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Polystyrene cups and containers: Styrene migration

a a
M. S. Tawfik & A. Huyghebaert
a
Department of Food Technology and Nutrition, Faculty of Agriculture and Applied
Biological Sciences, Coupure links 653, Ghent, B‐9000, Belgium
Published online: 10 Jan 2009.

To cite this article: M. S. Tawfik & A. Huyghebaert (1998): Polystyrene cups and containers: Styrene migration, Food
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 Food Additives and Contaminants, 1998, Vol. 15, No. 5, 592-599
Polystyrene cups and containers: styrene migration
M. S. Tawfik† and A. Huyghebaert
Department of Food Technology and Nutrition, Faculty of Agricul-
ture and Applied Biological Sciences, Coupure links 653, B-9000
Ghent, Belgium.
Downloaded by [The University Of Melbourne Libraries] at 21:50 30 April 2013
(Received 4 June 1997; revised 25 September; accepted
24 October 1997)
The level of styrene migration from polystyrene cups
was monitored in different food systems including:
water, milk (0.5, 1.55 and 3.6% fat), cold beverages
(apple juice, orange juice, carbonated water, cola, beer
and chocolate drink), hot beverages (tea, coffee,
chocolate and soup (0.0, 0.5, 1, 2, and 3.6% fat), take
away foods (yogurt, jelly, pudding and ice-cream), as
well as aqueous food simulants (3% acetic acid, 15, 50,
and 100% ethanol) and olive oil. Styrene migration
was found to be strongly dependent upon the fat content
and storage temperature. Drinking water gave migra-
tion values considerably lower than all of the fatty
foods. Ethanol at 15% showed a migration level
equivalent to milk or soup containing 3.6% fat. Max-
imum observed migration for cold or hot beverages and
take-away foods was 0.025% of the total styrene in the
cup. Food simulants were responsible for higher migra-
tion (0.37% in 100% ethanol). A total of 60 food
samples (yogurt, rice with milk, fromage, biogardes,
and cheese) packed in polystyrene containers were
collected from retail markets in Belgium, Germany,
and the Netherlands. The level of styrene detected in
the foods was always fat dependent.
Keywords: polystyrene, cups, migration, beverages,
food simulants
Introduction
There has been widespread concern in recent years
with the migration of substances from packaging
materials into foods, particularly the migration of
† To whom correspondence should be addressed.
0265-203X/98 $12.00 © 1998 Taylor & Francis Ltd
monomers from plastics. The diffusion of chemicals
from polymers is of interest to the U.S. Food and
Drug Administration (FDA) in its regulation of
polymeric food packaging materials (Snyder and
Breder 1985). Styrene is one of the most widely used
monomers in food-contact polymers. Various types of
polystyrene cups, including foam, impact, and crystal
were studied.
Packaging and disposable serviceware are the major
applications for styrene plastics (Watson and Wallace
1985). The primary food-contact applications of
polystyrene are containers for yogurt, cream, cottage
cheese, ice-cream, and fruit juice, meat trays, biscuit
trays, egg cartons, take-away food and drink cups,
and produce boxes (Flanjak and Sharrard 1984).
The amounts of polystyrene used in manufacturing
foam, impact and crystal polystyrene cups in the U.S.
were 90, 144, and 50 million pounds, respectively
(Varner and Breder 1981). In the United Kingdom,
cups for vending machines and disposable drinking
containers are estimated to account for some 45% of
the total production of food-grade rigid polystyrene
(Castle et al. 1991).
Residual monomers in food-contact polymers are
known to migrate into foods, and there is growing
interest in the effects of some of these chemicals on
human health. Several adverse health effects are
attributed to styrene. Humans experience eye, nose,
throat, and skin irritation when exposed to the
vapours. Styrene has a toxic effect on the liver, acts
as a depressant on the central nervous system, and
causes neurological impairment. An increase in the
frequency of chromosomal aberrations has been ob-
served in the lymphocytes of human subjects occupa-
tionally exposed to styrene (Varner et al. 1983).
Previous work indicated that styrene levels of 60-
2250 ppm were present in polystyrene food packaging
(Varner and Breder 1981). Several studies have re-
ported the presence of styrene in food products,
caused by migration of residual styrene from the
polymer. Withey and Collins (1978) reported styrene
detected in dairy products at levels up to 245 ppb in
sour cream. In hot chocolate and chocolate spread
 Styrene migration to different food stuffs
they found 13ppb and 2ppb, respectively. Gilbert
and Startin (1983) found different levels of styrene
in food products, e.g. 180ppb in chopped candied
peel. Varner et al. (1983) examined the styrene
migration into margarine and they found that there
was no detectable migration. Snyder and Breder
(1985) studied the migration of styrene from poly-
styrene into various solvents. They concluded that
styrene migrated at similar rates into 20% ethanol,
corn oil, and HB-307 (a synthetic triglyceride).
The work in this paper evaluates the level of food
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contamination by styrene monomer derived from
food contact materials, especially disposable drinking
containers, to study the effect of different parameters
including the fat content, temperature and time on the
migration level, and to compare the ability of differ-
ent foodstuffs and simulants to induce the migration
of monomer.
Materials and methods
Cups
Clear polystyrene cups (volume 200 ml, surface area
1.31 dm2), which are commonly used for cold and hot
drinks vending machines in the Belgian market were
used.
Samples
Foodstuffs. Different foodstuffs involved in this
study included:
(a) UHT milk samples with different fat contents (0.5,
1.55, and 3.6%); (b) cold beverages (apple juice,
orange juice, carbonated water, cola, beer, chocolate
drink); (c) hot beverages (tea, coffee, chocolate drink)
obtained as dry powders, and reconstituted with
boiling distilled water before use; (d) jelly and pud-
ding prepared before putting in cups; (e) soup samples
(fat content 0, 0.5,1, 2, 3.6%) prepared with boiling
water before use; and (f) ice-cream packed in cups
before storage.
Food simulants. 3% acetic acid, 15, 50, 100%
ethanol, and olive oil.
593
Survey samples, were purchased from supermarkets
and stored at 4°C until analysed. The samples were
usually stored for no longer than seven days before
being analysed.
Chemicals
Styrene (99%) and oc-methyl styrene (99%) were
obtained from Aldrich-Europe, Belgium. All other
chemicals and solvents used were analytical grade,
i.e. purity > 99% , obtained from Across Chemical
N.V., Belgium.
HPLC
Chromatographic analysis was performed with an
Analis HPLC (model 305) with UV/VIS absorbance
detector and a data module integrator/recorder. The
column (250 x 4.6 mm) was packed with Lichrosorb
RP-18 10 ul and the mobile phase was distilled water-
acetonitrile (25%-75%) at flow rate of l.Oml/min.
Sample injection volume was 50 ul. The detector was
set at 245 nm.
Determination of styrene in polystyrene cups
A cup was weighed, cut into pieces, dissolved in
dichloromethane, and subsequently precipitated with
iso-octane. The sample was centrifuged at 4000 rpm
for 20min. The clear supernatant was removed and
concentrated to about 1.0 ml for HPLC analysis as
described above.
Migration experiments
The test conditions of the samples are shown in
table 2. Parallel migration tests using simulants were
performed. Samples of all tested products or simu-
lants which had not been in contact with polystyrene
containers were analysed as blank controls. Three
replicates and two duplicate samples at timed inter-
vals were performed for every experiment.
 594 M. S. Tawfik and A. Huyghebaert
Styrene analysis in food samples
A 50 g measure of the homogenized sample was
placed into a 250 ml round bottom flask, mixed with
50 ml of distilled water and 25 ml of acetonitrile
(HPLC grade). Anti-bumping granules and 2 ml of
calcium chloride (20%) were added, plus 2 ml of oc-
methylstyrene (4mg/litre in methanol) were added as
internal standard. The flask was fitted with a splash
head, straight condenser and take-off and the solution
was slowly distilled over a period of 1 hour, collecting
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about 24 ml of the distillate in a 25 ml volumetric
flask. The distillate was made up to 25 ml with
distilled water (Flanjak and Sharrad 1984). The
calculation of recovered styrene was done according
to the calibration curve method by addition of 10 ul
increments (up to 100 ul) of styrene working solution
(90.6mg/litre in methanol) to a styrene-free sample of
the food (calibration standard). An identical volume
of internal standard was added to each sample. The
retention times for styrene and oc-methylstyrene were
approximately 6 and 7.5 min respectively. In the food
simulants (acetic acid, ethanol, olive oil), styrene was
distilled and determined by the same procedure.
Known amounts of styrene monomer (0.05mg/kg)
were added to some food samples to determine
recovery of styrene from different foodstuffs. The
limit of detection of the analytical method for styrene
analysis in food samples is 0.001 mg/kg (table 2).
Results and discussion
Migration of monostyrene from polystyrene (PS)
cups into hot and cold beverages and food simulants
Recovery of added styrene from various foods is
presented in table 1. The range of recovery was
82.4% to 99.2%, the lowest being ice-cream. The
determined amount (mean of three determinations
from three cups) of styrene in polystyrene cups was
90.35 ppm. The migrated levels of styrene monomer
from the PS cups into water at different incubation
temperature and time are presented in table 2. The
migration level increased with time, and the rate was
accelerated by increasing storage temperature. The
migration of monostyrene to water at 4° and 20°C
were < 0.001 mg/kg after three days. Durst and
Laperle (1990) indicated that at a constant tempera-
Table 1. Recovery of added styrene from various foods.
No. of Amount added
Sample experiments (mg/kg) % Recovery*
Water 5 0.05 99.2
Milk 5 0.05 96.7
Juice 3 0.05 98.9
Ice-cream 5 0.05 82.4
Soup 5 0.05 97.6
Yogurt 5 0.05 91.8
Mozzarella 7 0.05 85.3
Cheese 7 0.05 87.9
* Results presented as an average of three determinations from three
separate samples.
ture, the styrene pick-up should be proportional to
the square root of the time for some initial period.
Exposure conditions were chosen based on a number
of criteria. In the case of simulants, the European
Community test conditions (EEC 1985) close to those
of expected use were chosen (24 h at 40°C for cold
beverages, and 1 h at 100°C for hot beverages), but
for actual foods, conditions were chosen that at-
tempted to recreate a worst case exposure. For
instance, cold beverages were exposed overnight
(about 16 h at room temperature), whilst exposing
the vending machine cups to hot beverages for 1 h at
100°C is far more rigorous than any real exposure, as
a beverage does not come from a machine at this
temperature, and anyway would cool very rapidly.
The aggressiveness of the latter set of conditions is
illustrated by the fact that some of the cups collapsed
due to heat softening.
Directive 93/8/EEC lays down the test conditions to
be chosen according to conditions of contact in actual
use. In our migration experiments, we applied differ-
ent conditions, as our main interest was focused on
the actual use of these cups and the comparison
between the different storage times and temperatures.
Migration levels of styrene from PS cups into hot and
cold beverages and food simulants measured in these
studies are reported in table 2. There is a relationship
between the extent of migration and food composi-
tion, e.g. the fat content. The migration of styrene
from the cups into whole milk (3.6% fat) was more
than into half-fat milk (1.55% fat) and both were
more than into skimmed milk (0.5% fat) at different
temperatures and storage times. The differences be-
tween the three fat percentages were clearer at the
highest temperatures (60 and 100°C) after 2 hours of
storage, but there were no significant differences
 Styrene migration to different food stuffs 595

Table 2. Migration of styrene from polystyrene cups into hot and cold beverages and food simulants.
Styrene residues*
Beverage/simulant Test conditions mg/kg mg/dm
Distilled water 1 h at 100°C 0.007 0.001
2 hat 100°C 0.014 0.002
3 days at 60°C 0.017 0.0026
3 days at 40°C 0.015 0.002
3 days at 20°C < 0.001 < 0.0002
3 days at 4°C < 0.001 < 0.0002
Whole milk (3.6% fat) 2 hat 100°C 0.071 0.011
2h at 60°C 0.015 0.0022
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2hat40°C < 0.001 < 0.0001

24hat40°C 0.024 0.0036
2hat20°C < 0.001 < 0.0001
24hat20°C 0.0125 0.0019
24hat4°C < 0.001 < 0.0001
3 days at 4°C 0.003 0.0004
Half-fat milk (1.55% fat) 2 hat 100°C 0.069 0.0102
2hat60°C 0.004 0.0006
2h at 40°C < 0.001 < 0.0001
24hat40°C 0.0187 0.0028
2hat20°C < 0.001 < 0.0001
24hat20°C 0.0077 0.001
24hat4°C < 0.001 < 0.0001
3 days at 4°C < 0.001 < 0.0001
Skimmed milk (0.5% fat) 2 hat 100°C 0.034 0.005
2 hat 60°C 0.001 0.0001
2 h at 40°C < 0.001 < 0.0001
24 h at 40°C 0.015 0.0022
2hat20°C < 0.001 < 0.0001
24hat20°C 0.005 0.0007
24hat4°C < 0.001 < 0.0001
3 days at 4°C < 0.001 < 0.0001
Apple juice 16hat20°C 0.005 0.0007
Orange juice 16hat20°C 0.003 0.0005
Carbonated water 16hat20°C 0.0058 0.0009
Cola 16hat20°C 0.005 0.0007
Beer 16hat 20°C 0.006 0.0009
Drinking chocolate 16hat20°C 0.0045 0.0007
Drinking yogurt (3% fat) 3 days at 4°C < 0.001 < 0.0001
7 days at 4°C 0.008 0.001
14 days at 4°C 0.010 0.001
Jelly 1 day at 4°C < 0.001 0.0002
3 days 4 at °C 0.005 0.0008
7 days at 4 °C 0.007 0.001
Pudding with whole milk 1 day at 4°C < 0.001 0.0001
3 days at 4°C 0.008 0.0012
7 days at 4°C 0.009 0.0014
Ice-cream 30 days at -10°C 0.0187 0.002
60 days at -10°C 0.024 0.003
Tea l h a t 100°C 0.008 0.001
Coffee l h a t 100°C 0.007 0.001
Chocolate 1 h at 100°C 0.007 0.001
 596 M. S. Tawfik and A. Huyghebaert

Table 2—Continued
Styrene residues*
Beverage/simulant Test conditions mg/kg mg/dm
Soup (3.6% fat) 1 h at 100°C 0.015 0.002
(2%) 1 h at 100°C 0.0102 0.0019
(1%) In at 100°C 0.009 0.0017
(0.5%) 1 h at 100°C 0.007 0.001
(0.0%) 1 h at 100°C 0.002 0.0004
1 h at 100°C 0.029 0.004
3% acetic acid 24hat40°C 0.009 0.0014
1 h at 100°C 0.015 0.002
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15% ethanol 24hat40°C 0.026 0.004

1 h at 100°C 0.211 0.032
50% ethanol 24 h at 40°C 0.035 0.005
1 h at 100°C 0.343 0.051
100% ethanol 24hat40°C 0.058 0.009
1 h at 100°C 0.121 0.015
Olive oil 24hat40°C 0.082 0.011
* Results presented as an average of three determinations from three samples. Results were corrected by recovery correction
factors.

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20°C 40°C 60°C 100°C
Temperature
D 0.50% B 1.55% •3.60% |

Figure 1. Migration of styrene monomer from polystyrene cups into milk with different fat contents after 2 hours of
storage at different temperatures.

between them at 20 and 40°C (figure 1). The fat
migration dependence is also confirmed as shown,
with increasing styrene migration proportional to
increasing fat content of soup (table 2).
Migration in drinking water was considerably lower
than all of the three milk types and soups under the
same test conditions. These results were in agreement
with the results of O'Neill et al. (1994) who measured
the styrene monomer migration from polystyrene
cups into milk containing 0.5, 3.5 or 10% fat. They
concluded that water gave migration values con-
siderably lower than all of the three milk types.
Ramshaw (1984) has also stated that the amount of
migrated styrene is higher in products with a higher
fat content.
 Styrene migration to different food stuffs 597

0.07 x

~ 0.06
E
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sh
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i
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>>
55
0.01 --

+ +
3.6 1.55 0.5 15 50 100
% fat % ethanol
Figure 2. Migration of styrene monomer from polystyrene cups into different types of milk after 24 hours at 40°C
compared with different concentrations of ethanol in water.

The migration of styrene into some cold beverages
and yogurt are shown in table 2. For drinking yogurt
(3% fat) the styrene migration increased with storage
time. Flanjak and Sharrad (1984) showed that the
mean values of all samples of yogurt in the Victoria
and New South Wales survey were 0.021 and
0.032 mg/kg respectively. In the literature the mi-
grated value of styrene monomer into yogurt is quite
variable, and ranges from 0.003 to 0.220 mg/kg (Rosli
and Marek 1977, Withey and Collins 1978, Gawell
and Larsson 1980). As with the drinking yogurt, the
rate of migration into the rest of the tested products
(jelly, pudding, and ice-cream) was followed with
increasing time (table 2).
For hot beverages (tea, coffee, and chocolate), in all
cases styrene migration occurred. The amount of
styrene leached was in the range of 0.001 mg/dm2.
Varner and Breder (1981) reported that hot coffee and
tea extract styrene to the same extent as does hot
water. Similarly, in this study, the amount of styrene
migrated per unit area was 0.001 mg/dm2 for foam
cups with water, tea, or coffee.
Due to the complex composition of most foodstuffs,
the determination of migration levels in food pro-
ducts can cause unresolvable analytical difficulties.
Consequently, it is necessary to use both conventional
food simulants and standardized test conditions
which are meant to simulate the migration behaviour
of substances into foods under actual conditions of
use (O'Neill et al. 1994). The directive 82/71 I/EEC
lists the following food simulants: (a) distilled water
of equivalent quality; (b) 3% (w/v) acetic acid in
aqueous solution; (c) 15% (v/v) ethanol in aqueous
solution; (d) rectified olive oil or else sunflower oil or
a synthetic triglyceride (e.g. HB-307). In the current
study 3% acetic acid, ethanol (15, 50, 100%), and
olive oil were used as food simulants. The 15%
ethanol was shown to correlate approximately with
3.6% fat in milk or soup. The results obtained from
the migration tests in this way are summarized in
figures 2 and 3. In a previous study by O'Neill et al.
(1994) the styrene concentration found in the 3.5%
fat milk was assumed to be comparable to that of the
50% ethanol. Snyder and Breder (1985) studied the
migration of styrene from polystyrene into various
solvents: water, 3% acetic acid, 8, 20, 50, and 100%
ethanol, corn oil, HB-307, heptane, hexadecane, and
decanol. They reported that all solvents extracted
only 1-2% of the total available styrene, with the
exception of 100% ethanol, which extracted 7% after
2 weeks at 40°C. In addition, Jickells et al. (1993)
reported that testing for 2h at 175°C into olive oil
resulted in significantly high migration of styrene.
Migration of styrene monomer into foods
The concentrations of styrene residue in food pack-
aged in polystyrene containers are summarized in
table 3. Once more, the results confirm the relation
 598 M. S. Tawfik and A. Huyghebaert

1 -r

E
c
0.1 - •

s
o
u
e
o
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o

i
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C/5
n£
0.001 +
3.6 1 0.5 15 50 100
% fat % ethanol
Figure 3. Migration of styrene monomer from polystyrene cups into different kinds of soup after 1 hour at 100°C
compared with different concentrations of ethanol in water.

Table 3. Styrene monomer residues in food packaged in polystyrene containers.

Styrene residues*
Food No. of samples mg/kg mg/dm 2
Yogurt (3.5% fat) 5 0.044 0.006
Yogurt (2.6% fat) 5 0.039 0.004
Mixed yogurt (2.9% fat) 5 0.036 0.004
Biogarde (3.4% fat) 7 0.048 0.009
Rice with milk (1.5% fat) 4 0.032 0.003
Fromage (1.5% fat) 5 0.030 0.003
Fromage (2.6% fat) 6 0.041 0.005
Mozzarella (14.0% fat) 7 0.069 0.011
Cheese (13.5% fat) 8 0.062 0.010
Cheese (8.9% fat) 8 0.054 0.008
Results presented as an average of three determinations from three samples. Results were corrected by recovery correction
factors.

between migration and fat content. Various studies
have shown that styrene migrates from polymeric
containers into foods. Withey and Collins (1978)
found that styrene migrated into high-butterfat cream
at levels of 22ppb after 5 days, 44ppb after 17 days
and 59 ppb after 24 days. Lower levels of migration
occurred in cottage cheese, sour cream, yogurt,
homogenized milk, cultured milk and honey. Studies
conducted by Davies (1979), using impact polystyrene
with residual styrene levels of 500 ppm, showed that
the monomer migrated into single cream (19.5% fat)
at concentrations of 20 ppb after 1 day, 107 ppb
after 7 days, and 170 ppb after 21 days, while in
double cream (53% fat) the level reached to
20 ppb after 1 day, 150 ppb after 7 days, and
270 ppb after 21 days. In a survey study, Flanjak
and Sharrad (1984) determined the migration of
styrene monomer from polystyrene containers into
146 samples from Victoria and New South Wales
which included yogurt, cream cheese, desserts, ice-
cream, egg white, onion dip, and margarine. They
found that the highest levels of styrene were 50 ppb
in yogurt and the lowest values (less than 10 ppb)
were in margarine samples. They suggested that
because of the hydrophobic nature of styrene the
efficiency of the distillation process for margarine is
not very high, which is consistent with low recovery
values obtained.
 Styrene migration to different food stuffs
Conclusion
The results in this study indicated that the migration
of styrene from polystyrene cups into different bev-
erages does not increase more than 0.08% (in whole
milk stored at 100°C for 2 hours) of the total amount
of styrene in the cup. The level of migration essen-
tially depends upon the fat content, storage tempera-
ture, and time. Migration testing employing aqueous
food simulants will necessarily lead -^Hinder-estima-
tion of the migration processes occurring in real food
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products. The styrene concentration in the 3.6% fat
milk or soup, is assumed to be comparable to that of
the 15% ethanol at 40°C after 24 hours. Further, the
migration of styrene into hot beverages was more
than into the cold ones, and was affected by the time
of contact.
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