Environ Monit Assess (2017) 189:631
https://doi.org/10.1007/s10661-017-6342-3
Impact of temperature and storage time on the migration
of antimony from polyethylene terephthalate (PET) containers
into bottled water in Qatar
Fatima Al-Otoum & Mohammad A. Al-Ghouti &
Ozeas S. Costa Jr & Majeda Khraisheh
Received: 9 April 2017 / Accepted: 31 October 2017
# Springer International Publishing AG, part of Springer Nature 2017
Abstract Prosperity in Qatar and the consequent stress-
es on water resources resulted in a sustainable increase
in the bottled drinking water market. Reports on health
concerns and possible migration of chemicals from the
plastic material into the water have driven the current
investigation. This study aims to address the extent of
antimony (Sb) leaching from polyethylene terephthalate
(PET) water bottles subject to temperature variations
(24–50 °C) due to Qatar’s hot climate and improper
storage conditions. A representative basket including
66 different imported and locally produced water bottles
was considered. The concentrations of Sb in bottled
water ranged from 0.168 to 2.263 μg/L at 24 °C and
from 0.240 to 6.110 μg/L at 50 °C. Antimony concen-
trations in PET bottles at 24 °C was significantly lower
than those at 50 °C (p = 0.0142), indicating that the
F. Al-Otoum
Ministry of Public Health, Public Health Department, P.O. Box:
42, Doha, Qatar
e-mail: falotoum@moph.gov.qa
M. A. Al-Ghouti (*)
Department of Biological and Environmental Sciences, College of
Arts and Sciences, Qatar University, P.O. Box: 2713, Doha, Qatar
e-mail: mohammad.alghouti@qu.edu.qa
O. S. Costa Jr,
School of Earth Sciences, The Ohio State University at Mansfield,
395 Ovalwood Hall, 1760 University Drive, Mansfield, OH
44906, USA
M. Khraisheh
Chemical Engineering Department, College of Engineering, Qatar
University, P.O. Box: 2713, Doha, Qatar
temperature was a principal factor affecting the release
of Sb from the plastic into the water. Although the
detected Sb amounts were below the guidelines en-
dorsed by WHO and Qatar (standard 5 μg/L) at 24 °C,
the concentration measured at 50 °C was higher than the
recommended WHO values (6.11 μg/L).
Keywords Antimony . Drinking water quality . Plastic
bottles storage . Leaching . Hot climates . Health effects
Introduction
Qatar is an arid country with very limited fresh water
recourses. The country depends heavily on desalination
for its main drinking water supply. Qatar’s prosperity,
due to the huge investment in the oil and gas sector, and
the population boom resulted in stresses being exerted
on the local water supplies. Lifestyle attitudes in Qatar
are associated with the huge sustained rise in the use of
bottled water for drinking and cooking purposes
mirroring reported trends in other countries (Andra
et al. 2012; Carneado et al. 2015; Chapa-Martínez
et al. 2016; Fan et al. 2014; Reimann et al. 2010,
2012; Rowell et al. 2016). In Qatar, nine local compa-
nies produce bottled water. Three companies produce
different size containers including 1.5 L and 330 mL
capacity. The remaining manufacturers produce larger
12-L water bottles. In addition to the locally produced
bottled water, Qatar imports different brands from sev-
eral countries to satisfy the diversity in market demand.
Various materials are typically used for the
631 Page 2 of 12
manufacturing of the plastic bottles but the most used in
Qatar are polyethylene terephthalate (PET).
The use of PET bottles increased tremendously in
recent years given its durability, chemical and physical
stability, and favorable economic costs. Its use is mainly
for food and beverage packaging (Carneado et al. 2015;
Sánchez-Martínez et al. 2013). In addition, PET is known
to have fewer chemical additives during its manufactur-
ing. One such additive is antimony trioxide (Sb2O3). This
widely used chemical, in PET manufacturing, acts mainly
as a catalyst during the solid phase polycondensation
reaction of PET. It is mainly used due to its elevated
catalytic activity, limited side reactions in addition to
negative impact on undesirable color addition to the final
product (Carneado et al. 2015; Westerhoff et al. 2008).
Cheng et al. (2010) reported that recycling plastic bottles
contain between 100 and 300 mg/kg of antimony triox-
ide. PET bottles made using antimony (Sb) typically
contain between 190 and 300 μg Sb/g (de Jesus et al.
2016), with the highest value recorded at 353 μg Sb/g
(Bach et al. 2012). With such high concentration of
antimony in bottled water, research in recent years fo-
cused on issues related to its leaching into the water and
possible health effects (Bach et al. 2012; Duh 2002).
Short-term exposures to levels higher than 6 μg/L can
cause side effects such as nausea, vomiting, and diarrhea
(Aghaee et al. 2014). Higher blood cholesterol and lower
blood sugar are other side effects for long-term exposure
(Westerhoff et al. 2008). Recent studies reported that
there seems to be evidence of carcinogenicity of Sb2O3
when tested on experimental animals (Smichowski
2008). Moreover, it has been estimated that around 38%
(nearly 7.4 μg Sb/day) of the Sb daily intake in adults
results from drinking water (Chapa-Martínez et al. 2016;
Fan et al. 2014). The USEPA (USEPA 1999) and the
Council of the European Communities (98/83/EC 1998)
categorized Sb and its associated known compounds as a
priority pollutant with different maximum permitted
levels reported. For example, Japan offers the most strin-
gent Sb levels allowed in drinking water at 2 μg Sb/L
while a value of 5 and 6 μg Sb/L are acceptable in the EU
and North America, respectively (Andra et al. 2012; Ikem
et al. 2002).
In recent years, a number of studies investigated the
leaching of Sb from PET into the bottled water. Studies
included various countries such as USA, Africa, Turkey,
and some EU countries (Brenčič et al. 2010; Frengstad
et al. 2010; Greifenstein et al. 2013; Güler 2007;
Sánchez-Martínez et al. 2013).
Environ Monit Assess (2017) 189:631
An early study by Shotyk and Krachler (2007) re-
ported evidence of Sb migration from PET bottles into
drinking water stored at high temperatures and under
sunlight. The authors reported that the concentration of
Sb was found to be between 0.156 and 0.343 μg/L; a
substantial increase compared to levels found in tap
drinking water in the country of study. Various factors
are thought to affect the release of Sb from PET bottles
including temperature, pH, and exposure to sunlight
(Chapa-Martínez et al. 2016; Rowell et al. 2016). Re-
ports by Westerhoff et al. (2008) indicated that the pH
had limited significance on the migration of Sb under
normal drinking water pH from 6 to 8 (Chapa-Martínez
et al. 2016). pH impact was more dominant in carbon-
ated water bottles due to the lower pH associated with
sparkling carbonated water (Bach et al. 2012).
Westerhoff et al., (2008) employed a power function to
investigate the effect of temperature and its time-
dependent relationship on the migration of Sb from the
containers to the water. It was reported that the rate of
release of Sb in water was much higher at temperature
exceeding 60 °C. The authors considered nine different
brands of bottled drinking water in the USA and found
that levels of Sb in the water ranged between 0.095 and
0.521 μg/L. In addition, a comprehensive study by
Reimann et al., (Reimann et al. 2010, Reimann et al.
2012) considered the migration of 75 different
chemicals into drinking water contained in glass and
plastic bottles. It was mainly found that various contam-
inants leached from both containers to the water. Con-
trary to expectation, a number of trace chemicals were
reported in drinking water contained in glass bottles.
Keresztes et al., (2009) considered the effect of CO2 in
water and studied a number of carbonated and
noncarbonated brands sold in the Hungarian market.
The results indicated that carbonated water (due to the
lower pH) contained higher levels of Sb compared to
noncarbonated pH neutral waters. Some studies have
looked into the effect of storage on the quality of bottled
water. The first of such studies evaluated microbiologi-
cal changes occurring during different storage condi-
tions in the UK (Armas and Sutherland 1999). The
bacteriological impact of duration and location of bot-
tled water storage was also investigated in the USA
(Duranceau et al. 2012). They concluded that greater
contamination was observed in variable-temperature
storage conditions, as compared to constant-
temperature environments. Aghaee et al., (2014) exam-
ined the effects of storage time and temperature on the
Environ Monit Assess (2017) 189:631
release of antimony and other trace metals from PET
bottles. According to this study, storage duration had a
significant positive effect (p ≤ 0.05) on Sb and Al
concentrations, while a negative effect was observed in
Fe concentrations. In a recent comprehensive study,
Guart et al. (2014) found that the number of organic
compounds detected in water stored in PET bottles for a
year (97 compounds) was more than twice that of fresh
samples (43 compounds detected). The concentrations
of the detected compounds were also higher after 1 year
of storage.
The effect of the color of the container was evaluated
by Reimann et al. (2010) and Marcinkowska et al.
(2017). These authors found that the color of the con-
tainer has a significant effect for a number of elements:
Cr, Th, La, Zr, Nd, Ce, Pr, Nb, Ti, Fe, Co, and Er.
Given Qatar’s hot climate in addition to issues related
to storage of the water bottles in closed rooms with no
air-conditioning and possible exposure to sunlight, this
study aims to investigate the impact of such factors on
the migration of Sb into drinking water from PET bot-
tles. Both locally produced and imported bottled waters
were considered. More specifically, the study aims to
investigate the effect of high temperature on the
leaching of Sb into the water as well as the relationship
between Sb concentrations and storage time. Inductively
coupled plasma-mass spectrometry (ICP-MS) was uti-
lized to estimate the concentration of Sb in bottled water.
The outcomes of this study will be shared with the
concerned parties (monitoring authorities and water pro-
ducing companies) to develop guidelines addressing the
ideal storage conditions for bottled water and to review
the PET specification for each brand.
Materials and methods
Commercial bottled waters
A representative random basket of 22 bottled water
brands were purchased from various shops in different
cities in Qatar representing locally manufactured and
filled bottles in addition to imported brands covering
> 85% of the available brands in Qatar. All water bottles
contained noncarbonated water. The date of production
varied from one brand to another and the variations were
recorded. The bottled water brands and the region of
production are given in (Table 1). The indoor tempera-
ture was measured for each shop using a digital
Page 3 of 12 631
thermometer and was found around 24 °C. Three bottles
were used from each batch. The bottles sampled had
volumes that ranged from 330 to 550 mL. For the 500
and 550 mL, the Sb content was recalculated into
330 mL to unify the volume for the entire study. The
global identification resin number was checked for each
bottle and confirmed that PET was the type of plastic
used in all studied water bottles. The color of plastic was
clear in all bottles apart from three that had a faint blue
tint.
Storage conditions
To investigate the effect of storage conditions, five local
water bottling companies around Doha were visited.
Some of the companies provided air-conditioned stor-
age areas, while others provided shaded stores only.
During the field visits, temperatures were measured
and found to range from 30 to 45.5 °C under the shade.
The measuring process was repeated twice to cover the
temperature variation during 4 weeks of May. The time
of measuring the temperature began at 12:00 PM and
extended for 3 h. The bottles were stored, upon pur-
chase, in the laboratory at room temperature (22.2 °C)
for further use. Sample handling was done carefully to
minimize any external contamination.
Migration of Sb into water contained in PET bottles
Analyses of the total concentration of Sb were conduct-
ed in one batch with ICP-MS. All reagents used in the
experimental work were of analytical grade. In addition,
solutions prepared used ultra-clean water. Glassware
was cleaned by soaking it in nitric acid (10% v/v) before
rinsing with ultra-pure water. Standard stock solution of
Sb(III) was prepared using procedure as described in
Chapa-Martínez et al. (2016). Required dilutions were
prepared from the stock solutions immediately before
use.
The concentration of Sb in the samples was carried
out in triplicate for each brand. Argon gas utilized was
of special purity (> 99.9%). To set the system, calibra-
tion curves were constructed by analyzing NIST single-
elements. The ultra-clean water used in the experimental
work had a resistivity of 18 ΩMS cm at ambient
temperature.
To study the effect of temperature, bottled water
samples were placed into incubators set at 50 °C for
10 days and analyzed for Sb concentration using the
631 Page 4 of 12 Environ Monit Assess (2017) 189:631

Table 1 Sb concentration in samples of bottled water available in Qatar and stored at two different temperatures (n = 3 for each experiment).
Standard deviations are indicated for each calculated average

Brand # Country/region Sb at 24 °C (μg/L) Sb at 50 °C (μg/L) #days of manufacturing

PET1 Middle East 1 0.22 ± 0.011 0.27 ± 0.013 62

PET2 Qatar 0.22 ± 0.017 0.24 ± 0.019 19
PET3 GCC1 0.25 ± 0.009 0.33 ± 0.043 46
PET4 GCC1 0.25 ± 0.005 0.29 ± 0.042 160
PET5 GCC1 0.28 ± 0.009 0.30 ± 0.012 44
PET6 GCC1 0.31 ± 0.010 0.51 ± 0.104 70
PET7 GCC1 0.33 ± 0.047 0.45 ± 0.025 103
PET8 GCC2 0.33 ± 0.006 0.45 ± 0.044 226
PET9 Qatar 0.34 ± 0.051 0.40 ± 0.051 28
PET10 Qatar 0.38 ± 0.028 1.21 ± 0.237 18
PET11 Qatar 0.43 ± 0.028 0.69 ± 0.287 18
PET12 MiddleEast2 0.47 ± 0.100 0.60 ± 0.034 115
PET13 GCC1 0.51 ± 0.069 0.78 ± 0.038 53
PET14 Middle East 1 0.85 ± 0.056 2.56 ± 0.495 107
PET15 GCC3 1.56 ± 0.066 4.81 ± 0.293 170
PET16 Middle East1 1.57 ± 0.103 4.06 ± 0.264 94
PET17 Asia1 1.91 ± 0.058 4.62 ± 0.355 111
PET18 EU1 1.98 ± 0.010 5.10 ± 0.214 201
PET19 EU2 2.19 ± 0.074 6.11 ± 0.584 155
PET20 EU2 2.26 ± 0.139 5.59 ± 0.986 188
PET21 EU3 2.27 ± 0.081 5.93 ± 0.572 212
PET22 Qatar 2.28 ± 0.065 4.46 ± 0.443 29

ICP-MS. Three replicates from each brand were ana-
lyzed at 24 and 50 °C, respectively. Both nitric acid and
deionized water were used for sample extraction.
Statistical analysis
Due to the fact that the experimental designs of the this
study were a completely randomized design (CRD) and
the experiments were factorial, analysis of variance
(ANOVA) for two factors was used for the assessment of
the temperature experiment (changes between 24 and 50°).
Results and discussion
Initial total soluble Sb concentration in bottled water
The initial Sb concentration in water bottled in 22
different PET brands of water bottles commercially
available and purchased in two main cities in Qatar
was analyzed on day 0 (day of purchase). Recorded
results are detailed in Table 1. The Sb concentrations
were found to range between 0.21 and 2.39 μg/L.
The average concentration at 24 °C was
0.963 ± 0.818 μg/L. In general, all samples tested
showed an initial Sb content well below the recom-
mended level set by the EU (5 μg/L) and USA
(6 μg/L). However, four of the tested brands had
Sb concentrations above the most restrictive Japa-
nese limit of 2 μg/L. The observed concentrations
were in-line with values reported for 12 brands
studied in Mexico (ranging between 0.28 and
2.30 μg/L), 23 brands in the Serbian market (0.3–
1.81 μg/L), and 132 brands from 28 countries
(Chapa-Martínez et al. 2016), but higher than those
reported by Reimann et al. (2010) in Europe (Sb
concentration < 0.45 μg/L), Fan et al. (2014) in
China (Sb concentration < 0.02 μg/L at 25 °C),
Environ Monit Assess (2017) 189:631
and Westerhoff et al. (2008) in the USA (Sb con-
centration < 0.52 μg/L at 22 °C).
With the exception of Qatari brand #22 (average Sb
concentration of 2.28 μg/L at 24 °C), all water bottles
manufactured in Qatar showed low levels of initial Sb
concentrations, ranging from 0.22 to 0.43 μg/L (Fig. 1).
Of the remaining brands evaluated in this study, ten had
initial Sb concentrations below 1.0 μg/L—with values
ranging from 0.21 to 0.89 μg/L—and seven had initial
concentrations ranging from 1.47 to 2.39 μg/L.
The wide range of Sb concentrations has been ob-
served before (Fan et al. 2014) and is likely a result of
the variable quality and manufacturing processes of PET
plastics in different countries, as well as the high-
temperature storage conditions during transportation.
As such, our results suggest that locally sourced bottled
water have, in general, lower Sb concentrations than
those imported from countries outside the Gulf Cooper-
ation Council (GCC). The GCC group included brands
from Qatar, UAE, Kuwait, and Saudi Arabia. The Non-
GCC group included brands from Turkey, Lebanon,
Fiji, UK, France, and Italy.
Similar wide ranges have also been reported in
Shotyk and Krachler (2007) and Reimann et al.,
(Reimann et al. 2010, Reimann et al. 2012), where Sb
concentrations at ambient temperature ranged from
Fig. 1 Antimony (Sb) concentrations at 24 °C in PET water bottles produced in Qatar (n = 3)
Page 5 of 12 631
0.156 to 0.343 μg/L and from 0.095 to 0.521 μg/L,
respectively.
Bottles produced and filled in the GCC have initial
Sb concentrations of 0.25–1.56 μg Sb/L, which is, on
average, an order of magnitude higher that those
manufactured in Qatar. Marked variation also exists in
the values obtained for the two Middle Eastern coun-
tries, with values ranging from 0.22 to 1.57 μg Sb/L. In
particular, all European brands tested recorded values
close to or above 2 μg Sb/L. Although still below the
international standard of 5 μg/L, these values recorded
are higher than those of the brands manufactured in
Qatar, GCC countries, and Middle East countries.
Given that the exact blend of the PET bottles and the
exact factory associated with their manufacturing is
unknown, it is difficult to make conclusive comments
on the reasons behind the wide range of values ob-
served. As suggested above, both the quality of the
PET material and/or the storage conditions during trans-
portation could be responsible for the high Sb concen-
trations of imported water.
Sb release as a function of temperature
Temperature has been shown to significantly influence
Sb leaching from PET bottles (Chapa-Martínez et al.
631 Page 6 of 12
2016; Westerhoff et al. 2008). We evaluated the effect of
temperature on the leaching of Sb into the drinking
water in PET bottles for two main temperatures (24
and 50 °C). Although the summer average temperatures
in Qatar can reach up to 45 °C, higher temperatures such
as 50 °C are reasonable inside cars and in closed storage
without air-conditioning. Temperatures as high as 70 °C
were deemed reasonable by Chapa-Martínez et al.
(2016) who reported that this elevated temperature
mimics condition inside cars during summer time in
Mexico for example.
Sb concentrations at 24 °C ranged from 0.21 to
2.39 μg/L, while at 50 °C they ranged from 0.22 to
6.37 μg/L (Fig. 2). There is a significant difference
(p = 0.0142) between Sb concentrations at 24 and at
50 °C. With one exception, all samples with initial Sb
concentrations (at 24 °C) below 0.5 μg/L experienced
the smallest increases at 50 °C (between 8 and 62%),
while samples with initial Sb concentrations above
1.0 μg/L experienced increases varying between 139
and 210% on Sb concentrations at 50 °C.
It is noteworthy that a marked increase in Sb concen-
tration occurred mainly in the bottles manufactured
outside GCC countries. This may be explained by the
type or quality of PET used in the manufacturing of the
Fig. 2 Sb concentration of all 22 brands at both temperatures. The blue line represents the concentration of Sb at 24 °C and the red line
shows the Sb concentration at 50 °C
Environ Monit Assess (2017) 189:631
water bottles. It is also possible that the EU bottles are
mainly manufactured for consumptions in countries
where the temperatures are not as elevated as those
experienced in Qatar and in other GCC countries. Near-
ly 23% of the water samples at 50 °C showed Sb
concentrations > 5 μg/L, which exceeds the recom-
mended international standards and the guidelines set
by the Ministry of Environment of Qatar for Sb in
drinking water (5 μg/L).
Further exploration of the differences in Sb concen-
trations at different temperatures in water bottled from
GCC and non-GCC countries revealed striking differ-
ences between these two groups (Fig. 3). ANOVA anal-
ysis also indicates a statistically significant difference
between these groups at 50 °C (p = 0.046) but not at
24 °C (p = 0.134).
The results indicated that the migration of antimony
PET bottles generally increased under higher tempera-
ture (50 °C) reaching a value of Sb of around 6.11 μg/L
in EU brand #19, while the smallest increase (around
0.02 μg/L) was observed in two of the Qatari-
manufactured brands. These results can be attributed
to specific storage conditions during the exporting
from the origin countries. Storage conditions includ-
ing temperature are not typically reflected in the
Environ Monit Assess (2017) 189:631
Fig. 3 Antimony (Sb) concen-
trations at 24 and 50 °C in bottled
water from GCC and non-GCC
countries. Asterisks (*) indicate
outliers
labels of the bottled water. A study conducted by
Takahashi et al. (2008) indicated that the source of
the leached Sb into the water kept in PET plastic
bottles may be primarily from the degradation of
the plastic under high temperature and may not be
linked to Sb chemical components used in the
manufacturing of the PET bottles.
These results are in agreement with those reported by
Carrieri et al. (2012) which indicated a significant
leaching effect at temperatures > 45–60 °C. In addition,
the authors indicated that the antimony was the only
element that showed opposite behavior for glass and
PET. The water in PET bottles shows a higher Sb
concentration after 7 days of storage time at 2 °C. At
80 °C, the authors reported that a maximum value
18 μg/L was obtained. Westerhoff et al. (2008) reported
that in extreme conditions where bottles are exposed to
80 °C for 48 h period, a large increase in Sb concentra-
tion was detected raising from 0.2 μg/L to around
9.7 μg/L.
The effect of temperature was reported in a recent
study by Chapa-Martínez et al. (2016). An extensive
study on the impact of various experimental conditions
highlighted that temperature is the most significant fac-
tor related to the leaching of Sb into the water based on
statistical analysis. In their study, a temperature of 75 °C
showed considerably more Sb release than those stored
at room temperature. In addition, the results obtained in
Page 7 of 12 631
our study are also consistent with results reported by Fan
et al. (2014). In their study, water bottles exposed to
temperature change between 4 and 70 °C for a week. A
reported 4.4–319 times more Sb was reported under
those conditions (Fan et al. 2014).
The highly significant difference between Sb concen-
trations in bottled water from GCC and non-GCC coun-
tries described previously could be an artifact of the
longer storage time (differences in the bottling time from
production to analysis) as indicated in Fig. 4. The longer
the storage time, the more contact between the water and
the PET material.
In addition, the observed variation of Sb concentra-
tion from different countries of production could be
attributed to the variable qualities of the raw material
and method used in the manufacturing of the PET
plastic (Sax 2010).
Effect of storage time
Figure 5 shows the storage time (number of days from
production to the conclusion of the experiment) of all 22
brands evaluated in this study. As mentioned previously,
for most of the brands evaluated, there is a significant,
positive correlation between Sb concentration and stor-
age time (Fig. 4). Two of the brands evaluated had been
stored for a long time (150 and 216 days) prior to the
beginning of the analysis, but no significant effect of
631 Page 8 of 12 Environ Monit Assess (2017) 189:631

Fig. 4 The effect of storage time (days from production to analysis) on the Sb concentration (in μg/L) of different brands of bottled water
available in the Qatari market at 24 °C (R2 = 0.24 with outliers; R2 = 0.74 without outliers)

storage was observed: their Sb concentrations were 0.26
and 0.33 μg/L respectively (at 24 °C) and only increased
to 0.39 and 0.45 μg/L, respectively (at 50 °C). Another
brand had only been stored for 19 days at the beginning
of the analysis, but had initial Sb concentrations of
2.28 μg/L (at 24 °C) and 5.46 μg/L (at 50 °C). For most
of the remaining brands, those with the highest storage
time experienced the highest increases in Sb concentra-
tion once exposed to temperatures of 50 °C for 10 days
(Fig. 6).

Fig. 5 Brands of water bottle by country and their respective storage time (in days) before the conclusion of all analysis
Environ Monit Assess (2017) 189:631 Page 9 of 12 631

Fig. 6 Correlation between storage time and Sb concentration increase from 24 to 50 °C for all the 22 brands evaluated in this study

Statistically, the effect of long storage time on Sb
leaching was significant for samples at 24 °C
(p = 0.021) and at 50 °C (p = 0.015). Over 24% of the
increase in Sb concentrations between 24 and 50 °C was
due to the effect of storage (Fig. 6). This correlation is
even stronger without the three outliers mentioned
above (R2 = 0.685). A similar effect of storage time
has been reported in the literature (Aghaee et al. 2014;
Fan et al. 2014; Carneado et al. 2015; Chapa-Martínez
et al. 2016). However, Holland and Hay (2002) reported
that at temperature above 75 °C and in longer storage
conditions, a negative effect on the amounts of Sb was
observed. This was mainly attributed to the possibility
of having special functional groups resulting from the
631 Page 10 of 12 Environ Monit Assess (2017) 189:631

Table 2 Chronic daily intake values for adults and children ingesting water stored on PET bottles

Brand Country/ CDI-1 (ng/kg/ CDI-2 (ng/kg/ CDI-3 (ng/kg/ CDI-4 (ng/kg/ CDI-5 (ng/kg/ CDI-6 (ng/kg/
# region day) day) day) day) day) day)

PET1 Middle East 1 17.96 22.04 31.43 20.95 38.57 25.71

PET2 Qatar 17.96 19.59 31.43 20.95 34.29 22.86
PET3 GCC1 20.41 26.94 35.71 23.81 47.14 31.43
PET4 GCC1 20.41 23.67 35.71 23.81 41.43 27.62
PET5 GCC1 22.86 24.49 40.00 26.67 42.86 28.57
PET6 GCC1 25.31 41.63 44.29 29.52 72.86 48.57
PET7 GCC1 26.94 36.73 47.14 31.43 64.29 42.86
PET8 GCC2 26.94 36.73 47.14 31.43 64.29 42.86
PET9 Qatar 27.76 32.65 48.57 32.38 57.14 38.10
PET10 Qatar 31.02 98.78 54.29 36.19 172.86 115.24
PET11 Qatar 35.10 56.33 61.43 40.95 98.57 65.71
PET12 MiddleEast2 38.37 48.98 67.14 44.76 85.71 57.14
PET13 GCC1 41.63 63.67 72.86 48.57 111.43 74.29
PET14 Middle East 1 69.39 208.98 121.43 80.95 365.71 243.81
PET15 GCC3 127.35 392.65 222.86 148.57 687.14 458.10
PET16 Middle East1 128.16 331.43 224.29 149.52 580.00 386.67
PET17 Asia1 155.92 377.14 272.86 181.90 660.00 440.00
PET18 EU1 161.63 416.33 282.86 188.57 728.57 485.71
PET19 EU2 178.78 498.78 312.86 208.57 872.86 581.90
PET20 EU2 184.49 456.33 322.86 215.24 798.57 532.38
PET21 EU3 185.31 484.08 324.29 216.19 847.14 564.76
PET22 Qatar 186.12 364.08 325.71 217.14 637.14 424.76

CDI-1: Based on adult, 70 kg, 2 L a day consumption of water, storage at normal temperature of 24 °C; CDI-2: Based on adult, 70 kg, 2 L a
day consumption of water, storage at normal temperature of 50 °C; CDI-3: Based on child, 10 kg, 0.5 L a day consumption of water, storage
at normal temperature of 24 °C; CDI-4: Based on child, 30 kg, 1 L a day consumption of water, storage at normal temperature of 24 °C; CDI-
5: Based on child, 10 kg, 0.5 L a day consumption of water, storage at normal temperature of 50 °C; CDI-6: Based on child, 30 kg, 1 L a day
consumption of water, storage at normal temperature of 50 °C

destabilization of the PET at such temperature. Such
groups are thought to absorb the Sb released in water
and hence produce a negative effect. Takur et al. (2012)
also reported that bottle aging and increase in bottle
volume were associated with decreased migration of
antimony from PET bottles, even when storage times
increase. Similarly, Fan et al. (2014) used a release
kinetic equation to describe the release of Sb with time.
The authors reported that the Sb releasing rate decreased
with the storage duration for all the brands tested in their
study. The results showed that although the release rate
was still significant after a period of 4 weeks, it de-
creased gradually with longer storage times.
Studies by Chen et al., (2010), Chapa-Martínez et al.
2016, and Keresztes et al. (2009) indicated that the
impact of temperature is more important than that of
storage time or exposure to sunlight. Additionally, and
based on the findings of this study, there is a need for a
nationwide survey about the quality of all other brands
of bottled water sold in Qatar. The guidelines for the
ideal storage condition should be enforced on local
companies. In addition, enforcing the exporting water
companies to provide a specification of PET is neces-
sary as well as to follow the international standards of
safe PET industry. Public awareness is also important
since it can lead to more confidence in local water.
Human risk assessment of long-term exposure
Although results may initially indicate that levels of Sb
in drinking water are lower, in most cases, than the 4–
5 μg/L, it is essential to consider the long-term effects of
ingestion waters containing low dosage of Sb using
specific guideline values given by the US environmental
Environ Monit Assess (2017) 189:631
protection agency (USEPA 1999). For this purpose, the
CDI (chronic daily intake) values are estimated using
Eq. 1 (Chapa-Martínez et al. (2016).
CDI ¼ C  DI=BW ð1Þ
where C represents the concentration of Sb in the water
(ng/L) and DI represents the recommended average
intake of water per day. The amount is estimated at
2 L of drinking water per day for adults and 1 L per
day for children Fan et al. (2014). BW is the body
weight and a typical value between 70 and 72 kg is used
for adults and 10–32.7 kg is used for children (Chapa-
Martínez et al. 2016). The value obtained using Eq. 1 is
further divided by 0.38% as this value represents the
contribution of drinking water in the total Sb intake by
humans (Keresztes et al. 2009).
In our current study, the BW value of 70 kg for an adult
will be used while two values for children will be consid-
ered, namely 10 and 30 kg representing two ranges of age
groups in children (younger and older), respectively. In
addition, 10-kg children are assumed to drink 0.5 L of clear
water a day. Calculated results are detailed in Table 2. The
results obtained are compared to a set value known as the
reference dose value (RfD) that represents the daily oral
exposure. RfD value of 400 ng/kg/day was given in the
guidelines developed by the USEPA.
It can be seen from Table 2 that, in general, all brands
tested showed values below the RfD value set in the
USEPA at a normal temperature of 24 °C for adults. At
higher temperatures (50 °C), 4 EU brands had CDI levels
higher than the recommended RfD of 400 ng/kg/day,
reaching a maximum value of 498 ng/kg/day in brand
#19 (EU2) for adults. The value is nearly double the
recommended RfD at an elevated temperature of 50 °C
for the same brand for example when children are
considered.
In general, the CDI values are generally higher in
smaller children than in older children. The values for
adults are lower in general given the bigger body weight
(70 kg). The results indicate that there are indeed health
risks linked to the ingestion of Sb leached from PET bottles
in adults; the risk is more pronounced in younger children.
Conclusions
In this work, a survey of antimony concentration of 22
bottled water brands from ten different countries
Page 11 of 12 631
currently sold in the Qatari market was carried out.
The measurement was conducted at both ambient tem-
perature (24 °C) and at experimental conditions (50 °C).
The Sb concentration varies from one brand to another
and between locally sourced and imported brands. This
difference is attributed to the possibly high-temperature
storage conditions during transportation, as well as to
the poor quality of PET material and the long period of
storage from bottling to use. Of the 22 brands of bottle
water studied, five brands exceeded the recommended
limit set by Qatari standards (5 μg/L), four of these
brands were imported and one was locally produced.
The amount of Sb in bottled water at 24 °C ranged from
0.221 to 2.281 μg/L and from 0.23 to 6.11 μg/L at
50 °C. A substantial increase of Sb concentration occurs
when water in bottles were incubated at 50 °C. On the
whole, the concentration of Sb measured in this work
was less than the recommended level of Qatar Standards
at 24 °C but above the limit at 50 °C for some brands.
The study also highlighted that long-term health issues
that can indeed occur from ingesting water stored in
PET bottles in inadequate temperature controlled con-
ditions especially for younger children.
Acknowledgements The authors would like to thank the Cen-
tral Food Laboratory at Ministry of Public Health for their help to
analyze the samples. Special thank for Dr. Mohammad Al-Thani,
the director of public health; Mrs. Wassan Al-Baker; and Dr.
Mohamad Ali for their kind support.
References
98/83/EC, D. (1998). Council of the European Union, off. J. EUR.
Union, 41, 32–53.
Aghaee, E. M., et al. (2014). Effects of storage time and temper-
ature on the antimony and some trace element release from
polyethylene terephthalate (PET) into the bottled drinking
water. Journal of Environmental Health Science &
Engineering, 12, 133–139.
Andra, S. S., Makris, K. C., Shine, J. P., & Lu, C. (2012). Co-
leaching of brominated compounds and antimony from bot-
tled water. Environment International, 38(1), 45–53.
Armas, A. B., & Sutherland, J. P. (1999). A survey of microbio-
logical quality of bottled water sold in the UK and changes
occurring during storage. International Journal of Food
Microbiology, 48, 59–65.
Bach, C., Dauchy, X., Chagnon, M.-C., & Etienne, S. (2012).
Chemical compounds and toxicological assessments of
drinking water stored in polyethylene terephthalate (PET)
bottles: a source of controversy reviewed. Water Research,
46(3), 571–583.
631 Page 12 of 12
Brenčič, M., Ferjan, T., & Gosar, M. (2010). Geochemical survey
of Slovenian bottled waters. Journal of Geochemical
Exploration, 107(3), 400–409.
Carneado, S., Hernández-Nataren, E., López-Sánchez, J. F., &
Sahuquillo, A. (2015). Migration of antimony from polyeth-
ylene terephthalate used in mineral water bottles. Food
Chemistry, 166, 544–550.
Carrieri, G., De Bonis, M. V., & Ruocco, G. (2012). Modeling and
experimental validation of mass transfer from carbonated
beverages in polyethylene terephthalate bottles. Journal of
Food Engineering, 108(4), 570–578.
Chapa-Martínez, C. A., Hinojosa-Reyes, L., Hernández-Ramírez,
A., Ruiz-Ruiz, E., Maya-Treviño, L., & Guzmán-Mar, J. L.
(2016). An evaluation of the migration of antimony from
polyethylene terephthalate (PET) plastic used for bottled
drinking water. Science of the Total Environment, 565, 511–
518.
Cheng, X., Shi, H., Adams, C., & Ma, Y. (2010). Assessment of
metal contaminations leaching out from recycling plastic
bottles upon treatments. Environmental Science and
Pollution Research, 17, 1323–1330.
de Jesus, A., Dessuy, M. B., Huber, C. S., Zmozinski, A. V.,
Duarte, Á. T., Vale, M. G. R., & Andrade, J. B. (2016).
Determination of antimony in pet containers by direct anal-
ysis of solid samples using graphite furnace atomic absorp-
tion spectrometry and leaching studies. Microchemical
Journal, 124, 222–227.
Duh, B. (2002). Effect of antimony catalyst on solid-state poly-
condensation of poly(ethylene terephthalate). Polymer,
43(11), 3147–3154.
Duranceau, S. J., Emerson, H. P., & Wilder, R. J. (2012). Impact of
bottled water storage duration and location on bacteriological
quality. International Journal of Environmental Health
Research, 22(6), 543–559.
Fan, Y.-Y., Zheng, J.-L., Ren, J.-H., Luo, J., Cui, X.-Y., & Ma, L.
Q. (2014). Effects of storage temperature and duration on
release of antimony and bisphenol A from polyethylene
te re pht h al at e dr inking wa te r bot tl es of C h ina .
Environmental Pollution, 192, 113–120.
Frengstad, B. S., Lax, K., Tarvainen, T., Jæger, Ø., & Wigum, B. J.
(2010). The chemistry of bottled mineral and spring waters
from Norway, Sweden, Finland and Iceland. Journal of
Geochemical Exploration, 107(3), 350–361.
Greifenstein, M., White, D. W., Stubner, A., Hout, J., & Whelton,
A. J. (2013). Impact of temperature and storage duration on
the chemical and odor quality of military packaged water in
polyethylene terephthalate bottles. Science of the Total
Environment, 456–457, 376–383.
Guart, A., Bono-Blay, F., Borrell, A., & Lacorte, S. (2014). Effect
of bottling and storage on the migration of plastic constitu-
ents in Spanish bottled waters. Foof Chemistry, 156, 73–80.
Güler, C. (2007). Evaluation of maximum contaminant levels in
Turkish bottled drinking waters utilizing parameters reported
on manufacturer’s labeling and government-issued produc-
tion licenses. Journal of Food Composition and Analysis,
20(3–4), 262–272.
Environ Monit Assess (2017) 189:631
Holland, B. J., & Hay, J. N. (2002). The thermal degradation of
PET and analogous polyesters measured by thermal analy-
sis—Fourier transform infrared spectroscopy. Polymer,
43(6), 1835–1847.
Ikem, A., Odueyungbo, S., Egiebor, N. O., & Nyavor, K. (2002).
Chemical quality of bottled waters from three cities in eastern
Alabama. Science of the Total Environment, 285(1–3), 165–
175.
Keresztes, S., Tatar, E., Mihucz, V. G., Virag, I., Majdik, C., &
Zaray, G. (2009). Leaching of antimony from PET bottles
into mineral water. Science of the Total Environment, 407,
4731–4735.
Marcinkowska, M., Lorenc, W., & Baralkiewicz, D. (2017). Study
of the impact of bottles material and color on the presence of
AsIII, AsV, SbIII, SbV and CrVI in matrix-rich mineral water—
multielemental speciation analysis by HPLC/ICP-DRC-MS.
Microchemical Journal, 132, 1–7.
Reimann, C., Birke, M., & Filzmoser, P. (2010). Bottled drinking
water: Water contamination from bottle materials (glass, hard
PET, soft PET), the influence of colour and acidification.
Applied Geochemistry, 25(7), 1030–1046.
Reimann, C., Birke, M., & Filzmoser, P. (2012). Temperature-
dependent leaching of chemical elements from mineral water
bottle materials. Applied Geochemistry, 27(8), 1492–1498.
Rowell, C., Kuiper, N., & Preud’Homme, H. (2016). Is container
type the biggest predictor of trace element and BPA leaching
from drinking water bottles? Food Chemistry, 202, 88–93.
Sánchez-Martínez, M., Pérez-Corona, T., Cámara, C., & Madrid,
Y. (2013). Migration of antimony from PET containers into
regulated EU food simulants. Food Chemistry, 141(2), 816–
822.
Sax, L. (2010). Polyethylene terephathalate may yield endocrine
disruptors. Environmental HEALTH PRESPECTIVES,
118(4), 445–448.
Shotyk, W., & Krachler, M. (2007). Contamination of bottled
water with antimony leaching from PET increases upon
storage. Environmnetal Science and Technology., 41(5),
1560–1563.
Smichowski, P. (2008). Antimony in the environment as a global
pollutant: a review on analytical methodologies for its deter-
mination in atmospheric aerosols. Talanta, 75(1), 2–14.
Takahashi, Y., Sakumak, K., Itai, T., Zengh, G., & Mitsunobu, S.
(2008). Speciation of antimony in PET bottles produced in
Japan and China by X-ray absorption fine structure spectros-
copy. Environment Science and Technology, 42, 9045–9050.
Takur, A., Sharp, L., Stern, B., Tizaoui, C., & Benkreira, H.
(2012). PET bottle use patterns and antimony migration into
bottled water and soft drinks: the case of British and Nigerian
bottles. Journal of Environmental Monitoring, 14, 1237–
1247.
USEPA (1999) Integrated Risk Information System (IRIS) on
Antimony. National Center for Environmental Assessment,
Washington DC.
Westerhoff, P., Prapaipong, P., Shock, E., & Hillaireau, A. (2008).
Antimony leaching from polyethylene terephthalate (PET)
plastic used for bottled drinking water. Water Research,
42(3), 551–556.