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# 1998 Elsevier Science Ltd. All rights reserved.
PII: S1089-3156(98)00040-3 0189-3156/98/$Ðsee front matter
Reusing old polymer as new food packages is a vast ecological objective. From the scienti®cal point of
view various problems must be resolved for ensuring the food safety. Thus the new food packages are in
sandwich form where the recycled polymer layer with potential contaminant is located between two virgin
polymer layers. The main problem arising is the prediction of the time of food protection. A contaminant
transfer occurs during the coextrusion process through the package, being responsible for a decrease in
this time of food protection. The eect of the thickness of the package is especially considered. It appears
during the coextrusion process because the cooling period of the package strongly increases with the
thickness; it also plays a role in the contaminant transfer through the package and into food. The process
of contaminant transfer is studied not only during the coextrusion stage, but also with the food-package
system. The eect of the thickness of the package on the time of food protection is especially studied.
# 1998 Elsevier Science Ltd. All rights reserved.
(Keywords: food safety; polymer package; recycling; tri-layer package; processing; heat and mass transfers)
COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998 331
Effect of food package thickness on the time of food protection: A. L. Perou et al.
Communities5±7. However, as the recycled polymer temperature developing into the package. Asso-
is potentially contaminated from its previous use, ciated with this heat transfer a contaminant trans-
the new food package must be made of tri-layer fer takes place with a temperature-dependent
polymers, the recycled polymer layer being located diusivity leading to a pro®le of contaminant
between two virgin polymer layers7±9. The transfer concentration through the package in the ®nal
process of contaminant in the food-package system tri-layer package. A numerical model is thus
is controlled by diusion through the package10,11 built, taking into account both the heat and mass
and either by convection into the liquid food12 transfer18,19.
or diusion through the solid food13,14. As it The other purpose of this study is to determine
takes time for the contaminant to diuse through by calculation the time of food protection obtained
the virgin polymer layer located between the recy- with this coextruded tri-layer package. The case of
cled polymer and the food, this virgin polymer a liquid food is considered, and the contaminant
layer plays the role of a functional barrier to food transfer is controlled either by convection into the
contamination. food and diusion through the package with a
The main problem which arises is the prediction constant diusivity. The transfer of the food into
of this time of food protection. It can be deter- the package is neglected. The initial pro®le of con-
mined either by highly time-consuming experi- taminant concentration is that obtained at the end
ments or by calculation. The mathematical of the coextrusion process. Moreover, the eect of
treatment is feasible for the transfer through the the thickness of the package is examined, when the
package alone when the diusivity is constant10,11. three polymer layers have the same thickness.
When the package is in contact with the liquid
food, with a ®nite coecient of convective transfer
THEORETICAL
in the liquid next to the package surface, a numer-
ical treatment is necessary12,13, in spite of an The following two processes are considered in suc-
attempt to mix the equations obtained on one hand cession: the ®lms coextrusion with heat transfer
with an in®nite volume of liquid and a ®nite coef- and mass transfer at high temperature; the con-
®cient of convective transfer and on the other hand taminant transfer with the food-package system at
with a ®nite volume of liquid and an in®nite con- room temperature.
vection coecient15.
In fact, the problem is far more complex and two Process of ®lms coextrusion
main assumptions have been made in the previous
studies in calculating the time of food protection: Assumptions
(i) the transfer of the liquid food into the polymer
does not interfer on the contaminant transfer, in 1. The three thin ®lms are coextruded and heat
spite of that fact intervenes in case of plasticized and mass transfers are unidirectional through
PVC16,17; and (ii) the contaminant is only located the thickness of these ®lms.
in the recycled polymer layer with a uniform 2. The recycled polymer layer is located between
concentration. This second assumption means that the two virgin polymer layers.
no contaminant transfer takes place during the 3. The three layers are in perfect contact with no
coextrusion of the tri-layers of the package18. In resistance to heat and mass transfer.
fact, during the preparation of the package each 4. Initially, the contaminant concentration is
polymer layer is heated and melted and the tri- uniform in the recycled polymer layer, while
layer polymers are coextruded. The tri-layer ®lm is the virgin polymer layers are free from con-
then allowed to cool down in air. It has been taminant.
shown by calculation that during this short period 5. The package initially at the uniform tempera-
of time at high temperature, a diusion of the ture of coextrusion (300 or 330 C) is cooled
contaminant takes place with a temperature- down is motionless air at 20 C. Heat is trans-
dependent diusivity either with bi-layer18 or a tri- ferred by free convection at the air±package
layer19 package. interface and by conduction through the
The ®rst objective in this paper is to evaluate the package.
contaminant transfer during the coextrusion pro- 6. As soon as the three polymer layers are coex-
cess expressed by a concentration pro®le of con- truded, during the cooling period in air, a
taminant in the package. Of course, during the contaminant transfer takes place through the
coextrusion process heat is transferred by free package controlled by Fickian diusion. The
convection at the package surface and by conduc- diusivity varies with temperature by follow-
tion through the package, leading to pro®les of ing an Arrhenius' law.
332 COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998
Effect of food package thickness on the time of food protection: A. L. Perou et al.
COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998 333
Effect of food package thickness on the time of food protection: A. L. Perou et al.
334 COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998
Effect of food package thickness on the time of food protection: A. L. Perou et al.
temperature decreases quickly at the begin- thickness acts not only upon the rate of con-
ning of the process (curves 1, 2, 3 at 300 C taminant transfer but also on the relative
and 10 , 20 , 30 at 330 C). amount of contaminant transferred Mt =Min ,
2. The eect of the coextrusion temperature with this statement: the thinner the ®lm, the
clearly appears. faster the contaminant transfer and the
3. The thickness of the ®lm intervene on the rate greater the relative amount of contaminant
of decrease in temperature with the obvious transferred.
statement: the thinner the ®lm, the faster the 3. The eect of the coextrusion temperature is of
rate of decrease in temperature. The tempera- great importance whatever the thickness of
ture decreases to around 200 C after only 2 s the ®lm (1, 2, 3 at 300 C and 10 , 20 , 30 at
for the 90 microns thick ®lm. 330 C). Especially the relative amount
4. The thickness of the ®lm is responsible for a Mt =Min of contaminant transferred largely
dierence in temperature through the ®lm increases with the coextrusion temperature.
depending on position. Of course, the tem- 4. Of course, the rate of contaminant transfer
perature on the surface and at the middle of essentially varies with the temperature depen-
the ®lm is about the same for the thinner ®lm, dency of the diusivity. Tedious experiments
while a signi®cant dierence appears for the and calculation are done at temperature
thicker ®lm. around the softening temperature and not yet
published22. Calculation of the diusivity
Contaminant transfer during coextrusion needs a numerical model similar to that
Resulting from the high temperature of the coex- described in this paper.
trusion process, a contaminant transfer takes place 5. The pro®les of concentration of contaminant
through the ®lm. This transfer is controlled by dif- developed through the ®lm at the end of the
fusion with a concentration-dependent diusivity, coextrusion stage, e.g. after a few seconds, are
and thus the rate of transfer decreases during the shown in Figure 5 (90 microns), Figure 7
stage of cooling. (150 microns) and in Figure 9 (300 microns)
The results are expressed in two ways: with the for the coextrusion temperature of 330 C.
kinetics of contaminant transfer in Figure 4, and These pro®les are noticed 0 in these three ®g-
with the pro®les of concentration developed ures, being also the initial pro®les of con-
through the ®lm at the end of the coextrusion centration during the contaminant transfer in
process. the package±food system.
Some conclusions are worth nothing: 6. Comparison between these pro®les at time 0
shown in Figures 5, 7 and 9 shows clearly the
1. The transfer of contaminant through the ®lms eect of the thickness of the ®lm on the
is very fast, as shown in Figure 4, and it takes transfer. Thus for the thinner ®lm of
place in a few seconds. 90 microns, the contaminant reaches the ®lm
2. The eect of the thickness of the ®lm on the surfaces, while it does not for the larger
contaminant transfer appears in Figure 4. The thicknesses.
COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998 335
Effect of food package thickness on the time of food protection: A. L. Perou et al.
7. The midplane of the ®lm is a plane of sym- 1. These pro®les of contaminant developed at
metry for the temperature transfer, as well as various times give a fuller insight into the
for the mass transfer. The relative concentra- nature of the process of transfer through the
tion of contaminant at this midplane is of package.
interest: it is around 0.8 for the thinner ®lm, 2. The pro®les are symmetrical with the mid-
0.9 for the 150 micron ®lm and more than 0.95 plane as plane of symmetry when the con-
for the 300 micron ®lm. taminant is still located in the package.
3. When the contaminant reaches the food sur-
Contaminant transfer with the package-food system face, a transfer in the food takes place, and
the pro®les of concentration are not symme-
The contaminant transfer in the package±food trical. On the whole, the concentration on the
system at room temperature is controlled by diu- package surface in contact with the surround-
sion through the three layer package and convec- ing is higher than on the surface package in
tion into the liquid food. The diusivity is contact with food.
considered as constant because the concentration 4. For long times, e.g. 0.1 for Dt=L2 , the con-
of contaminant is very low in the package. The centration on the package surface in contact
values of the parameters: the diusivity, the coe- with the surrounding is even greater than in
cient of convective transfer and the volume of the recycled polymer layer, as already
liquid are shown in Table 2. The value of the coef- shown12.
®cient of convective transfer into the liquid is that 5. The gradient of concentration is always 0 on
obtained in olive oil23. The thickness of 1.6 cm for the package surface in contact with the sur-
the liquid corresponds with a liquid food of 1 litre rounding, as the contaminant does not eva-
in cubic shape. porate in air.
The results are expressed either through the pro- 6. Because of the dimensionless numbers, these
®les of contaminant concentration developed curves can be considered as master curves
which can be used for evaluating the transfer
Table 1 Characteristics for heat and mass transfer during coextru- of contaminant through the package.
sion the stage of coextrusion thickness of the tri-layer package: 0.005/
0.005/0.005 cm
Kinetics contaminant transfer in the food
9:9 10ÿ4 6:8 10ÿ7 T
cm2 sÿ1 T:Celsius The kinetics of contaminant transferred into the
l 6:1 10ÿ4 9:6 10ÿ8 T
cal cmÿ2 sÿ1 degÿ T:Celsius
food are drawn for the three thicknesses of the
h 2 10ÿ4 exp j ÿ TL ÿ Tair j025
cal cmÿ2 sÿ1 degÿ1 T:Celsius
ÿ
D 28 240 exp ÿ 13 T800
cm2 sÿ1 T:Celsius
package coextruded at 330 C, in Figure 6
(90 microns), Figure 8 (150 microns) and Figure 10
(300 microns). Dimensionless numbers are used for
Table 2 Characteristics of the contaminant transfer into the food each thickness: the amount transferred after time t
Diusivity D 10ÿ10 cm2 sÿ1
as a fraction of the initial amount of contaminant
Convective coecient h 10ÿ8 cm sÿ1 in the recycled polymer; Dt=L2 instead of time.
Thickness of the liquid (per unit area of package)=1.6 cm These kinetics are drawn under three conditions:
1 litre of food in cubic shape
in the hypothetical case when no contaminant
336 COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998
Effect of food package thickness on the time of food protection: A. L. Perou et al.
transfer takes place during the coextrusion stage an increase in this temperature is responsible
(curve 1); when coextrusion takes place with a for a signi®cant decrease in time of food pro-
contaminant transfer at 300 C (curve 2) and at tection.
330 C (curve 20 ). 4. It stands to reason that the coextrusion pro-
The following conclusions are obtained: cess cannot be neglected, as a signi®cant
Figure 6 Kinetics of contaminant transferred into the food from the Figure 9 Pro®les of contaminant concentration developed at various
tri-layer package of 90 microns: (1) with no transfer during coextru- times (Dt=L2 ) through the tri-layer package of 300 microns coextruded
sion, (2) with coextrusion at 300 C, and (20 ) at 330 C. at 330 C.
Figure 7 Pro®les of contaminant concentration developed at various Figure 10 Kinetics of contaminant transferred into the food from the
times (Dt=L2 ) through the tri-layer package of 150 microns coextruded tri-layer package of 300 microns: (1) with no transfer during coextru-
at 330 C. sion, (2) with coextrusion at 300 C, and (20 ) at 330 C.
COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998 337
Effect of food package thickness on the time of food protection: A. L. Perou et al.
transfer of contaminant takes place through Thus this paper has pointed out the importance of
the package. The eect of the diusivity the problem in food-package system with polymer
through the polymer at the coextrusion tem- recycling. It has also laid the way for further stu-
perature and the temperature-dependency of dies using the same numerical treatment in order to
the diusivity have to be determined with increase the time of food protection. Various ways
accuracy. Some work is in progress along this can be traced: trying to decrease the cooling period
direction22. after coextrusion; using dierent relative thick-
nesses for the layers of the package with a larger
thickness for the functional barrier in contact with
the food; and improving the experimental techni-
CONCLUSIONS que for determining the temperature-dependency
of the contaminant. The theoretical approach and
Following this study, it stands to reason that a the numerical model described in this paper can be
contaminant transfer takes place in a signi®cant of help to resolve these problems.
manner through the tri-layer ®lm during the stage
of coextrusion. Thus the contaminant is located
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338 COMP. AND THEOR. POLYMER SCIENCE Volume 8 Number 3/4 1998