Applied Geochemistry 27 (2012) 1492–1498

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Applied Geochemistry
journal homepage: www.elsevier.com/locate/apgeochem

Temperature-dependent leaching of chemical elements from mineral water

bottle materials
Clemens Reimann a,⇑, Manfred Birke b, Peter Filzmoser c
a
Norges Geologiske Undersøkelse (NGU), Postbox 6315, Sluppen, N-7491 Trondheim, Norway
b
Bundesanstalt für Geowissenschaften und Rohstoffe (BGR), Stilleweg 2, 30655 Hannover, Germany
c
Department of Statistics and Probability Theory, Vienna University of Technology, Wiedner Hauptstr. 8-10, 1040 Vienna, Austria

a r t i c l e i n f o a b s t r a c t

Article history: It is well established that minute amounts of chemical elements will leach from bottle materials (glass or
Received 1 March 2012 PET – polyethylene terephthalate) to water stored in such bottles. This study investigated whether leach-
Accepted 6 May 2012 ing increases with storage temperature. For glass bottles this is clearly the case for a long list of elements:
Available online 14 May 2012
Ag, Al, As, B, Ba, Ca, Co, Cr, Cs, Cu, Fe, Ga, Ge, K, La, Li, Mg, Mo, Na, Ni, Pb, Rb, Sb, Se, Sn, Sr, Ti, U, V, W and Zr.
Editorial handling by R. Fuge
However, for glass bottles drinking water maximum admissible concentration values as defined by Euro-
pean authorities are not exceeded even after 1 week of leaching at 80 °C. The critical temperature limit
where leaching substantially increases for many elements appears to be 45 °C. For PET bottles, Sb is
the only element where leaching is observed at all temperatures and again leaching strongly increases
at 45 °C. For PET bottles Sb concentrations observed in water after 1 week storage at 80 °C reach almost
four times the maximum admissible concentration values for drinking water but do not exceed the rel-
evant higher limit for food (including water) packaged in PET.
Ó 2012 Elsevier Ltd. All rights reserved.

1. Introduction health-relevant concentrations. Reimann et al. (2010) reported re-

Bottled water is increasingly replacing tap water as the main in-
take of drinking water in several European countries (e.g., Eisen-
bach, 2004; see Fig. 6 in Reimann and Birke (2010)). It is sold in
cheap plastic or glass bottles and is often stored in these bottles
under unpredictable conditions for several months before con-
sumption. Misund et al. (1999) found clear indications for contam-
ination of the water by the bottle materials, e.g., with Pb and Zr
from glass bottles. More recently it has been convincingly demon-
strated that glass bottles will contaminate bottled water with Pb
while many polyethylene terephthalate (PET) bottles contaminate
the water with Sb. Concentrations of the investigated elements in-
creased with storage time (Shotyk et al., 2006; Shotyk and Krach-
ler, 2007a,b; Krachler and Shotyk, 2009). Keresztes et al. (2009)
report Sb concentrations of 210–290 mg/kg in PET from Hungarian
mineral water bottles, and significant leaching of Sb to the water
depending on storage conditions and bottle volume. Welle and
Franz (2011) report median concentrations of 220 mg/kg Sb in
PET bottle materials and determined diffusion coefficients for Sb
in PET bottles in a temperature range between 105 and 150 °C.
They concluded that Sb levels of water in PET bottles will not reach
⇑ Corresponding author.
E-mail address: clemens.reimann@ngu.no (C. Reimann).
sults from a leaching test covering 57 chemical elements for glass
and PET bottles of different color and concluded that water stored
in PET bottles will be almost invariably contaminated with Sb,
while glass bottles contaminate the water with a much longer list
of elements (Pb, Al, Zr, Ti, Th, La, Pr, Fe, Zn, Nd, Sn, Cr, Tb, Er, Gg, Tb,
Bi, Sm, Y, Lu, Yb, Tm, Nb and Cu). Concentrations of these elements
in the water usually increased with storage time. In addition an
influence of bottle color on the leaching results could be demon-
strated. In a comment to the paper by Reimann et al. (2010), Mül-
ler-Simon (2010) pointed out that leaching of Pb from glass to
water stored in glass bottles should not take place due diffusion
coefficients being far too low. Based on that comment it was
decided to study the leaching of chemical elements from a variety
of glass bottles in three different colors in comparison to a few PET
bottles at different temperatures in a range from 2 to 80 °C because
if diffusion is a relevant process during leaching, the concentra-
tions of elements affected should increase with temperature. Re-
sults are used to investigate the following questions:
(1) Which elements show a trend to increasing concentrations
with increasing temperature of leaching and which elements
remain unaffected?
(2) What are the differences between different bottle colors?
(3) What are the differences between the two main bottle mate-
rials glass and PET?

0883-2927/$ - see front matter Ó 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.apgeochem.2012.05.003
Table 1
Total element concentrations (XRF analyses) in 10 glass bottles (5 clear, 3 blue and 2 green). Some exceptionally high values are marked in bold and underscored.

ID Color SiO2 (wt.%) TiO2 (wt.%) Al2O3 (wt.%) Fe2O3 (wt.%) MnO (wt.%) MgO (wt.%) CaO (wt.%) Na2O (wt.%) K2O (wt.%) P2O5 (wt.%)
146-C-GLA Blue 72.03 0.058 1.86 0.12 0.013 2.56 10.10 12.20 0.648 0.020
280-C-GLA Blue 71.24 0.055 1.71 0.20 0.015 3.27 9.83 12.72 0.538 0.016
558-C-GLA Blue 72.39 0.037 1.43 0.08 0.010 2.26 10.19 12.71 0.524 0.019
082-C-GLA Green 71.50 0.052 1.70 0.14 0.013 3.06 9.94 12.64 0.630 0.016
ITA001-1 Green 71.81 0.052 2.07 0.35 0.017 1.24 10.24 12.73 0.969 0.020
819-S-GLA Clear 72.42 0.038 1.25 0.08 0.008 3.16 9.57 12.41 0.624 0.020
660-S-GLA Clear 72.63 0.039 1.25 0.08 0.010 2.95 9.86 12.20 0.580 0.019
522-M-GLA Clear 71.00 0.039 1.51 0.07 0.011 2.75 10.59 13.05 0.525 0.018
HUN023-1 Clear 73.02 0.036 1.58 0.06 0.004 0.70 10.68 12.24 1.028 0.018

C. Reimann et al. / Applied Geochemistry 27 (2012) 1492–1498

130-S-GLA Clear 72.51 0.029 1.43 0.08 0.010 2.20 10.21 12.62 0.523 0.019
ID Color As (mg/ Ba (mg/ Bi (mg/ Ce (mg/ Co (mg/ Cr (mg/ Cu (mg/ Nb (mg/ Ni (mg/ Pb (mg/ Rb (mg/ Sb (mg/ Sc (mg/ Sn (mg/ Sr (mg/ Th (mg/ Y (mg/ Zn (mg/ Zr (mg/
kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg) kg)
146-C- Blue 10 392 <2 22 24 17 10 3 <2 88 16 <8 3 20 177 7 8 125 128
GLA
280-C- Blue 8 236 4 <18 27 19 11 3 14 72 14 9 2 28 155 9 9 77 129
GLA
558-C- Blue 11 325 4 <18 32 44 8 4 2 117 12 <8 2 10 162 5 8 84 68
GLA
082-C- Green 14 466 <2 27 4 29 13 <2 4 193 16 11 3 22 131 7 9 39 111
GLA
ITA001-1 Green 18 459 4 <18 7 1165 23 3 10 313 32 43 3 31 105 5 9 48 107
819-S- Clear 15 531 <2 22 <3 23 10 4 <2 256 19 9 <1 31 79 6 7 58 90
GLA
660-S- Clear 19 516 <2 30 <3 20 8 3 2 282 17 13 3 30 87 8 6 59 88
GLA
522-M- Clear 14 379 <2 23 <3 16 6 <2 <2 152 12 13 3 9 149 7 9 47 94
GLA
HUN023- Clear 8 1925 <2 <18 6 18 7 <2 <2 84 27 57 2 7 74 10 8 366 115
1
130-S- Clear 10 316 3 <18 <3 15 8 <2 <2 109 14 <8 2 6 159 6 6 37 68
GLA

1493
 1494
Table 2
Summary of the analytical results from the leaching test at different temperatures. Elements where no effect was observed are not shown. Values in bold indicate the onset of increased leaching. All values in lg/L.

Material Color N Temp. (°C) Ag Al As B Ba Ca Co Cr Cs Cu Fe

Glass Clear 9 2 Med <0.001 8.9 <0.01 0.285 <0.1 23.2 <0.002 <0.03 0.00164 0.0544 0.163
Max <0.001 32.7 0.0122 0.484 1.4 6610 0.00702 0.0469 0.0204 7.66 8.86
22 Med <0.001 15.25 <0.01 0.232 0.0035 27.2 <0.002 <0.03 0.00059 0.09635 0.423
Max <0.001 50.4 0.0269 0.409 1.99 7440 0.00733 0.0759 0.0201 7.34 18.3
45 Med <0.001 5.3 0.0175 0.345 0.692 148 <0.002 <0.03 0.00197 0.042 0.264
Max 0.00256 10.9 0.0316 0.435 2.48 7510 0.00767 0.0839 0.0217 7.5 19.1
60 Med <0.001 5.42 0.0347 0.578 1.51 331 0.00297 <0.03 0.00372 0.0541 0.268
Max 0.00268 16.1 0.074 0.732 3.2 7840 0.0386 0.0798 0.0242 7.58 19.2
80 Med 0.00134 18.7 0.128 1.6 4.45 1100 0.00529 0.0372 0.00993 0.1 0.763
Max 0.00876 41.1 0.305 2.29 8.91 8360 0.0163 0.087 0.0414 3.66 18.8
Glass Blue 23 2 Med <0.001 9.61 <0.01 0.399 0.364 204 0.0285 0.0375 0.001 0.0783 1.32
Max <0.001 13.9 <0.01 0.609 6.39 8390 0.0719 0.158 0.00331 0.22 8.4
22 Med <0.001 9.47 <0.01 0.287 0.48 218 0.0322 0.0657 <0.001 0.0744 1.73
Max 0.00164 12.9 0.011 0.5 11 12600 0.0767 0.182 0.00285 0.183 10.9

C. Reimann et al. / Applied Geochemistry 27 (2012) 1492–1498

45 Med 0.0016 10.7 0.0251 0.491 1.13 353 0.0794 0.0643 0.00293 0.103 2.68
Max 0.0384 82.4 0.18 2.09 16.5 14900 0.202 0.215 0.00691 0.546 11.4
60 Med 0.00312 12.2 0.0747 1.03 2.2 723 0.115 0.0891 0.00581 0.155 1.67
Max 0.0574 143 0.347 3.55 20 16200 0.273 0.322 0.0116 0.953 9.2
80 Med 0.00519 20.4 0.253 2.66 4.83 1550 0.181 0.168 0.0176 0.232 2.98
Max 0.0822 422 1.18 11.7 35.5 16200 0.62 1.05 0.0678 0.856 7.91
Glass Green 5 2 Med <0.001 10.7 <0.01 0.384 0.443 36.5 0.00336 0.0936 0.00139 0.538 1.72
Max <0.001 11.3 <0.01 0.509 2.45 11000 0.0174 0.234 0.00241 0.825 2.2
22 Med <0.001 11.9 <0.01 0.329 0.531 59.7 0.00407 0.0698 0.00109 0.636 0.71
Max <0.001 12.3 <0.01 0.375 3.44 14200 0.00971 0.375 0.00131 1.36 4.96
45 Med <0.001 13.1 0.0199 0.357 0.882 85.2 0.00882 0.602 0.00365 0.76 1.62
Max 0.00113 66.2 0.123 1.19 6.92 15400 0.0675 0.723 0.0123 2.33 5.3
60 Med 0.00116 16.3 0.028 0.575 1.26 130 0.0131 0.811 0.00442 0.782 1.81
Max 0.00327 116 0.231 2.14 9 16600 0.107 1.06 0.0209 2.86 5.36
80 Med 0.00366 30.2 0.0787 0.746 2.51 399 0.0192 1.67 0.00801 1.08 5.22
Max 0.00872 367 0.79 5.39 19.2 13000 0.0643 3.13 0.0626 3.8 9.55
PET 3 2 Med <0.001 <0.3 <0.01 0.247 <0.1 <10 <0.002 <0.03 <0.001 0.0369 <0.1
Max <0.001 <0.3 <0.01 0.25 0.142 11.3 0.00689 <0.03 <0.001 0.107 0.165
22 Med <0.001 <0.3 <0.01 0.2 <0.1 <10 <0.002 <0.03 <0.001 0.0316 <0.1
Max <0.001 <0.3 <0.01 0.203 0.295 10.5 0.0169 <0.03 <0.001 0.115 0.46
45 Med <0.001 <0.3 <0.01 0.198 <0.1 <10 0.00366 <0.03 <0.001 0.031 <0.1
Max <0.001 <0.3 <0.01 0.198 0.433 <10 0.0235 <0.03 <0.001 0.119 0.812
60 Med <0.001 <0.3 <0.01 0.238 <0.1 11.5 0.00522 <0.03 <0.001 0.0286 <0.1
Max <0.001 0.825 0.0212 0.709 1.76 76.7 0.0249 <0.03 <0.001 0.137 0.898
80 Med <0.001 <0.3 0.0182 0.271 <0.1 <10 0.0259 <0.03 <0.001 0.0256 <0.1
Max <0.001 <0.3 0.109 0.276 3.14 11.9 0.0408 <0.03 <0.001 0.129 1.26

Material Color N Temp. (°C) Ga Ge K La Li Mg Mo Na Ni Pb Rb Sb Se Sn

Glass Clear 9 2 Med 0.000653 <0.005 <10 0.00174 <0.1 1.1 <0.001 <10 0.0405 0.0236 0.00365 <0.002 <0.01 0.00545
Max 0.00168 <0.005 10.2 0.0127 <0.1 80.9 0.00624 22.8 0.0493 0.955 0.033 0.0119 <0.01 0.0209
22 Med 0.000737 <0.005 <10 0.0007385 <0.1 2.105 <0.001 <10 0.04365 0.0484 0.00359 <0.002 <0.01 0.004485
Max 0.00391 <0.005 11.8 0.0135 <0.1 116 0.00199 78.8 0.0609 0.995 0.0368 0.0163 <0.01 0.0139
45 Med 0.000561 <0.005 11.2 0.00202 <0.1 11.6 0.00149 223 0.0449 0.193 0.0292 0.00974 <0.01 0.00517
Max 0.00138 <0.005 18.4 0.0136 <0.1 126 0.00763 366 0.0615 0.938 0.0567 0.036 <0.01 0.015
60 Med 0.000547 <0.005 23.3 0.00374 <0.1 27.5 0.00271 453 0.0512 0.269 0.065 0.0299 <0.01 0.00481
Max 0.00259 <0.005 39.5 0.0142 0.116 135 0.0195 827 0.0633 0.856 0.117 0.0658 <0.01 0.0117
80 Med 0.0012 0.00741 77.8 0.00763 0.251 54 0.00846 1950 0.0523 0.448 0.227 0.113 <0.01 0.0036
Max 0.00355 0.00922 109 0.0163 0.489 216 0.0605 2640 0.0662 1.3 0.371 0.394 0.022 0.0216
Glass Blue 23 2 Med 0.00105 <0.005 <10 0.00936 <0.1 9.13 0.00198 12.4 0.06 0.237 0.00867 0.00216 <0.01 0.00709
 Max 0.00186 <0.005 10.1 0.0142 0.134 75 0.00476 103 0.0984 0.551 0.0141 0.00917 0.0102 0.0949
22 Med <0.0005 <0.005 <10 0.00803 <0.1 10.2 0.00126 63.4 0.0554 0.223 0.0113 0.00242 <0.01 0.00486
Max 0.00161 <0.005 <10 0.0131 0.177 96.2 0.00362 165 0.354 0.618 0.0182 0.00874 <0.01 0.0424
45 Med 0.000725 <0.005 16.2 0.00977 <0.1 41.4 0.00263 615 0.0602 0.299 0.0419 0.0119 <0.01 0.00618
Max 0.00755 0.00805 53.6 0.0173 0.34 222 0.0154 1180 0.118 0.804 0.172 0.0758 <0.01 0.0599
60 Med 0.00054 <0.005 42.3 0.0107 0.173 74.6 0.00671 1530 0.0703 0.354 0.0977 0.0414 <0.01 0.00798
Max 0.0146 0.0139 142 0.019 0.488 319 0.0698 3520 0.138 0.933 0.305 0.181 0.0414 0.132
80 Med 0.0014 0.0137 117 0.0138 0.556 138 0.0179 4690 0.0744 0.564 0.302 0.18 0.0118 0.0149
Max 0.0588 0.0522 498 0.0545 1.43 905 0.263 11500 0.187 1.33 1.22 0.946 0.153 0.333
Glass Green 5 2 Med <0.0005 <0.005 <10 0.00349 <0.1 3.03 0.00216 <10 0.0777 0.184 0.0105 <0.002 <0.01 0.0101
Max 0.000864 <0.005 11.9 0.012 <0.1 141 0.00266 48.6 0.151 0.206 0.0214 0.00316 <0.01 0.029
22 Med <0.0005 <0.005 <10 0.00151 <0.1 5.46 0.00134 14.1 0.0617 0.253 0.0136 0.00261 <0.01 0.0181
Max 0.000661 <0.005 <10 0.00551 0.122 164 0.00147 130 0.122 0.274 0.0144 0.00591 <0.01 0.036
45 Med 0.000705 <0.005 12.1 0.00234 <0.1 10.6 0.00148 238 0.0549 0.361 0.0368 0.0136 <0.01 0.0358
Max 0.00928 0.00691 57.9 0.00683 0.279 279 0.00615 1470 0.138 0.403 0.154 0.0869 <0.01 0.0505
60 Med 0.000859 <0.005 16.1 0.00259 <0.1 15.3 0.00299 448 0.0791 0.404 0.0484 0.0249 <0.01 0.0379
Max 0.0162 0.0123 99.2 0.00761 0.426 355 0.011 2640 0.15 0.46 0.273 0.149 <0.01 0.0693
80 Med 0.00159 <0.005 36.2 0.00642 0.131 34.2 0.00392 1460 0.0673 0.598 0.119 0.0714 <0.01 0.0503
Max 0.041 0.0397 286 0.0134 0.981 788 0.0286 7500 0.0719 0.742 0.958 0.481 0.0195 0.163

C. Reimann et al. / Applied Geochemistry 27 (2012) 1492–1498

PET 3 2 Med <0.0005 <0.005 <10 0.000609 <0.1 <1 <0.001 <10 0.0263 0.00388 <0.001 0.00276 <0.01 0.00194
Max <0.0005 <0.005 <10 0.00317 <0.1 <1 0.00112 <10 0.0492 0.006 0.00143 0.0233 <0.01 0.00205
22 Med <0.0005 <0.005 <10 <0.0005 <0.1 <1 <0.001 <10 0.0326 0.00422 <0.001 0.0117 <0.01 0.00102
Max <0.0005 <0.005 <10 0.00406 <0.1 <1 <0.001 <10 0.0485 0.00884 <0.001 0.0541 <0.01 0.00137
45 Med <0.0005 <0.005 <10 <0.0005 <0.1 <1 <0.001 <10 0.0305 0.00485 <0.001 1.24 <0.01 0.00191
Max <0.0005 <0.005 <10 0.00617 <0.1 <1 <0.001 <10 0.0523 0.0101 0.00392 1.52 <0.01 0.00203
60 Med <0.0005 <0.005 <10 <0.0005 <0.1 <1 <0.001 <10 0.0325 0.00601 <0.001 2.75 <0.01 0.00192
Max 0.000605 <0.005 <10 0.00636 <0.1 <1 0.0038 <10 0.0471 0.0213 0.0017 3.32 <0.01 0.00203
80 Med <0.0005 <0.005 <10 0.00073 <0.1 <1 <0.001 <10 0.0378 0.00696 0.00129 10.9 <0.01 0.00298
Max <0.0005 <0.005 <10 0.00749 <0.1 <1 0.00115 <10 0.0435 0.013 0.00142 15.8 <0.01 0.00311
Material Color N Temp. (°C) Sr Ti U V W Zr
Glass Clear 9 2 Med 0.184 <0.01 0.00136 <0.01 0.0022 <0.001
Max 10.8 0.0554 0.0138 <0.01 0.00505 0.00541
22 Med 0.126 0.0119 0.000885 <0.01 <0.002 <0.001
Max 16.5 0.0866 0.015 <0.01 0.00438 0.00321
45 Med 0.373 0.0211 0.00124 <0.01 <0.002 <0.001
Max 17.5 0.0366 0.0133 0.0126 0.00326 0.00311
60 Med 0.796 0.0198 0.00206 0.0147 0.00246 0.00113
Max 17.6 0.0777 0.0132 0.0368 0.0111 0.00532
80 Med 1.69 0.0695 0.00272 0.0648 0.00553 0.00629
Max 18 0.145 0.0113 0.188 0.00817 0.0385
Glass Blue 23 2 Med 0.659 0.0951 0.00281 <0.01 0.00301 0.0016
Max 49.5 0.182 0.0117 <0.01 0.00597 0.00366
22 Med 0.67 0.0847 0.00308 <0.01 <0.002 <0.001
Max 80.7 0.306 0.0219 <0.01 0.0035 0.00954
45 Med 0.928 0.171 0.0032 0.0119 0.00255 <0.001
Max 91.5 0.504 0.037 0.043 0.0093 0.0843
60 Med 1.8 0.173 0.00358 0.0316 0.00412 0.001
Max 95 0.838 0.0468 0.0839 0.0301 0.16
80 Med 4.13 0.133 0.00399 0.111 0.0106 0.00525
Max 100 2.68 0.0381 0.282 0.0816 0.907
Glass Green 5 2 Med 0.187 0.0222 0.000905 <0.01 0.0022 0.00141
Max 73.4 0.0406 0.0112 <0.01 0.00318 0.00374
22 Med 0.359 0.0152 0.00106 <0.01 <0.002 <0.001
Max 99.5 0.11 0.0207 <0.01 0.00277 0.00317
45 Med 0.294 0.038 0.00148 <0.01 0.00214 <0.001
Max 108 0.161 0.0324 0.0659 0.0156 0.0119

1495
(continued on next page)
1496 C. Reimann et al. / Applied Geochemistry 27 (2012) 1492–1498

2. Material and methods

0.00537
<0.001

<0.001
<0.001
<0.001
<0.001
<0.001
<0.001
<0.001
<0.001
<0.001
<0.001
0.021

0.11 Forty mineral water bottles bought in supermarkets from all

Zr

over Europe were used for this test: 23 blue glass bottles, 9 clear
glass bottles, 5 green glass bottles and for comparison 3 PET bot-
tles. The volume of the bottles was 1.5 L. These bottles were thor-
oughly (3 times) rinsed with high purity (demineralised) water,
filled with demineralised water (SERALPUR-90, 18.2 MX) and
0.00382

0.00532

0.00218

0.00843
0.00207
0.0153

0.0281

<0.002
<0.002
<0.002
<0.002
<0.002

<0.002
<0.002
25 lL 69% HNO3 (Roth Suprapure, density 1.41 kg/L) was added/L
to acidify the water to pH 3.5 under clean room conditions. After
W

filling the bottles they were stored for 1 week at different temper-
atures (2, 22, 45, 60, 80 °C) before determination of the concentra-
tions of 60 elements (Ag, Al, As, B, Ba, Be, Bi, Br, Ca, Cd, Ce, Co, Cr, Cs,
Cu, Dy, Er, Eu, Fe, Ga, Gd, Ge, Hf, Hg, Ho, I, K, La, Li, Lu, Mg, Mn, Mo,
Na, Nb, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Sm, Sn, Sr, Ta, Tb, Te, Th, Ti, Tl,
0.0157

0.0437
0.121

0.431
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01

Tm, U, V, W, Y, Yb, Zn and Zr) in the water using an inductively cou-

V

pled plasma quadrupole mass spectrometer (ICP-QMS – Agilent

7500ce). The instrument is equipped with a standard peristaltic
pump, a MicroMist concentric nebulizer, a Peltier-cooled spray
chamber, the Plasma Forward Power and the Shield Torch System.
The methods used are in accordance with the German norms DIN
0.000699

0.000968
0.000507
0.00217

0.00332

0.00084
<0.0005
0.0573

0.0741

0.0616

0.0861
0.0399

0.0456
0.0404

38406-E29 (ICP-MS). All details on the analytical procedure, iso-

topes measured, detection limits and quality control are detailed
U

in the previous paper (Reimann et al., 2010) and in even more de-
tail in a recent book (Reimann and Birke, 2010).
To document likely average element concentrations in glass, 10
bottles (5 clear, 3 blue and 2 green) were destroyed and milled in
an agate disk mill. Subsequently, 1 g of milled glass was mixed
0.0704
0.184
0.231
0.348
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01
<0.01

with 5 g lithium metaborate and 25 mg lithium bromide in Pt95–

Ti

Au5 crucibles and fused for 20 min at 1200 °C in an automatic flux-

er (HAG 12–1500). Total concentrations of 10 major elements
(Al2O3, CaO, Fe2O3, K2O, MgO, MnO, Na2O, P2O5, SiO2 and TiO2)
and 30 trace elements (As, Ba, Bi, Ce, Co, Cr, Cs, Cu, Ga, Hf, La,
Mo, Nb, Nd, Ni, Pb, Rb, Sb, Sc, Sm, Sn, Sr, Ta, Th, U, V, W, Y, Zn,
0.362

0.836

0.119
0.163

0.147

0.139
0.156
0.166
0.113
0.144
<0.1

<0.1
115

115

Zr) were determined by wavelength dispersive X-ray fluorescence

Sr

spectrometry (WD-XRFS) using PAN2400 and AXIOS WD-XRFs

with Cr- and Rh-anode X-ray tubes, respectively. To correct for ma-
trix effects and spectral interferences calibration curves were con-
structed using 130 certified reference materials. In addition, special
Med

Med

Med

Med

Med

Med

Med

certified reference materials (SpS, Glass sand, IMRM) were ana-

Max

Max

Max

Max

Max

Max

Max

lyzed together with the glass samples; all results were within 5%
of the reference values. It was not possible to analyze the PET
bottles because this requires a special cryogenic mill. Antimony
concentrations in PET (200–300 mg/kg) are, however, well estab-
lished in the literature (Keresztes et al., 2009; Welle and Franz,
Temp. (°C)

2011).
22

45
60

80

60

80
2

3. Results and discussion

Table 1 shows concentrations of the 10 major oxides and 19

trace elements as found in glass bottles. For the remaining trace
elements analyzed, either all or the majority of results were below
N

the respective detection limits (Cs: 3, Ga: 2, Hf: 6, La: 15, Mo: 3,
Nd: 13, Sm: 14, Ta: 4, U: 3, V: 6, W: 4 mg/kg). While the variation
for the major oxides is small (but note Fe in green and blue bottles),
trace element concentrations can vary substantially from bottle to
bottle. The blue bottles show 4–5 times higher Co concentrations
Color

in the glass than all other bottles, one green bottle returned an ex-
treme Cr concentration of 1165 mg/kg. Otherwise variation in ele-
ment concentrations does not appear to depend on color, there are
Table 2 (continued)

only single or few bottles that show extreme concentrations for

certain elements, like the maximum concentration for Ba of
1925 mg/kg in a clear bottle, or for Zn of 366 mg/kg in another
Material

clear bottle. The median Pb concentration in glass is 135 mg/kg,

PET

however, 4 bottles (2 clear, 2 green) show values between 193

and 313 mg/kg. Two high values of Sb, 43 and 53 mg/kg, in a green
 C. Reimann et al. / Applied Geochemistry 27 (2012) 1492–1498 1497

Fig. 1. Boxplot comparison of leaching from different bottle materials and colors at different temperatures (2, 22, 45, 60, 80 °C). Storage time: 1 week at indicated
temperature. All values in lg/L.

and a clear bottle are also noteworthy. These large differences in Table 2 summarizes the results of 1 week leaching at different
the bottle composition explain the outliers observed in the leach- temperatures for those elements that are strongly leaching to the
ing experiment reported in Reimann et al. (2010). water and where a clear influence of temperature on bottle leach-
1498 C. Reimann et al. / Applied Geochemistry 27 (2012) 1492–1498
ing was observed (Ag, Al, As, B, Ba, Ca, Co, Cr, Cs, Cu, Fe, Ga, Ge, K,
La, Li, Mg, Mo, Na, Ni, Pb, Rb, Sb, Se, Sn, Sr, Ti, U, V, W and Zr).
Though some leaching must again be noted for almost all ele-
ments, especially from the glass bottles, no clear effect of temper-
ature on leaching was found for Be, Bi, Br, Cd, Ce, Dy, Er, Eu, Gd,
Hf, Hg, Ho, I, Lu, Mn, Nb, Nd, Pr, Sc, Sm, Ta, Tb, Te, Th, Tl, Tm, Y,
Yb and Zn. Table 2 demonstrates that for the remaining elements
temperature has a clear effect on how much of an element leaches
from the bottle material to the water. Note the very low concen-
trations reported for most elements in the PET bottles – for most
elements (except Sb) it is actually possible to judge the effect of
leaching against the minimum concentrations observed in the
PET bottles.
Fig. 1 shows examples of the different behavior for temperature
dependent leaching from the different bottle colors and materials.
Strong leaching effects usually start at a temperature of 45–60 °C
and in most cases leaching increases with temperature (see As
and V as typical examples). Significant differences are observed
for the different glass bottle colors and blue glass bottles (closely
followed by the green variety) usually leach more and at lower
temperatures than the clear bottles. Cobalt is an element where
the effect is well visible for the blue bottles, for green glass bottles
the equivalent is visible in the boxplots for Cr (Fig. 1). This is not
unexpected in the light of the results presented in Table 1. Lead
is one of the elements where relatively high values are observed
in water stored in the glass bottles when compared to the same
water stored in PET, the difference is almost 2 orders of magnitude
at all temperatures. Clear glass bottles show a strong increase of Pb
concentrations with temperature, while this increase is small for
blue and green glass bottles, mostly because the colored glass bot-
tles begin with quite high Pb concentrations in the water after
1 week of storage at 2 °C. There can thus be little doubt that some
Pb is leaching from the glass to the water and that diffusion from
the glass to the water is a likely process. The diagrams also demon-
strate that the leaching effect can be fairly small (1–2 orders of
magnitude, e.g., V in Fig. 1) but can also cover up to 4–5 orders
of magnitude for the observed element concentration (e.g., Sb in
Fig. 1).
Antimony is the only element that shows opposite behavior for
glass and PET (Fig. 1), the water in the PET bottles shows higher Sb
concentrations after only a week of storage at 2 °C. There is a clear
increase of Sb concentrations in the water with an increase of
temperature for both bottle materials and for all colors. PET bottles
show a strong increase of Sb concentrations at temperatures above
45 °C (see Fig. 1). At 60 °C the maximum admissible concentration
for drinking water of 5 lg/L Sb (European Union, 1998) is almost
reached. At 80 °C a maximum value of 18 lg/L Sb is observed.
The interesting situation here is that while the maximum admissi-
ble concentration for drinking water is set to 5 lg/L (European
Union, 1998) this value is no longer valid once the water is pack-
aged in PET, at that moment the packaging guideline values are va-
lid and for Sb the value is now 40 lg/L (European Union, 2011),
eight times the maximum admissible concentration for drinking
water. The questions raised with regards to defining maximum
admissible concentration values for drinking water in Reimann
and Banks (2004) appear to be as relevant in 2012 as they were
in 2004.
4. Conclusions
The results of the analysis of 10 glass bottles show large varia-
tions in the trace element content of the glass and surprisingly high
maximum values (e.g., Ba, Cr, Pb, Zn). These results indicate that a
larger survey into the trace element chemistry of commercial glass
ware might be justified.
When drinking water is stored in glass or PET bottles certain
chemical elements will leach over time from the bottle material
to the water. Considerably more elements leach from glass than
from PET bottles. For certain elements (Ag, Al, As, B, Ba, Ca, Co,
Cr, Cs, Cu, Fe, Ga, Ge, K, La, Li, Mg, Mo, Na, Ni, Pb, Rb, Sb, Se, Sn,
Sr, Ti, U, V, W and Zr) leaching increases with storage temperature,
while others (Be, Bi, Br, Cd, Ce, Dy, Er, Eu, Gd, Hf, Hg, Ho, I, Lu, Mn,
Nb, Nd, Pr, Sc, Sm, Ta, Tb, Te, Th, Tl and Tm) appear unaffected by
temperature. Although element concentrations in the water can
increase by 1–2 orders of magnitude due to the contact with the
bottle walls, maximum admissible concentrations for drinking
water as defined by the European authorities are usually not ex-
ceeded. Leaching from PET bottles is pronounced for Sb, but this
is practically the only element leaching from PET. A substantial in-
crease of Sb concentrations occurs when the water in the bottles
reaches a temperature of more than 40 °C. At 80 °C the maximum
admissible concentration for drinking water for Sb is already ex-
ceeded by a factor of almost four. It can be concluded that storage
conditions are important for bottled water quality and that storage
of water in PET bottles at temperatures above 40 °C should be
avoided.
Acknowledgements
We wish to thank our colleagues Hans Lorenz of the ICP-MS lab
and Frank Korte of the XRF lab at BGR for providing and analyzing
the leachates and the 10 glass bottles.
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