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INTRODUCTION
Bottled water is a beverage that is rapidly gaining in popularity.
World consumption in 2007 was in excess of 200 million liters.
According to the latest report in Worlds Water,1 the average
annual consumption is over 100 liters per person in 15 countries
from the world ranking, and over 200 liters per person in the
countries at the top of this ranking, namely Mexico, Italy, and the
United Arab Emirates.
The constantly rising popularity of bottled waters is the result of
a number of factors, the most important of which are:
organoleptic,
microbiological, and
chemical.
1
Department of Analytical Chemistry, Chemical Faculty, Gdansk University of Technology (GUT), Narutowicza Street 11/12, Gdansk 80-233, Poland. Correspondence: Malwina
Diduch, Department of Analytical Chemistry, Chemical Faculty, Gdansk University of Technology (GUT), Narutowicza Street 11/12, Gdansk 80-233, Poland.
Tel.: 48 58 347 10 10. Fax: 48 58 347 26 94.
E-mail: malwina.jakubik@gmail.com
Received 2 March 2012; accepted 15 August 2012; published online 24 October 2012
112
Table 1.
Regulations and standards for water intended for human consumption and bottled water.
Parameter
Organic chemicals
Acrylamide
Benzene
Total pesticides
PAHs
Phenolics
Unit
mg/l
mg/l
mg/l
mg/l
mg/l
EEC (1998)
EEC (2003)
WHO (2008)
EPA (2009)
IBWA (2009)
FDA (2010)
Drinking water
(MAC)
Bottled water
(MAC)
Drinking water
(GV)
Drinking water
(MCL)
Bottled water
(SOQ)
Bottled water
(SOQ)
0.0001
0.001
0.5
0.1
0.0005
0.01
0.005
0.001
0.001
0.005
0.001
0.003
0.01
5
0.7
0.01
0.1
1
0.06
0.01
0.1
1
0.06
0.01
4.0
1
0.06
0.01
0.08
0.01
0.08
Chlorite
mg/l
Haloacetic
mg/l
acids
Total
mg/l
0.1
trihalometanes
Abbreviations: EEC, European Economic Community; EPA, US Environmental Protection Agency; FDA, US Food and Drug Administration; GV, guideline value;
IWBA, International Bottled Water Association; MAC, maximum admissible concentration; MCL, maximum contaminant level; SOQ, standard of quality; WHO,
World Health Organization.
For sources (EEC, EPA, FDA, IWBA, and WHO), see references.
Surfactants
Phthalates
Polychlorinated
biphenyls
Volatile organic
compounds
Alkylphenols
Carbonyl
compounds
Perfluorinated
chemicals
municipal sewage treatment plants), industrial (resource extraction, process efuents, landlls), and agricultural (pesticide and
fertilizer applications) activities.24,3234 The transport and
deposition of such substances are intimately connected with the
hydrological cycle and the geology of the terrain in question. It
depends on the natural geological conditions of how quickly the
layer of groundwater moves and how fast the water pollution
spreads.32 In addition, the various hydrogeochemical processes
(sorption, oxidation and reduction, leaching, weathering,
hydrolysis) and physical parameters (temperature, pressure)
affect the diversity of mineral waters.35 Table 2 presents
information (collected from the literature) on organic contaminants present in bottled water samples and on their likely sources.
Exploitation of Wells
The means used to acquire subterranean waters depends mainly
on whether they are from a water table (where the pressure head
113
Table 2.
Category of
contaminant
Source
Contaminant
Reference
Natural
Degradation
of phyto- and
zooplankton
Suffet
et al.,36
Salemi
et al.37
Anthropogenic
primary
Forming
activities
Gesomin
Methylisoborneol
Isopropyl
methoxypyrazine
Isobutyl
methoxypyrazine
Pesticides:
ethyl dibromide
atrazine
chlordane
DDT and
metabolites
hexachlorobenzene
lindane
MCPA
DBCP
1,3-dichloropropene
aldicarb
aldrin
dieldrin
methoxychlor
permethrin
simazine
1,2-dichloropropane
Chlorine derivatives
of aromatic
hydrocarbons:
chloroform
1,1-dichloroethane
1,2-dichloroethane
1,1,1-trichloroethane
vinyl chloride
1,1-dichloroethene
1,2-dichloroethene
trichloroethene
Aromatic hydrocarbons:
benzene
toluene
ethyl benzene
xylene
1,4-dichlorobenzene
Plasticizers:
phthalate
adipate
Acrylamide
Formaldehyde
Amino acids:
glycine
isoleucine
leucine
Industrial and
technological
activities
Cemeteries
and
graveyards
Wilson
and
Tisdell39
Bottling Process
As bottled water comes from many different sources that are
exploited using a range of technologies, it is processed in a
number of ways in order to maintain its quality, for example, to
remove solid particles, undissociated or undesirable chemical
compounds, and biological material.44
The sum total of processes for obtaining water satisfying a
particular set of criteria is known as water treatment. The choice of
treatment methods depends not only on the initial composition of
the water, but also, above all, on the target quality criteria. These
processes are costly in terms of both investment and operation,
they may generate solid and/or liquid wastes, and they may be
the source of undesirable disinfection by-products; their implementation is a complex, multistage process42 involving:
WHO38
Zychowski
et al.,40
Zychowski41
ltration,
oxidation,
deionization, and
bioelimination.29
114
Table 3.
Levels of organic contaminants in bottled water samples including effect of packing type and storage conditions (literature information).
Parameter
Initial range
Type of water
Origin
Reference
PET bottle
Volatile organic compounds
Ethylbenzene
0.15.17 mg/l
Styrene
0.546.4 mg/l
Toluene
0.11.18 mg/l
Xylene
0.20.77 mg/l
Little or no
difference (o2%)
in the contaminant
levels was
detected as a
function of storage
conditions
Bottled 71
brands, 113
samples
Saudi Arabia,
United Arab
Emirates, Kuwait,
Egypt, Lebanon,
Italy, Turkey,
Spain, Scotland,
Iceland,
Al-Mudhaf
et al.23
Results indicate
that all carbonyl
compounds
migrated to
bottled water
Bottled
(carbonated,
noncarbonated)
Poland
Nawrocki
et al.20
Bottled
(carbonated,
noncarbonated)
20 brands
Japan, Europe,
North America
Mutsuga
et al.80
Bottled
21 brands
China
Li et al.81
Bottled 5
brands
Spain
Casajuana
and
Lacorte4
Bottled 5
brands
Greece
Amiridou
and
Dimitra82
Carbonyl compounds
Acetaldehyde
Acetone
Formaldehyde
0.6317.8 mg/l
5.1125.6 mg/l
0.896.1 mg/l
Acetaldehyde
Formaldehyde
7.827.9 mg/l
37.2107.8 mg/l
b.d.l.
b.d.l.
b.d.l. 0.007 mg/
l
b.d.l. 0.059 mg/
l
b.d.l.
b.d.l.
b.d.l.
b.d.l.
b.d.l. 0.01 mg/l
0.0030.011 mg/l
0.0200.070 mg/l
0.0820.355 mg/l
0.0390.188 mg/l
0.0020.003 mg/l
0.0300.031 mg/l
BPA
DBP
DEP
DEHP
4-NP
0.0046 mg/la
0.0044 mg/la
0.0033 mg/la
0.35 mg/la
0.0079 mg/la
BEP
DBP
DMP
0.429.87 mg/l
0.453.48 mg/l
0.010.05 mg/l
Bottled 5
samples
Italy
Signorile
et al.83
BBP
DBP
DEP
DEHP
DMP
DOP
0.002 mg/l
0.2 mg/l
0.04 mg/l
2.88 mg/l
0.10 mg/l
b.d.l.
Bottled 1
brand
Czech Republic
Prokupkova
et al.84
DEHA
DEHP
0.0120.046 mg/l
0.0240.071 mg/l
Exposed to temperatures
34 1C and 60 1C, during 17
and 48 h, respectively
Pure
(distilled)
water was
filled into
PET bottles
of different
origin
Honduras, Nepal,
Switzerland
Schmid
et al.11
BPA
0.200.30 mg/l
China
Wu et al.85
NP
OP
b.d.l.
b.d.l.
b.d.l.
b.d.l.
Bottled 6
samples
Bottled 6
samples
Mexico
LoyoRosales
et al.86
21.538.0 mg/l
Bottled 15
brand, 19
samples
Argentina
Tombesi
and Freije87
Antioxidant
BHT
Difference not
statistically
significant
(Po0.05)
115
Table 3. (Continued ).
Parameter
Initial range
Type of water
Origin
Reference
Bottled 1
brand
Spain
Casajuana
and
Lacorte4
Bottled 1
brand
Czech Republic
Prokupkova
et al.84
Bottled 3
brands
Spain
Casajuana
and
Lacorte4
Bottled 12
brands
Mexico
LoyoRosales
et al.86
Bottled 6
brands
Mexico
LoyoRosales
et al.86
Glass bottle
Alkylphenols and phthalates
BADGE
b.d.l.
BBP
b.d.l.
BPA
b.d.l.
DBP
b.d.l.
DEP
b.d.l.
DEHP
DMP
b.d.l.
4-NP
0.078 mg/l
BBP
DBP
DEP
DEHP
DMP
DOP
b.d.l.
0.18 mg/l
b.d.l.
9.78 mg/l
b.d.l.
b.d.l.
b.d.l.
b.d.l.
b.d.l.
b.d.l.
0.089 mg/l
0.001 mg/l
1.73 mg/l
PE bottle
Alkylphenols and phthalates
BADGE
b.d.l.
BBP
b.d.l.
BPA
b.d.l. 0.002 mg/
DBP
l
DEP
b.d.l.
DEHP
0.0810.139 mg/l
DMP
4-NP
b.d.l.
b.d.l.
b.d.l.
b.d.l.
0.0030.006 mg/l
0.0250.072 mg/l
0.1320.990 mg/l
0.1030.332 mg/l
0.0010.005 [mg/l
b.d.l.
PVC bottle
Alkylphenols and
phthalates
NP
OP
300 ng/l
b.d.l.
The levels of NP
increased during
the first hours, and
tended to stabilize
after 120 h at
B140 ng/l
HDPE bottle
Alkylphenols and
phthalates
NP
OP
180 ng/la,
12a
The levels of NP
increased during
the first hours, and
tended to stabilize
after 120 h at
B230 ng/l
116
Table 4.
Parameter
Range
Water type
Origin
Reference
Bottled 71 brands,
113 samples
Saudi Arabia,
United Arab
Emirates, Kuwait,
Egypt, Lebanon,
Italy, Turkey, Spain,
Scotland, Iceland,
Al-Mudhaf et al.23
Pesticides
a-HCH
b-HCH
b-HCH
d-HCH
Aldrin
DDD
DDE
DDT
Dieldrin
Endosulfan I
Endosulfan II
Endosulfan sulfate
Endrin
Endrin aldehyde
0.0450.098 mg/l
0.0480.152 mg/l
0.0190.033 mg/l
0.0120.046 mg/l
0.0120.027 mg/l
0.0030.009 mg/l
0.0290.060 mg/l
00030.009 mg/l
ND
ND0.005 mg/l
ND
ND0.033 mg/l
ND0.008 mg/l
0.0010.007 mg/l
Bottled 36 samples
Mexico
Diaz et al.25
Perfluorinated chemicals
PFBuS
PFDA
PFDoDA
PFDS
PFHpA
PFHxA
PFHxS
PFNA
PFOA
PFOS
PFOSA
PFTDA
PFUnDA
THPFOS
o0.27 ng/l
0.630.82 ng/l
o0.34 ng/l
o0.1 ng/l
0.40.61 ng/l
0.870.102 ng/l
o0.18 ng/l
0.130.42 [ng/l]
0.160.67 ng/l
o0.24 ng/l
0.19 ng/l
o0.90 ng/l
o0.43 ng/l
o0.1 ng/l
Bottled 4 samples
Spain
Ericson et al.18
Polychlorinated biphenyls
SPCB
0.0350.067 mg/l
Bottled 6 brands, 96
samples
Mexico
Salinas et al.24
Bottled (purified,
mineral, natural spring,
distilled) 10 brands
China
Bottled 13 brands
Greece
Leivadara et al.7
Bottled (mineral) 14
brands
Saudi Arabia
Bottled
Al-Mudhaf et al.23
Bottled 13 brands
Saudi Arabia,
United Arab
Emirates, Kuwait,
Egypt, Lebanon,
Italy, Turkey, Spain,
Scotland, Iceland
Greece
Leivadara et al.7
Bottled 5 brands
Egypt
Saleh et al.88
b.d.l.
b.d.l.0.1 mg/l
b.d.l.0.6 mg/l
21.365.1 mg/l
b.d.l.
2171.8 mg/l
b.d.l.
b.d.l.2.2 mg/l
b.d.l.
2.75.2 mg/l
b.d.l.
b.d.l.
1.01.5 mg/l
Trihalogenomethanes
Bromodichloromethane
Bromoform
Chloroform
Dibromochloromethane
Bromodichloromethane
Bromoform
Chloroform
Dibromochloromethane
b.d.l.1.07 mg/l
b.d.l.18.07 mg/l
b.d.l.0.29 mg/l
b.d.l.1.83 mg/l
0.100.58 mg/l
0.1137.55 mg/l
0.11.85 mg/l
0.11.76 mg/l
Bromodichloromethane
Bromoform
Chloroform
Dibromochloromethane
1.72.6 mg/l
117
Table 4. (Continued ).
Parameter
Bromodichloromethane
Chloroform
Dibromochloromethane
Bromodichloromethane
Bromoform
Chloroform
Dibromochloromethane
Bromodichloromethane
Bromoform
Chloroform
Chloromethane
Dibromochloromethane
Bromodichloromethane
Bromoform
Chloroform
Dibromochloromethane
Range
6973 mg/l
7986 mg/l
60 mg/l
0.011.0 mg/l
0.013.0 mg/l
0.01 0.9 mg/l
0.010.6 mg/l
0.0112.4 mg/l
0.013.3 mg/l
0.0221.3 mg/l
0.091.14 mg/l
0.0410.6 mg/l
b.d.l.
b.d.l.
b.d.l.
b.d.l.
Water type
Origin
Reference
Bottled 45 samples
Spain
Font-Ribera et al.19
Bottled (spring,
purified, distilled) 17
brands, 95 samples
USA
Ikem29
Bottled 13 brands
Greece
Leivadara et al.7
disorders throughout life, including sexual precocity, hormonerelated cancers (e.g., testicular and breast cancer), reproductive
tract abnormalities, and infertility. Other impacts of EDs may
include effects on thyroid function, obesity, and metabolism.66
According to a report by experts from the International Life
Science Institute (ILSI),52 PET is a biologically neutral material with
regard to consumption and skin contact. Tests carried out to
measure its potential toxicity and gene toxicity also yielded
negative results.53 Only the results of studies into the possible
migration of antimony trioxide (Sb2O3) is a cause of concern.52
Antimony trioxide is the usual catalyst in the polycondensation
reaction producing PET.66,67 Estimates show that it is used in
B90% of plants producing synthetic packaging materials.
Consequently, the most commercially available PET packaging
contains 190300 mg Sb/kg.68,69 In comparison, the average level
of antimony in the Earths crust is 0.5 mg/kg, and in pristine
subterranean waters it is 2 ng/l.70
Research examining the possibility of antimony being leached
from packaging material is being carried out independently in
many centers around the world: Greece,68 Germany, Canada,70,71
Turkey,72 Hungary,73 Cyprus,74 United States,75 and Japan.76 One
may infer from these results that the concentration of antimony in
water stored in PET bottles is up to 30 times greater than that in
water stored in glass or polypropylene bottles.71
The effectiveness of antimony leaching depends on many
factors, but the major one is temperature.77 This process takes
place faster even when the temperature has been raised to only
B5060 1C.73,75 The surface area to volume ratio of the bottle is
also important: waters in bottles of smaller volume (0.250.5 l)
have a higher level of antimony than those in 2.5 l and larger
containers.73,75 In the case of waters of the same brand, higher Sb
levels were found in carbonated than in still waters.73,74 The color
of the bottle is also important:75 in the case of hard PET, the
highest Sb levels were found in colorless, pale blue, and pale
green bottles.56
Even though the antimony concentrations in most types of
bottled water do not exceed permitted levels of this element
(drinking waters: WHO (20 mg/l), EPA (6 mg/l), ECC (5 mg/l); bottled
waters: IBWA and FDA (6 mg/l)), they can nonetheless have a
negative effect on human health, given the elements carcinogenicity and the fact that up to 40% of the adult daily requirement
for Sb may be supplied by drinking water.73
In the bottling industry, PET bottles are predominant, but there
are worldwide brands such as Perrier and S. Pellegrino that
continue to use glass bottles. Because such bottles can be
recycled and reused, they are regarded as environmentally
friendly. Moreover, todays glass bottles are 20% lighter than
& 2013 Nature America, Inc.
those produced two decades ago.78 Even so, they are still much
more expensive to transport than PET bottles.
Research into the possible migration of elements from glass
packaging has tended to focus on determining levels of lead
(Pb).79 However, it turns out that the list of elements leached from
glass bottles is much longer than from PET:56 there is 19 times
more Ce in water from glass bottles than from PET bottles, 14
times more Pb, 7 times more Al, and from 7 to 2.4 times more Zr,
Ti, Hf, Th, La, Pr, Fe, Zn, Nd, Sn, and Cr.
The results of all these tests revealed big differences in leaching
effectiveness between various types of bottle, regardless of the
material from which they were made. In many cases the intensity
of the process is a serious problem. The reasons for the variable
reactivity of bottles are neither fully understood nor unequivocal.
According to Pinto and Reali,63 not all PET materials are of the
same chemical quality. Quality may vary depending on the raw
material as well as the technology used in bottle production that
could drag technological contaminants. To a large extent, this may
be because of the age of the bottles (this applies mainly to
returnable bottles) and the extent to which they were made from
recycled materials.10,56
There is a need for more information on the identity/quantity of
chemicals leaching into food, human exposure, and long-term
impact on health, and especially the ED source, long-term
exposure, and mixture effects remain to be investigated. Table 3
lists information on the inuence of the type of bottle and the
storage conditions on the content of selected organic chemical
contaminants.
LEVELS OF ORGANIC CONTAMINANTS DETERMINED IN
SAMPLES OF BOTTLED WATER
The quality of water sold in bottles is the result of many factors,
from its pristine quality, through the methods of its acquisition
and treatment, to the conditions under which it is stored and
transported.
Indirectly, the composition of the nal product may be affected
by the legislation binding in its country of origin, because water
must meet requirements specied in them. Table 4 sets out
literature information on levels of organic contaminants determined
in samples of different kinds of bottled water. The differences in
levels, in the case of primary contaminants, are mainly due to the
location of wells, their type and distance from farming, and/or
industrial areas. As far as secondary contaminants are concerned,
the means of treating the water are of greatest importance.
Although in most cases the determined levels of organic
contaminants are below permitted levels and such water, if
118
consumed in moderate quantities, will not seriously affect human
health, these contaminants do signicantly impair its organoleptic
properties.4
SUMMARY
The inference to be drawn from the analyses of bottled water
samples is that their contamination by organic compounds is
increasing. The continually rising popularity of bottled waters and
the conventional wisdom that they are of the highest quality
merely serve to underscore the need to carry out further and more
detailed studies in this respect. This is a complex problem, because
the quality of bottled waters is the resultant of numerous factors,
starting with its initial composition, through a bottling process, to
the conditions in which the nal product is stored and transported.
The results of studies on bottled water quality enable a better
understanding of the phenomena impairing the quality of bottled
water and are a valuable source of information for consumers. They
will also provide a solid foundation upon which revisions of
regulations governing bottled water quality can be based.
CONFLICT OF INTEREST
The authors declare no conict of interest.
ACKNOWLEDGEMENTS
This work was supported by a scholarship for PhD students MISTRZ programme,
Warsaw, 2009.
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