391.5 / 52.95 / 35.33 / 284.8
Mean / 12.04 / 51.45 / 0.96 / 413.4 / 52.43 / 33.71 / 344.1
SD / 0.35 / 3.81 / 0.43 / 79.05 / 4.69 / 4.22 / 136.6

Water / Sampling site / Value / Arsenic / Lead / Cadmium / Mercury / Copper / Nickel / Zinc
Saar / S1
Güdingen / Range / 8.78-11.97 / 43.15-58.78 / 0.72-1.21 / 163.2-313.2 / 49.35-68.33 / 26.75-35.47 / 284.3-391.5
Median / 10.49 / 51.24 / 0.86 / 167.4 / 51.74 / 33.22 / 365.8
Mean / 10.43 / 51.10 / 0.91 / 202.8 / 55.29 / 32.16 / 351.9
SD / 1.34 / 6.41 / 0.21 / 73.62 / 8.80 / 4.09 / 47.22
S2
Rehlingen / Range / 13.58-17.47 / 54.27-69.22 / 0.89-1.79 / 228.3-278.8 / 69.98-89.38 / 38.25-47.32 / 390.2-636.5
Median / 14.28 / 66.54 / 1.10 / 253.5 / 70.66 / 43.77 / 529.9
Mean / 14.90 / 64.14 / 1.22 / 253.5 / 75.17 / 43.28 / 521.6
SD / 1.74 / 6.72 / 0.42 / 20.64 / 9.48 / 4.65 / 101.6

n.d. not determined

Table S2: Metals and arsenic in zebra mussels (Dreissenapolymorpha) from the German ESB sampling sites.
Concentrations are given as µg/g dry weight except for mercury (ng/g)

Water / Sampling site and period / Value / Arsenic / Lead / Cadmium / Mercury / Copper / Nickel
µg/g dw / µg/g dw / µg/g dw / ng/g dw / µg/g dw / µg/g dw
LakeBelau / B
LakeBelau
1997-2009 / Range / 6.20-7.81 / 0.10-0.53 / 0.18-0.56 / 32.57-76.50 / 8.59-21.90 / 6.32-18.97
Median / 6.66 / 0.20 / 0.28 / 43.02 / 11.78 / 11.00
Mean / 6.99 / 0.26 / 0.33 / 49.74 / 13.84 / 11.67
SD / 0.60 / 0.18 / 0.14 / 16.37 / 5.07 / 3.96
Danube / D1
UIm
2003-2009 / Range / 2.56-3.62 / 0.45-0.86 / 0.61-0.88 / 37.72-60.68 / 12.67-18.93 / 7.36-17.70
Median / 2.90 / 0.80 / 0.72 / 53.78 / 17.04 / 14.05
Mean / 3.03 / 0.71 / 0.74 / 51.69 / 16.49 / 13.23
SD / 0.35 / 0.17 / 0.10 / 7.73 / 2.12 / 3.34
D2
Kelheim
2004-2009 / Range / 3.06-5.11 / 0.90-1.61 / 0.21-0.53 / 51.82-122.0 / 17.25-43.97 / 11.54-29.10
Median / 3.96 / 1.14 / 0.34 / 102.0 / 27.08 / 19.19
Mean / 3.99 / 1.18 / 0.36 / 92.36 / 28.44 / 19.42
SD / 0.67 / 0.28 / 0.12 / 30.51 / 9.93 / 6.14
D3
Jochenstein
2004-2009 / Range / 5.71-7.46 / 2.52-4.08 / 1.02-1.27 / 107.0-125.0 / 18.00-51.75 / 37.68-54.18
Median / 6.59 / 2.60 / 1.15 / 113.2 / 25.48 / 43.20
Mean / 6.63 / 2.92 / 1.15 / 114.6 / 29.34 / 45.64
SD / 0.66 / 0.66 / 0.11 / 7.86 / 12.96 / 7.67

Table S2 (cont): Metals and arsenic in zebra mussels (Dreissenapolymorpha) from the German ESB sampling sites.
Concentrations are given as µg/g dry weight except for mercury (ng/g)

Water / Sampling site and period / Value / Arsenic
µg/g dw / Lead
µg/g dw / Cadmium
µg/g dw / Mercury
ng/g dw / Copper
µg/g dw / Nickel
µg/g dw
Elbe / E1
Prossen
1999-2009 / Range / 4.40-7.66 / 2.37-4.98 / 0.44-1.18 / 80.23-216.2 / 13.47-20.28 / 18.73-28.82
Median / 6.17 / 3.40 / 0.61 / 120.7 / 16.60 / 22.60
Mean / 6.00 / 3.55 / 0.74 / 140.4 / 16.36 / 23.29
SD / 0.84 / 0.93 / 0.28 / 46.01 / 2.00 / 3.68
E2
Zehren
2000-2009 / Range / 2.79-5.87 / 2.02-13.98 / 0.52-6.40 / 150.7-271.7 / 11.80-24.75 / 5.44-22.45
Median / 4.59 / 4.43 / 0.87 / 215.8 / 19.30 / 12.48
Mean / 4.58 / 6.12 / 1.72 / 215.2 / 18.77 / 12.67
SD / 1.03 / 4.13 / 1.94 / 38.22 / 3.38 / 4.72
E3
Barby
1998-2009 / Range / 3.67-6.58 / 0.78-9.91 / 0.34-1.00 / 114.3-335.5 / 9.41-19.50 / 8.50-18.92
Median / 5.61 / 2.43 / 0.60 / 220.7 / 14.24 / 14.21
Mean / 5.57 / 2.93 / 0.56 / 204.0 / 14.25 / 14.50
SD / 0.90 / 2.40 / 0.19 / 70.33 / 2.49 / 3.10
E4
Cumlosen
1998-2009 / Range / 3.81-6.70 / 0.99-4.32 / 0.39-2.07 / 114.8-314.5 / 13.27-17.73 / 8.86-23.05
Median / 5.95 / 1.91 / 0.77 / 146.3 / 15.35 / 17.83
Mean / 5.56 / 2.12 / 0.93 / 164.1 / 15.41 / 17.10
SD / 1.00 / 0.94 / 0.48 / 59.28 / 1.38 / 4.61
E5
Blankenese
1995-2009 / Range / 7.04-12.78 / 2.25-5.26 / 0.92-2.36 / 163.6-328.6 / 19.08-33.07 / 14.90-42.57
Median / 9.42 / 3.79 / 1.13 / 244.0 / 27.20 / 25.86
Mean / 9.58 / 3.82 / 1.24 / 246.5 / 26.79 / 27.34
SD / 1.78 / 0.97 / 0.40 / 48.0 / 4.90 / 8.60

Table S2 (cont.): Metals and arsenic in zebra mussels (Dreissenapolymorpha) from the German ESB sampling sites.
Concentrations are given as µg/g dry weight except for mercury (ng/g)

Water / Sampling site and period / Value / Arsenic
µg/g dw / Lead
µg/g dw / Cadmium
µg/g dw / Mercury
ng/g dw / Copper
µg/g dw / Nickel
µg/g dw
Rhine / R1
Weil
1995-2009 / Range / 3.09-5.32 / 0.93-3.46 / 0.82-1.37 / 61.67-186.8 / 18.26-31.97 / 18.55-37.63
Median / 4.08 / 2.08 / 0.90 / 156.7 / 21.83 / 29.11
Mean / 4.13 / 2.12 / 0.98 / 140.5 / 24.11 / 28.17
SD / 0.82 / 1.08 / 0.20 / 47.32 / 5.67 / 6.58
R2
Iffezheim
1995-2009 / Range / 5.52-7.91 / 1.59-4.06 / 0.81-2.00 / 93.85-203.8 / 21.09-33.58 / 21.78-63.58
Median / 6.63 / 3.36 / 1.28 / 148.0 / 28.63 / 43.13
Mean / 6.67 / 3.00 / 1.34 / 148.1 / 27.98 / 42.90
SD / 0.98 / 1.27 / 0.57 / 46.51 / 5.46 / 22.10
R3
Koblenz
1995-2009 / Range / 3.73-6.13 / 1.77-6.36 / 0.66-2.12 / 54.82-155.8 / 18.87-42.30 / 10.02-37.51
Median / 4.70 / 3.19 / 1.00 / 88.37 / 27.35 / 20.66
Mean / 4.73 / 3.56 / 1.16 / 95.71 / 26.84 / 22.24
SD / 0.86 / 1.81 / 0.50 / 35.15 / 7.11 / 9.63
R4
Bimmen
1995-2009 / Range / 4.43-7.70 / 3.25-10.89 / 1.38-2.91 / 67.04-197.0 / 24.17-41.55 / 17.08-37.38
Median / 5.28 / 5.19 / 2.14 / 132.7 / 32.48 / 25.04
Mean / 5.46 / 6.08 / 2.14 / 140.2 / 31.08 / 27.38
SD / 0.99 / 2.72 / 0.46 / 36.23 / 5.75 / 6.75
Saar / S1
Güdingen
1994-2009 / Range / 2.25-4.26 / 1.39-4.64 / 0.43-1.40 / 39.74-99.03 / 16.32-37.18 / 12.98-33.18
Median / 2.98 / 3.03 / 0.68 / 65.35 / 20.30 / 17.51
Mean / 2.98 / 3.13 / 0.81 / 69.69 / 21.43 / 19.07
SD / 0.66 / 0.99 / 0.31 / 17.30 / 5.22 / 6.28
S2
Rehlingen
1994-2009 / Range / 2.24-5.69 / 2.53-6.44 / 0.32-0.85 / 34.56-196.4 / 19.23-29.36 / 18.00-32.48
Median / 3.29 / 3.32 / 0.44 / 57.16 / 23.36 / 22.60
Mean / 3.48 / 3.63 / 0.49 / 70.68 / 23.25 / 22.84
SD / 0.88 / 1.06 / 0.17 / 42.55 / 3.08 / 3.97

Table S3: Metals and arsenic in muscle and liver of bream (Abramisbrama) from the German ESB sampling sites.

Water / Sampling site and period / Value / Bream muscle / Bream liver
Arsenic
µg/g dw / Lead
ng/g dw / Mercury
ng/g dw / Copper
µg/g dw / Lead
ng/g dw / Cadmium
ng/g dw / Copper
µg/g dw / Zinc
µg/g dw
Lake Belau / B-Lake Belau
Muscle:
1997-2011
Liver:
2003-2009 / Range / 0.11-0.67 / 0.50-53.58 / 106.0-225.8 / 0.98-1.48 / 42.26-131.8 / 113.3-364.5 / 59.56-128.2 / 118.3-179.2
Median / 0.19 / 28.20 / 153.78 / 1.25 / 46.53 / 155.8 / 81.38 / 124.3
Mean / 0.24 / 27.64 / 156.17 / 1.23 / 66.78 / 197.4 / 87.62 / 136.5
SD / 0.18 / 22.13 / 41.30 / 0.16 / 43.45 / 114.0 / 29.14 / 28.98
Danube / D1- UIm
Muscle:
2004-2011
Liver:
2004-2010 / Range / 0.26-0.47 / 5.13-27.05 / 322.2-529.5 / 1.08-1.40 / 37.08-80.28 / 228.7-538.0 / 52.03-104.8 / 113.2-157.0
Median / 0.32 / 16.88 / 435.4 / 1.23 / 62.50 / 271.3 / 90.38 / 132.5
Mean / 0.34 / 16.91 / 447.5 / 1.24 / 61.62 / 321.0 / 82.48 / 133.7
SD / 0.08 / 7.36 / 67.69 / 0.12 / 12.74 / 106.5 / 21.62 / 17.37
D2-Kelheim
Muscle:
2004-2011
Liver:
2004-2010 / Range / 0.31-0.75 / 7.48-42.92 / 494.5-1295 / 1.14-1.26 / 98.90-169.2 / 204.8-884.5 / 81.48-213.2 / 120.8-201.0
Median / 0.61 / 33.60 / 714.3 / 1.22 / 132.8 / 323.7 / 123.3 / 144.2
Mean / 0.58 / 28.98 / 808.1 / 1.21 / 127.6 / 417.0 / 127.2 / 150.1
SD / 0.16 / 12.65 / 287.5 / 0.05 / 24.76 / 257.4 / 41.81 / 27.19
D3-Jochenstein
Muscle:
2004-2011
Liver:
2004-2010 / Range / 0.46-0.92 / 16.88-73.32 / 1053-1530 / 1.10-1.77 / 111.9-274.0 / 1207-2183 / 79.35-159.3 / 109.7-175.8
Median / 0.52 / 28.64 / 1325 / 1.27 / 130.8 / 1382 / 108.2 / 141.5
Mean / 0.60 / 35.57 / 1332 / 1.36 / 151.8 / 1590 / 114.9 / 141.3
SD / 0.17 / 18.08 / 159.1 / 0.24 / 56.98 / 373.6 / 31.20 / 27.83

Table S3 (cont.): Metals and arsenic in muscle and liver of bream (Abramisbrama) from the German ESB sampling sites.

Water / Sampling site and period / Value / Bream muscle / Bream liver
Arsenic
µg/g dw / Lead
ng/g dw / Mercury
ng/g dw / Copper
µg/g dw / Lead
ng/g dw / Cadmium
ng/g dw / Copper
µg/g dw / Zinc
µg/g dw
Elbe / E1-Prossen
Muscle:
1993-2011
Liver:
2002-2010 / Range / 0.20-0.47 / 44.60-178.5 / 824.2-2859 / 1.08-1.72 / 142.0-467.0 / 715.8-3140 / 61.20-145.3 / 109.6-172.6
Median / 0.34 / 90.48 / 1592 / 1.36 / 310.2 / 2102 / 75.68 / 117.8
Mean / 0.34 / 95.56 / 1658 / 1.37 / 303.7 / 1925 / 86.67 / 128.1
SD / 0.07 / 36.45 / 562.5 / 0.16 / 106.7 / 912.4 / 25.64 / 22.09
E2-Zehren
Muscle:
1993-2011
Liver:
2002-2010 / Range / 0.10-0.64 / 42.24-172.4 / 958.1-3376 / 1.21-1.98 / 258.5-541.3 / 2352-9070 / 92.13-157.2 / 120.0-163.8
Median / 0.42 / 104.2 / 2033 / 1.38 / 372.8 / 5650 / 126.5 / 150.2
Mean / 0.44 / 112.3 / 2050 / 1.44 / 376.4 / 5512 / 126.4 / 146.7
SD / 0.13 / 36.24 / 601.7 / 0.19 / 108.8 / 1887 / 23.68 / 16.60
E3-Barby
Muscle:
1993-2011
Liver:
2002-2010 / Range / 0.29-0.64 / 51.36-167.9 / 1050-4196 / 1.21-2.46 / 259.5-542.3 / 1093-8888 / 78.37-193.5 / 134.8-186.7
Median / 0.40 / 85.86 / 1540 / 1.48 / 363.2 / 4640 / 136.8 / 169.5
Mean / 0.42 / 93.59 / 1902 / 1.62 / 382.1 / 4875 / 134.7 / 158.7
SD / 0.10 / 33.47 / 881.1 / 0.40 / 83.42 / 2330 / 41.91 / 19.83
E4-Cumlosen
Muscle:
1993-2011
Liver:
2002-2010 / Range / 0.21-0.83 / 36.44-164.0 / 1041-3286 / 1.47-4.55 / 161.8-303.8 / 2355-7564 / 61.37-112.7 / 108.2-156.5
Median / 0.31 / 70.88 / 1492 / 2.38 / 263.00 / 4068 / 92.85 / 140.5
Mean / 0.34 / 78.92 / 1782 / 2.51 / 259.6 / 4249 / 90.74 / 137.2
SD / 0.14 / 33.77 / 713.9 / 0.78 / 44.43 / 1647 / 16.74 / 16.81
E5Blankenese
Muscle:
1993-2011
Liver:
2002-2010 / Range / 0.38-0.76 / 7.86-158.8 / 351.2-1650 / 1.28-3.81 / 74.05-131.8 / 74.27-249.2 / 17.93-51.05 / 64.23-113.5
Median / 0.52 / 57.88 / 577.7 / 2.04 / 86.22 / 133.3 / 19.67 / 76.13
Mean / 0.53 / 60.18 / 882.8 / 2.28 / 94.86 / 143.6 / 25.16 / 82.04
SD / 0.10 / 38.72 / 469.1 / 0.88 / 18.97 / 52.69 / 11.22 / 14.83

Table S3 (cont.): Metals and arsenic in muscle and liver of bream (Abramisbrama) from the German ESB sampling sites.

Water / Sampling site and period / Value / Bream muscle / Bream liver
Arsenic
µg/g dw / Lead
ng/g dw / Mercury
ng/g dw / Copper
µg/g dw / Lead
ng/g dw / Cadmium
ng/g dw / Copper
µg/g dw / Zinc
µg/g dw
Rhine / R1-Weil
Muscle:
1995-2011
Liver: 2002-2010 / Range / 0.24-0.54 / 15.82-78.29 / 364.2-916.3 / 1.03-2.19 / 51.08-120.2 / 42.83-204.4 / 15.65-60.73 / 55.50-83.73
Median / 0.42 / 32.83 / 697.9 / 1.51 / 59.60 / 138.4 / 32.43 / 68.23
Mean / 0.40 / 41.66 / 689.3 / 1.50 / 76.43 / 130.0 / 33.96 / 67.80
SD / 0.09 / 21.88 / 162.2 / 0.26 / 27.40 / 53.98 / 12.27 / 10.62
R2-Iffezheim
Muscle:
1995-2011
Liver: 2002-2010 / Range / 0.39-0.79 / 15.85-268.0 / 688.3-1429 / 1.02-1.64 / 164.8-275.0 / 587.4-1183 / 81.37-102.17 / 109.3-129.8
Median / 0.56 / 58.62 / 1023 / 1.31 / 186.8 / 851.2 / 88.50 / 124.0
Mean / 0.58 / 75.02 / 1037 / 1.28 / 196.3 / 892.1 / 91.30 / 123.5
SD / 0.12 / 61.05 / 164.7 / 0.20 / 35.01 / 215.1 / 6.96 / 6.17
R3-Koblenz
Muscle:
1995-2011
Liver: 2002-2010 / Range / 0.32-0.68 / 27.08-118.5 / 366.5-878.4 / 0.93-1.31 / 100.4-199.3 / 145.3-1466 / 40.43-95.62 / 68.38-107.7
Median / 0.44 / 67.20 / 483.3 / 1.16 / 157.4 / 408.0 / 62.67 / 92.15
Mean / 0.47 / 65.26 / 527.1 / 1.14 / 150.9 / 526.0 / 65.11 / 91.04
SD / 0.11 / 27.34 / 156.3 / 0.12 / 29.10 / 452.1 / 16.97 / 12.48
R4-Bimmen
Muscle:
1995-2011
Liver: 2002-2010 / Range / 0.43-0.97 / 61.86-186.2 / 560.6-1945 / 1.00-1.61 / 137.2-389.8 / 602.3-3104 / 52.67-133.7 / 88.82-145.7
Median / 0.64 / 82.89 / 895.0 / 1.23 / 282.50 / 2352 / 96.92 / 123.0
Mean / 0.69 / 104.45 / 984.5 / 1.23 / 274.02 / 2074 / 99.49 / 120.4
SD / 0.18 / 41.55 / 349.1 / 0.19 / 90.43 / 1035 / 29.70 / 22.34
Saar / S1-Güdingen
Muscle:
1994-2011
Liver: 2002-2010 / Range / 0.15-0.56 / 35.83-255.7 / 315.5-548.6 / 1.15-1.67 / 96.26-170.83 / 108.8-238.5 / 34.93-77.50 / 68.95-114.3
Median / 0.24 / 74.46 / 439.1 / 1.42 / 132.7 / 170.5 / 44.82 / 94.40
Mean / 0.28 / 85.43 / 435.4 / 1.41 / 131.3 / 175.6 / 49.79 / 95.43
SD / 0.11 / 51.27 / 59.50 / 0.12 / 24.55 / 42.11 / 14.68 / 13.25
S2-Rehlingen
Muscle:
1994-2011
Liver: 2002-2010 / Range / 0.30-0.76 / 30.30-122.2 / 397.5-633.0 / 1.04-1.65 / 119.0-187.2 / 86.78-230.0 / 91.22-155.0 / 111.3-156.5
Median / 0.51 / 51.67 / 521.4 / 1.26 / 158.3 / 166.2 / 114.6 / 129.3
Mean / 0.52 / 64.84 / 524.7 / 1.24 / 155.3 / 169.4 / 119.0 / 133.9
SD / 0.15 / 29.25 / 65.42 / 0.14 / 19.77 / 50.69 / 18.51 / 13.97

Table S4: Time trend analysis of arsenic and metals in suspended particulate matter (SPM) from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%. Time span: 2005 – 2009 (5 years). Exception: Saar: 2006 – 2009 (4 years)

Water / Sampling site / Parameters / SPM
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel / Zinc
Elbe / E1
Prossen / Yearly trend / 9.7% n.s. / 6.9% n.s. / 10% n.s. / 5.7% n.s. / 12% n.s. / 12% n.s. / 8.3% n.s.
95%-CI / -7.5; 30 / -14; 32 / -11; 37 / -23; 45 / -5.0; 31 / -11; 40 / -8.8; 28
r² / 0.50 / 0.25 / 0.41 / 0.09 / 0.61 / 0.44 / 0.42
p / <0.182 / <0.397 / <0.244 / <0.616 / <0.117 / <0.222 / <0.236
E2
Zehren / Yearlytrend / 1.4% n.s. / 7.5% n.s. / 16% n.s. / 6.2% n.s. / 10% n.s. / 17% n.s. / 15% n.s.
95%-CI / -26; 39 / -27; 58 / -37; 118 / -48; 116 / -30; 73 / -27; 90 / -29; 86
r² / 0.01 / 0.10 / 0.17 / 0.02 / 0.15 / 0.28 / 0.21
p / <0.862 / <0.599 / <0.497 / <0.790 / <0.529 / <0.359 / <0.327
E3
Barby / Yearlytrend / -11% n.s. / -2.2% n.s. / -1.5% n.s. / -11% n.s. / -4.7% n.s. / -2.2% n.s. / -5.1% n.s.
95%-CI / -28; 9.9 / -14; 12 / -23; 26 / -19; -2.1 / -9.4; 0.3 / -15; 13 / -18; 10
r² / 0.51 / 0.09 / 0.01 / 0.83 / 0.75 / 0.08 / 0.30
p / <0.174 / <0.616 / <0.831 / <0.033 / <0.061 / <0.649 / <0.344
E4
Cumlosen / Yearly trend / -3.1% n.s. / 0.7% n.s. / 2.6% n.s. / -4.4% n.s. / -2.4% n.s. / 4.4% n.s. / 0.7% n.s.
95%-CI / -12; 6.3 / -14; 17 / -41; 77 / -15; 7.0 / -13; 9.6 / -17; 31 / -16; 22
r² / 0.29 / 0.01 / 0.01 / 0.35 / 0.12 / 0.10 / 0.00
p / <0.353 / <0.870 / <0.861 / <0.296 / <0.562 / <0.597 / <0.879
E5
Blankenese / Yearlytrend / 1.5% n.s. / 5.7% n.s. / 27% n.s. / 1.5% n.s. / 4.4% n.s. / 6.3% n.s. / 5.8% n.s.
95%-CI / -3.8; 7.0 / -3.2; 15 / -63; 331 / -8.2; 13 / -0.9; 10 / 1.1; 12 / -7.7;21
r² / 0.20 / 0.57 / 0.11 / 0.07 / 0.70 / 0.83 / 0.36
p / <0.454 / <0.142 / <0.586 / <0.661 / <0.080 / 0.033 / <0.281

Table S4 (cont.): Time trend analysis of arsenic and metals in suspended particulate matter (SPM) from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%. Time span: 2005 – 2009 (5 years). Exception: Saar: 2006 – 2009 (4 years)

Water / Sampling site / Parameters / SPM
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel / Zinc
Saale / SA
Wettin / Yearlytrend / -4.5% n.s. / -1.9.0% n.s. / 12% n.s. / -13% n.s. / -3.4% n.s. / 0.30% / -0.8% n.s.
95%-CI / -23; 19 / -13; 11 / -; 246 / -27; 4.2 / -15; 9.9 / -15; 19 / -21; 23
r² / 0.14 / 0.08 / 0.03 / 0.67 / 0.20 / 0.00 / 0.00
p / <0.545 / <0.650 / <0.758 / <0.092 / <0.457 / <0.911 / <0.877
Mulde / Mu
Dessau / Yearlytrend / 3.7% n.s. / 1.1% n.s. / 7.7% n.s. / 5.2% n.s. / 4.3% n.s. / 13% increase / 17% n.s.
95%-CI / -5.1; 13 / -6.9; 9.3 / 1.7; 14 / -10; 23 / -0.2; 9.0 / 7.9; 18 / -18; 67
r² / 0.38% / 0.06 / 0.85 / 0.26 / 0.75 / 0.96 / 0.39
p / <0.271 / <0.678 / <0.029 / <0.384 / <0.059 / <0.007 / <0.260
Rhine / R1
Weil / Yearlytrend / -0.5% n.s. / 2.1% n.s. / 12% n.s. / 2.6% n.s. / -0.02% n.s. / 6.4% n.s. / 4.4% n.s.
95%-CI / -9; 9.3 / -10; 16 / -34; 88 / -29; 49 / -8.1; 8.9 / -9.0; 24 / -1.1; 10
r² / 0.01 / 0.08 / 0.12 / 0.02 / 0.00 / 0.35 / 0.68
p / <0.844 / <0.647 / <0.574 / <0.816 / <0.942 / <0.295 / <0.087
R2
Iffezheim / Yearlytrend / -3.2% n.s. / 2.2% n.s. / 7.4% n.s. / -2.4% n.s. / -1.6% n.s. / 3.5% n.s. / 2.4% n.s.
95%-CI / -8.2; 2.0 / -6.2; 12 / -16; 39 / -12; 8.7 / -6.0; 3.0 / -12; 22 / -0.20; 5.1
r² / 0.57 / 0.18 / 0.21 / 0.15 / 0.29 / 0.12 / 0.74
p / <0.142 / <0.482 / <0.445 / <0.523 / <0.353 / <0.564 / <0.063
R3
Koblenz / Yearlytrend / 3.1% n.s. / 3.4% n.s. / 14% n.s. / -3.9% n.s. / 0.2% n.s. / 8.0% n.s. / 5.0% n.s.
95%-CI / -5.6; 13 / -7.6; 16 / -18; 60 / -12; 5.0 / -10; 12 / -2.4; 20 / -2.0; 13
r² / 0.29 / 0.23 / 0.34 / 0.40 / 0.00 / 0.66 / 0.63
p / <0.353 / <0.414 / <0.299 / <0.249 / <0.909 / <0.096 / <0.110
R4
Bimmen / Yearlytrend / -1.0% n.s. / -1.3% n.s. / 1.7% n.s. / -8.9% n.s. / -3.4% n.s. / 2.1% n.s. / 7.3% n.s.
95%-CI / -3.8; 1.9 / -9.0; 7.1 / -34; 58 / -18; 1.6 / -11; 4.8 / -12; 18 / -25; 54
r² / 0.28 / 0.08 / 0.00 / 0.71 / 0.38 / 0.06 / 0.11
p / <0.365 / <0.654 / <0.877 / <0.075 / <0.270 / <0.683 / <0.581

Table S4 (cont.): Time trend analysis of arsenic and metals in suspended particulate matter (SPM) from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%. Time span: 2005 – 2009 (5 years).Exception: Saar: 2006 – 2009 (4 years)

Water / Sampling site / Parameters / SPM
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel / Zinc
Saar / S1
Güdingen / Yearlytrend / -2.9% n.s. / -2.1% n.s. / -14% n.s. / -18% decrease / -7.2% n.s. / 6.6% n.s. / 1.0% n.s.
95%-CI / -27; 31 / -27; 31 / -34; 10 / -47; 28 / -29; 21 / -16; 36 / -27; 40
r² / 0.08 / 0.05 / 0.77 / 0.64 /Kendall’s tau :***/SD(sm): 0.00 / 0.42 / 0.39 / 0.01
p / <0.704 / <0.770 / <0.128 / <0.200 /p<0.042 (tau) (p<0.001 (SD(sm)) / <0.353 / <0.377 / <0.877
S2
Rehlingen / Yearlytrend / -5.3% n.s. / 2.9% n.s. / -16% n.s. / -1.9% n.s. / -7.0% n.s. / 8.2% increase / -1.9% n.s.
95%-CI / -23; 16 / -20; 31 / -52; 48 / -18; 17 / -22; 10 / -0.4; 17 / -39; 58
r² / 0.39 / 0.12 / 0.47 / 0.09 / 0.62 / 0.89(Kendall’s tau: 1.00/SD(sm): 0.00 / 0.01
p / <0.380 / <0.656 / <0.319 / <0.694 / <0.215 / <0.062 / p<0.042 (tau) / p<0.001 (SD(sm)) / <0.850

Table S5: Time trend analysis of arsenic and metals in zebra mussels from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Zebra mussel
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel
Lake Belau / B / Period / 1997-2009 / 1999-2009 / 1997-2009 / 1997-2009 / 1997-2009 / 1997-2009
No of values / 7 / 6 / 7 / 7 / 7 / 7
Yearly trend / -0.3% n.s. / -15% n.s. / -7.4% decrease / -5.2% n.s. / -7.7% decrease / -6.2% decrease
95%-CI / 2.6; 1.9 / -25; -3.3 / -12; -2.3 / -10; 0.4 / -10; -4.9 / -11; -1.2
r² / 0.03 / 0.75 / 0.73 / 0.53 / 0.90 / 0.67
p / <0.702 / <0.026 / 0.015 / <0.061 / <0.001 / <0.025
Danube / D1
Ulm / Period / 2003-2009 / 2003-2009 / 2003-2009 / 2003-2009 / 2003-2009 / 2003-2009
No of values / 7 / 7 / 7 / 7 / 7 / 7
Yearly trend / -2.7% n.s. / 8.0% n.s. / -3.4% n.s. / 4.1% n.s. / 2.3% n.s. / 5.3% n.s.
95%-CI / -7.6; 2.6 / -3.6; 21 / -8.9; 2.4 / -3.1; 12 / -4.3; 9.5 / -8.5; 21
r² / 0.25 / 0.38 / 0.32 / 0.29 / 0.14 / 0.15
p / <0.249 / <0.141 / <0.187 / <0.208 / <0.420 / <0.391
D2
Kelheim / Period / 2004-2009 / 2004-2009 / 2004-2009 / 2004-2009 / 2004-2009 / 2004-2009
No of values / 6 / 6 / 6 / 6 / 6 / 6
Yearly trend / -4.0% n.s. / 12% increase / 3.3% n.s. / 12% n.s. / 21% increase / 16% increase
95%-CI / -14; 6.9 / 4.8; 20 / -20; 34 / -11; 40 / 17; 23 / 5.1; 30
r² / 0.22 / 0.85 / 0.03 / 0.30 / 0.99 / 0.81
p / <0.352 / <0.010 / <0.739 / <0.262 / <0.001 / <0.016
D3
Jochenstein / Period / 2004-2009 / 2004-2009 / 2004-2009 / 2004-2009 / 2004-2009 / 2004-2009
Noofvalues / 5 / 5 / 5 / 5 / 5 / 5
Yearlytrend / -0.8% n.s. / 2.4% n.s. / -0.3 n.s. / 0.9% n.s. / 18% n.s. / 7.7% n.s.
95%-CI / -9; 9.1 / -16; 23 / -9.4; 9.6 / -5.2; 7.5 / -2.6; 45 / -0.8; 17.4
r² / 0.03 / 0.05 / 0.00 / 0.07 / 0.72 / 0.74
p / <0.785 / <0.706 / <0.879 / <0.664 / <0.072 / <0.065

Table S5 (cont.): Time trend analysis of arsenic and metals in zebra mussels from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Zebra mussel
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel
Elbe / E1
Prossen / Period / 1999-2009 / 1999-2009 / 1999-2009 / 1999-2009 / 1999-2009 / 1999-2009
No of values / 11 / 11 / 11 / 11 / 11 / 11
Yearlytrend / 0.9% n.s. / 0.8% n.s. / 2.3% n.s. / -5.2% n.s. / -0.8% n.s. / -1.6% n.s.
95%-CI / -2.3; 4.2 / -5.2; 7.1 / -5.9; 12 / -11; 1.0 / -3.4; 1.8 / -4.9; 1.8
r² / 0.04 / 0.01 / 0.04 / 0.28 / 0.05 / 0.11
p / <0.558 / <0.767 / <0.563 / <0.089 / <0.498 / <0.310
E2
Zehren / Period / 2000-2009 / 2000-2009 / 2000-2009 / 2000-2009 / 2000-2009 / 2000-2009
No of values / 10 / 10 / 10 / 10 / 10 / 10
Yearly trend / 1.1% n.s. / 20% increase / -18% n.s. / 0.3% n.s. / -0.4% n.s. / 5.5% n.s.
95%-CI / -5.3; 7.8 / 6.3; 30 / -35; -4.3 / -4.6; 5.4 / -5.4; 5.0 / -4.4; 16
r² / 0.02 / 0.60 / 0.52 / 0.00 / 0.00 / 0.16
p / <0.711 / 0.008 / <0.018 / <0.855 / <0.852 / <0.244
E3
Barby / Period / 1998-2009 / 1998-2009 / 1998-2009 / 1998-2009 / 1998-2009 / 1998-2009
Noofvalues / 12 / 12 / 12 / 12 / 12 / 12
Yearlytrend / -0.5% n.s. / 7.8% n.s. / 3.7% n.s. / -7.6% decrease / 2.0% n.s. / -0.8% n.s.
95%-CI / -3.8; 2.8 / -4.3; 21 / -2.4; 10 / -11; -3.5 / -1.2; 5.3 / -5.2; 3.7
r² / 0.01 / 0.17 / 0.15 / 0.63 / 0.17 / 0.02
p / <0.726 / <0.187 / <0.207 / <0.002 / <0.184 / <0.687
E4
Cumlosen / Period / 1998-2009 / 1998-2009 / 1998-2009 / 1998-2009 / 1998-2009 / 1998-2009
Noofvalues / 10 / 10 / 10 / 10 / 10 / 10
Yearlytrend / -0.5% n.s. / -1.9% n.s. / 5.0% n.s. / -3.4% n.s. / 0.4% n.s. / -1.2% n.s.
95%-CI / -4.4; 3.7 / -9; 6.7 / -3.6; 14 / -8.6; 2.1 / -1.4; 2.2 / -7.2; 5.1
r² / 0.01 / 0.03 / 0.18 / 0.21 / 0.04 / 0.03
p / <0.787 / <0.623 / <0.223 / <0.184 / <0.609 / <0.661

Table S5 (cont.): Time trend analysis of arsenic and metals in zebra mussels from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Zebra mussel
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel
Elbe / E5
Blankenese / Period / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009
No of values / 13 / 12 / 13 / 13 / 13 / 13
Yearly trend / -0.1% n.s. / 2.2% n.s. / -2.3% n.s. / -1.8% n.s. / 3.0% increase / 5.3% increase
95%-CI / -2.7; 2.4 / -1.4; 6.0 / -5.6; 1.2 / -4.2; 0.7 / 1.2; 4.8 / 2.2; 8.5
r² / 0.00 / 0.15 / 0.16 / 0.19 / 0.55 / 0.57
p / <0.871 / <0.206 / <0.166 / <0.137 / <0.004 / <0.003
Rhine / R1
Weil / Period / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009
Noofvalues / 6 / 5 / 6 / 6 / 6 / 6
Yearlytrend / -2.9% n.s. / 2.5% n.s. / -2.8% decrease / 6.0% n.s. / 1.1% n.s. / 1.5% n.s.
95%-CI / -7.2; 1.7 / -16; 26 / -6.8; 1.4 / -4.2; 17 / -5.6; 8.2 / -5.6; 9.2
r² / 0.44 / 0.05 / 0.47 / Kendall’s tau: -0.73 / 0.39 / 0.04 / 0.07
p / <0.149 / <0.716 / <0.133 (p<0.039 (tau)) / <0.186 / <0.688 / <0.607
R2
Iffezheim / Period / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009
Noofvalues / 4 / 4 / 4 / 4 / 4 / 4
Yearlytrend / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
95%-CI / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
r² / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
p / n.d. / n.d. / n.d. / n.d. / n.d. / n.d.
R3
Koblenz / Period / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009
Noofvalues / 9 / 8 / 9 / 9 / 9 / 9
Yearlytrend / -1.1% n.s. / -1.0% n.s. / -4.2% decrease / -3.1% n.s. / -2.7% n.s. / -6.8% decrease
95%-CI / -3.8; 1.8 / -10; 9.0 / -9.1; 0.9 / -7.9; 2.0 / -5.8; 0.6 / -10; -2.8
r² / 0.10 / 0.01 / 0.35/ Kendall’s tau: -0.56 / 0.23 / 0.35 / 0.69
p / <0.411 / <0.789 / <0.091 / p<0.037 (tau) / <0.188 / <0.090 / <0.006

Table S5 (cont.): Time trend analysis of arsenic and metals in zebra mussels from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Zebra mussel
Arsenic / Lead / Cadmium / Mercury / Copper / Nickel
R4
Bimmen / Period / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009 / 1995-2009
No of values / 10 / 9 / 10 / 10 / 10 / 10
Yearly trend / -1.8% / 6.4% increase / 1% n.s. / 2.4% n.s. / -0.8% n.s. / -0.1% n.s.
95%-CI / -3.9; 0.40 / 1.3; 12 / -2.4; 4.5 / -1.9; 6.8 / -3.5; 2.0 / -4.0; 4.0
r² / 0.31 / 0.56 / 0.05 / 0.17 / 0.05 / 0.00
p / <0.093 / <0.020 / <0.521 / <0.231 / <0.533 / <0.915
Saar / S1
Güdingen / Period / 1994-2009 / 1994-2009 / 1994-2009 / 1994-2009 / 1994-2009 / 1994-2009
No of values / 15 / 15 / 15 / 15 / 15 / 15
Yearly trend / -0.7% n.s. / 1.9% n.s. / 4.9% increase / -1.6% n.s. / 2.5% increase / 2.6% n.s.
95%-CI / -3.1; 1.9 / -2.4; 6.4 / 1.1; 8.9 / -4.5; 1.4 / 0.3; 4.8 / -0.9; 6.3
r² / 0.02 / 0.07 / 0.38 / 0.09 / 0.32 / 0.17
p / <0.599 / <0.353 / <0.014 / <0.278 / <0.026 / <0.127
Rehlingen / Period / 1994-2009 / 1994-2009 / 1994-2009 / 1994-2009 / 1994-2009 / 1994-2009
No of values / 16 / 15 / 16 / 16 / 16 / 16
Yearly trend / -3.0% decrease / -0.1% n.s. / 2.6% n.s. / -6.8% decrease / 0.30% n.s. / -0.2% n.s.
95%-CI / -5.3; -0.6 / -3.3; 3.1 / -0.8; 6.2 / -10; -2.8 / -1.2; 1.9 / -2.3; 1.8
r² / 0.33 / 0.00 / 0.16 / 0.47 / 0.01 / 0.01
p / <0.019 / <0.883 / <0.126 / <0.003 / 0.684 / <0.781

Table S6: Time trend analysis of arsenic and metals in bream from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Breammuscle / Breamliver
Arsenic / Lead / Copper / Mercury / Lead / Cadmium / Copper / Zinc
Lake Belau / B / period / 1997-2009 / 1997-2009 / 1997-2009 / 1997-2009 / 2003-2009 / 2003-2009 / 2003-2009 / 2003-2009
No of values / 8 / 7 / 8 / 8 / 4 / 4 / 4 / 4
Yearly trend / 0.4% n.s. / -20% n.s. / 1.1% n.s. / -3.8% decrease / -5.4% n.s. / 17% n.s. / -11% decrease / -6.5% n.s.
95%-CI / -10;13 / -39; 3.3 / -1.4; 3.7 / -7.3; -0.3 / -49; 75 / -15; 63 / -18; -3.6 / -16; 4.4
r² / 0.0 / 0.5 / 0.16 / 0.54 / 0.07 / 0.70 / 0.95 / 0.77
p / <0.901 / <0.073 / <0.331 / <0.037 / <0.731 / <0.166 / <0.034 / <0.125
Danube / D1
Ulm / period / 2004-2011 / 2004-2011 / 2004-2011 / 2004-2011 / 2004-2010 / 2004-2010 / 2004-2010 / 2004-2010
No of values / 8 / 8 / 8 / 8 / 7 / 7 / 7 / 7
Yearly trend / -2.3% n.s. / -0.3% n.s. / 0.6% n.s. / -1.9% n.s. / 6.5% n.s. / -3.8% n.s. / -8.4% n.s. / -4.0% n.s.
95%-CI / -10; 6.4 / -20; 25 / -3.2; 4.5 / -7.9; 4.4 / -3.7; 17 / -17; 12 / -18; 2.2 / -8.7; 1.0
r² / 0.07 / 0.00 / 0.02 / 0.09 / 0.34 / 0.08 / 0.46 / 0.47
p / <0.539 / <0.923 / <0.721 / <0.483 / <0.168 / <0.534 / <0.092 / <0.09
D2
Kelheim / period / 2004-2011 / 2004-2011 / 2004-2011 / 2004-2011 / 2004-2010 / 2004-2010 / 2004-2010 / 2004-2010
No of values / 8 / 7 / 8 / 8 / 7 / 7 / 7 / 7
Yearly trend / -3.4% n.s. / -2.5% n.s. / 0.8% n.s. / 10% n.s. / 3.0% n.s. / 13% n.s. / 12% n.s. / 3.9% n.s.
95%-CI / -15; 8.9 / -27; 31 / -0.6; 2.2 / -0.8; 22 / -6.5; 14 / -14; 46 / 0.5; 23 / -4.1; 13
r² / 0.08 / 0.01 / 0.26 / 0.46 / 0.11 / 0.20 / 0.59 / 0.23
p / <0.508 / <0.817 / <0.199 / <0.063 / <0.467 / <0.385 / <0.043 / <0.277
D3
Jochen-stein / Period / 2004-2011 / 2004-2011 / 2004-2011 / 2004-2011 / 2004-2010 / 2004-2010 / 2004-2010 / 2004-2010
No of values / 8 / 8 / 8 / 8 / 7 / 7 / 7 / 7
Yearly trend / -7.6% n.s. / 9.6% n.s. / 4.9% n.s. / 1.0% n.s. / 6.8% n.s. / 5.7% n.s. / 4.9% n.s. / 3.7% n.s.
95%-CI / -14; -0.9 / -6.9; 30 / -0; 10 / -3.8; 6.1 / -7.8; 23 / -4.6; 17 / -8.4; 20 / -6.0; 14
r² / 0.56 / 0.24 / 0.50 / 0.04 / 0.21 / 0.28 / 0.14 / 0.15
p / <0.032 / <0.216 / <0.050 / <0.645 / <0.302 / <0.222 / <0.413 / <0.395

Table S6 (cont.): Time trend analysis of arsenic and metals in bream from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Bream muscle / Bream liver
Arsenic / Lead / Copper / Mercury / Lead / Cadmium / Copper / Zinc
Elbe / E1
Prossen / Period / 1993-2011 / 1993-2011 / 1993-2011 / 1993-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 19 / 18 / 19 / 19 / 9 / 9 / 9 / 9
Yearlytrend / 0.8% n.s. / -3.1% n.s. / -1.7% decrease / -5.3% decrease / -11% n.s. / -13% n.s. / -2.0% n.s. / -4.6% decrease
95%-CI / -1.1; 2.7 / -6.2; 0.1 / -2.3; -1.0 / -6.6; -3.8 / -16; -5.2 / -24; 0.6 / -9.5; 6.7 / -7.5; -1.5
r² / 0.05 / 0.21 / 0.63 / 0.78 / 0.72 / 0.42 / 0.04 / 0.64
p / <0.375 / <0.055 / <0.001 / <0.001 / <0.004 / <0.056 / <0.605 / <0.01
E2
Zehren / Period / 1993-2011 / 1993-2011 / 1993-2011 / 1993-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 19 / 18 / 19 / 19 / 9 / 9 / 9 / 9
Yearly trend / 4.2% increase / -3.0% n.s. / -1.3% decrease / -4.8% decrease / -6.6% n.s. / -10% decrease / -4.2% n.s. / -3.7% decrease
95%-CI / 1.1; 7.4 / -5,9; 0.0 / -2.2; -0.3 / -6.0; -3.5 / -13; 0.4 / -17; -3.2 / -8.9; 1.0 / -5.4; -1.9
r² / 0.33 / 0.22 / 0.32 / 0.79 / 0.41 / 0.62 / 0.34 / 0.76
p / <0.01 / <0.049 / <0.011 / <0.001 / <0.06 / <0.011 / <0.095 / 0.002
E3
Barby / Period / 1993-2011 / 1993-2011 / 1993-2011 / 1993-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 19 / 18 / 19 / 19 / 9 / 9 / 9 / 9
Yearly trend / -0.5% n.s. / -1.0% n.s. / -3.6% decrease / -5.0% decrease / 5.2% n.s. / 14% n.s. / 5.3% n.s. / 1.7% n.s.
95%-CI / -2.5; 1.4 / -4.2; 2.2 / -4.6; -2.6 / -7.4; -2.6 / -0.3; 10 / -4.2; 35 / -4.1; 16 / -2.2; 5.7
r² / 0.02 / 0.03 / 0.76 / 0.51 / 0.42 / 0.31 / 0.20 / 0.13
p / <0.569 / <0.508 / <0.001 / <0.001 / <0.059 / <0.119 / <0.228 / <0.344
E4
Cumlosen / Period / 1993-2011 / 1993-2011 / 1993-2011 / 1993-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 19 / 18 / 19 / 19 / 9 / 9 / 9 / 9
Yearly trend / 2.5% n.s. / -4.5% decrease / -4.6% decrease / -3.6% decrease / 0.5% n.s. / 0.2% n.s. / -1.4% n.s. / -0.4n.s.
95%-CI / -0.1; 5.3 / -7.4; -1.6 / -5.7; -3.5 / -6.3; -0.9 / -6.7; 6.0 / -11; 14 / -7.5; 5.1 / -4.4; 3.8
r² / 0.19 / 0.39 / 0.82 / 0.32 / 0.01 / 0.0 / 0.04 / 0.01
p / <0.058 / <0.005 / <0.001 / <0.011 / <0.830 / <0.918 / <0.620 / <0.813

Table S6 (cont.): Time trend analysis of arsenic and metals in bream from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Bream muscle / Bream liver
Arsenic / Lead / Copper / Mercury / Lead / Cadmium / Copper / Zinc
Elbe / E5
Blanke-nese / Period / 1993-2011 / 1993-2011 / 1993-2011 / 1993-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 19 / 18 / 19 / 19 / 9 / 9 / 9 / 9
Yearly trend / 0.3% n.s. / -9.3% decrease / -6.0% decrease / -8,4% decrease / 0.8% n.s. / -5,9% n.s. / 4.3% n.s. / 1.6% n.s.
95%-CI / -1.4; 1.9 / -14;-4.7 / -7.4; -4.6 / -10; -6,7 / -6.7; 5.4 / -16; 4.8 / -6,9; 16 / -3.6; 7.3
r² / 0.01 / 0.52 / 0.81 / 0.85 / 0.01 / 0.20 / 0.10 / 0.07
p / <0.754 / <0.001 / <0.001 / <0.001 / <0.751 / <0.224 / <0.415 / <0.495
Saale / SA
Wettin / Period / 1995-2011 / 1995-2011 / 1995-2011 / 1995-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 17 / 16 / 17 / 17 / 9 / 9 / 9 / 9
Yearly trend / 9.1% increase / 0.9% n.s. / -1.9% decrease / 2.9% increase / -12% decrease / 5.3% n.s. / -0.7% n.s. / -1.3% n.s.
95%-CI / 6.5; 12 / -3.6; 5.7 / -3.2; -0.6 / 1.1; 4.7 / -18; -5.8 / -3.0; 14 / -5.4; 4.1 / -5.8; 3.4
r² / 0.79 / 0.01 / 0.39 / 0.44 / 0.74 / 0.25 / 0.02 / 0.06
p / <0.001 / <0.684 / <0.007 / <0.004 / <0.003 / <0.173 / <0.727 / <0.517
Mulde / MU
Dessau / Period / 1995-2011 / 1995-2011 / 1995-2011 / 1995-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 17 / 16 / 17 / 17 / 9 / 9 / 9 / 9
Yearly trend / 0.3% n.s. / -4.8% decrease / -3.7% decrease / -8.1% decrease / 1.6% n.s. / 3.3% n.s. / 1.2% n.s. / -0.3% n.s.
95%-CI / -1.6; 2.3 / -8.4; -1.0 / -5.6; -1.7 / -10; -5.6 / -7.8; 12 / -4.2; 12 / -4.8; 7.6 / -4.5; 4.2
r² / 0.01 / 0.34 / 0.51 / 0.76 / 0.02 / 0.13 / 0.03 / 0.0
p / <0.718 / <0.017 / <0.001 / <0.001 / <0.709 / <0.345 / <0.662 / <0.857

Table S6 (cont.): Time trend analysis of arsenic and metals in bream from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Bream muscle / Bream liver
Arsenic / Lead / Copper / Mercury / Lead / Cadmium / Copper / Zinc
Rhine / R1
Weil / Period / 1995-2011 / 1995-2011 / 1995-2011 / 1995-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 16 / 15 / 16 / 16 / 9 / 9 / 9 / 9
Yearly trend / 3.5% increase / -5.7% decrease / 0.3% n.s. / -3.3% decrease / 0.7% n.s. / -1.8% n.s. / 7.5% n.s. / 2.6% n.s.
95%-CI / 1.3; 5.5 / -11; -0.2 / -1.7; 2.3 / -5.6; -1.1 / -11; 12 / -17; 16 / -2.8; 18 / -1.9; 7.5
r² / 0.47 / 0.28 / 0.01 / 0.41 / 0.0 / 0.01 / 0.29 / 0.21
p / <0.003 / <0.04 / <0.741 / <0.007 / <0.861. / <0.795 / <0.131 / <0.215
R2
Iffezheim / Period / 1995-2011 / 1995-2011 / 1995-2011 / 1995-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 17 / 16 / 17 / 17 / 9 / 9 / 9 / 9
Yearly trend / 2.0% n.s. / -4.8% n.s. / -0.6% n.s. / -1.3% n.s. / -2.4% n.s. / -1.0% n.s. / -0.5% n.s. / -0.8% n.s.
95%-CI / 0.0; 4.2 / -11; 2.5 / -2.3; 1.0 / -2.9; 0.3 / -7.0; 2.4 / -8.6; 7.3 / -2.9; 1.9 / -2.4; 0.7
r² / 0.22 / 0.12 / 0.04 / 0.17 / 0.17 / 0.01 / 0.03 / 0.20
p / <0.052 / <0.177 / <0.419 / <0.095 / <0.277 / <0.770 / <0.648 / <0.220
R3
Koblenz / Period / 1995-2011 / 1995-2011 / 1995-2011 / 1995-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 17 / 16 / 17 / 17 / 9 / 9 / 9 / 9
Yearly trend / 2.5% n.s. / -6.0% decrease / -0.9% n.s. / -0.9% n.s. / 1.6% n.s. / 30% increase / 4.8% n.s. / 2.8% n.s.
95%-CI / 0.6; 4.6 / -9.5; -2.1 / -1.9; 0.2 / -3.7; 1.9 / -4.7; 8.4 / 18; 42 / -2.8; 13 / -1.2; 7,0
r² / 0.33 / 0.43 / 0.17 / 0.03 / 0.05 / 0.87 / 0.24 / 0.28
p / <0.015 / <0.005 / <0.096 / <0.498 / <0.574 / <0.001 / <0.178 / <0.144
R4
Bimmen / Period / 1995-2011 / 1995-2011 / 1995-2011 / 1995-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 17 / 16 / 17 / 17 / 9 / 9 / 9 / 9
Yearly trend / 4.0% increase / -6.6% decrease / -1.6% decrease / -4.0% decrease / -2.8% n.s. / -4.3% n.s. / -1.3% n.s. / -0.8% n.s.
95%-CI / 2.1; 6.0 / -8.5; -4.5 / -3.0; -0.2 / -6.7; -1.4 / -13; 9.3 / -22; 17 / -11; 9.7 / -6.9; 5.7
r² / 0.59 / 0.76 / 0.30 / 0.41 / 0.04 / 0.04 / 0.01 / 0.01
p / <0.001 / <0.001 / <0.023 / <0.005 / <0.591 / <0.627 / <0.771 / 0.758

Table S6 (cont.): Time trend analysis of arsenic and metals in bream from the German ESB sites using the PIA programme (Bignert 2007), alpha 5%; power 80%

Water / Sampling site / Parameters / Bream muscle / Bream liver
Arsenic / Lead / Copper / Mercury / Lead / Cadmium / Copper / Zinc
Saar / S1
Güdingen / Period / 1994-2011 / 1994-2011 / 1994-2011 / 1994-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 18 / 17 / 18 / 18 / 9 / 9 / 9 / 9
Yearly trend / 5.5% increase / -6.3% decrease / -0.8% n.s. / 0.3% n.s. / -2.3% n.s. / 6.6% n.s. / 3.9% n.s. / 2.0% n.s.
95%-CI / 3.1; 8.0 / -9.5; -2.6 / -1.5; 0.0 / -1.1; 1.6 / -7.8; 3.7 / 0.6; 13 / -4.8; 13 / -2.5; 6.6
r² / 0.60 / 0.46 / 0.21 / 0.01 / 0.11 / 0.49 / 0.13 / 0.13
p / <0.001 / <0.003 / <0.055 / <0.684 / <0.392 / <0.035 / <0.342 / <0.337
S2
Rehlingen / Period / 1994-2011 / 1994-2011 / 1994-2011 / 1994-2011 / 2002-2010 / 2002-2010 / 2002-2010 / 2002-2010
No of values / 18 / 17 / 18 / 18 / 9 / 9 / 9 / 9
Yearly trend / 3.4% increase / -5.9decrease / -1.0% n.s. / 0.3% n.s. / 2.8% n.s. / 9.7% increase / 1.5% n.s. / 1.1% n.s.
95%-CI / 1.1; 5.8 / -8.8; -3.1 / -2.0; -0.1 / -1.0; 1.6 / -0.7; 6.5 / 2.5; 17 / -3.3; 6.5 / -2.2; 4.4
r² / 0.37 / 0.55 / 0.24 / 0.01 / 0.34 / 0.60 / 0.07 / 0.08
p / <0.007 / <0.001 / <0.037 / <0.641 / <0.095 / <0.015 / <0.501 / <0.460