Journal of Food Engineering 108 (2012) 570578

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Journal of Food Engineering

journal homepage: www.elsevier.com/locate/jfoodeng

Modeling and experimental validation of mass transfer from carbonated beverages

in polyethylene terephthalate bottles
Gabriella Carrieri, Maria Valeria De Bonis, Gianpaolo Ruocco
CFDfood - DITEC, Universit degli Studi dalla Basilicata, Campus Macchia Romana, Potenza 85100, Italy

a r t i c l e

i n f o

Article history:
Received 6 February 2011
Received in revised form 10 August 2011
Accepted 6 September 2011
Available online 12 September 2011
Keywords:
Mass transfer
Beverage packaging
Computational uid dynamics

a b s t r a c t
Mass transfer and related shelf life assessment is an important issue in the beverage industry. Product
change due to mass transfer is at stake and, with it, its consumer value and consideration.
Carbonation loss takes place at the product/package interface, and to the environment through the
package itself. In this paper a joint experimental/computational approach has been exploited: the CO2
loss through the polyethylene terephthalate barrier has been computed by means of a multidimensional
nite element code, while actual measurements have been carried out to validate the computations.
Residual carbonation histories are validated and presented for a variety of thermal regimes and for two
different bottles carrying the same capacity. The paper highlights on the combination of bottle weight,
initial carbonation and storage temperature, indicating the operational set for the longest shelf life within
the explored cases. Lighter bottles can be used with no inference on shelf life, while the carbonic loss
depends non-linearly on initial carbonation and temperature increment. The associated concentration
maps help infer on the importance of polyethylene terephthalate thickness uniformity.
It is then demonstrated that the model carries the exibility of a general tool, applicable to any carbonated beverage at any storage condition.
2011 Elsevier Ltd. All rights reserved.

1. Introduction
It is well known that the fundamental factors that contribute to
the keeping characteristics of a food product (shelf life) are both
the conditioning treatments and the packaging. The food is therefore a dynamic systems with a limited shelf life and very specic
demands, in terms of packaging. In many cases the shelf life is
strongly dependent on the resistance offered by the container
walls, through which the gas diffuses and escapes. An effective
package must prevent spoilage, and have gas, temperature, light,
and watervapor barrier properties adequate to retard quality
deterioration of packaged foods. Packaging must withstand processing conditions and distribution abuse (Singh and Singh, 2005).
Common examples of this condition are sparkling mineral
waters, and in general every carbonated drinks. Depending on
the adopted packaging material, anticipation of the carbon dioxide
loss over time through the bottle walls has always been desirable
and challenging at the same time. Several gas diffusion/permeation
mechanisms take place: solubilization/absorption of molecules on
the inner surface of the bottle, diffusion through the polymer and
desorption in the environment (Brooks, 2002; Han and Scanlon,
2005; Piringer and Baner, 2000). In case of a carbonic beverage,
its organoleptic properties are strongly determined by the gas con Corresponding author. Tel.: +39 3293606237; fax: +39 0971 205429.
E-mail address: gianpaolo.ruocco@unibas.it (G. Ruocco).
0260-8774/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jfoodeng.2011.09.001

tent, in such a way that a carbon dioxide reduction of only 15% is

generally enough for the drink to taste at (Swenson, 2002; Lewis
et al., 2003; Profaizer, 2005; Syrett, 2006).
The choice of the packaging material is paramount to preserve
the food features: in particular, the adoption of polythylene terephthalate for beverages helps pursue the food quality and safety
due to its own characteristics, such as barrier to gas and avorings,
transparency and easy processing (Brooks and Giles, 2002). But the
overall planning of packaging is also affected by environmental and
storage conditions, and characteristics of the package (Del Nobile
et al., 1997; Lewis et al., 2003; Chanda and Roy, 2007). In this paper, the storage temperature and package thickness uniformity are
studied, for their effect on the beverage shelf life, by means of a
generally applicable modeling tool. It is seen that a such a tool
may help the developments in polyethylene terephthalate technology and utilization, to satisfy the new demands from the food and
beverage markets.
Del Nobile et al. (1997) have already shown that modeling of a
packaged beverage is important, but their analysis was simplied
to a 1D geometry and limited to the keeping temperature. Instead,
local and transient food features could help establish rmer knowledge grounds, and unfold the dependence on other parameters
such as the bottle design and manufacture. To this end, Computational Fluid Dynamics (CFD) models could help gaining knowledge
on such fundamental and critical processing variables, to describe
the product evolution and help maintain its quality.

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G. Carrieri et al. / Journal of Food Engineering 108 (2012) 570578

Nomenclature
c
D
J
n
s
t
T
V

concentration (mg/l)
mass diffusivity (m2/s)
ow of gas (mol/m2s or kg/m2s)
normal versor
curvilinear coordinate (m)
time (s)
temperature (K)
volume (m3)

Greek
d

thickness (mm)

density (kg/m3)

Subscripts
0
initial
a
air
h
head space
p
package
PET
polyethylene terephthalate
w
water

In this paper, a general CFD tool has been employed for the rst
time to describe the diffusion and loss of CO2 through an actual
polyethylene terephthalate bottle, while experimental measurements have been performed to validate the model and establish
its accuracy. The objectives of the study were to employ a generally
applicable framework of transport phenomena to the assessment
of carbonation depletion and related product shelf life, by exploring the effects of thermal regimes, initial carbonation, and bottle
thickness non-uniformity.

sion caliper (Digital Caliper, Juwell Plus, Italy). The thickness d was
measured at every section as well with a precision micrometer (Mitutoyo, Tokyo, Japan), having cut such sections along the bottle prole by
a cutter (Coupe Bouteilles, Sidel, Luce, France). Bottle deformation due
to internal pressure build-up following polyethylene terephthalate
blowing and bottle carbonation was therefore accounted for. All
lengths and thicknesses are summarized in Table 2 and 3.

2. Experimental set-up and measurements

A rendering of the package is shown in Fig. 1. A pure diffusive

problem of CO2 is assumed to a 2D axial-symmetric model, exploiting the axi-symmetry. When the polyethylene terephthalate
container is stored at a given temperature, after thermal equilibrium

An experimental activity was rst set-up and performed in order to validate the model which will be presented later in the paper. The activity consisted in storing an adequate number of
bottles, containing sparkling water, in a variety of thermal conditions, for the necessary period of time. At given intervals, the permeability of the bottles was assessed by sampling the residual gas
in the stored product. Then the sampled bottles were disposed of.
All bottles were manufactured in polyethylene terephthalate
with a cap in HDPE (High-Density Polyethylene). Gas sampling
and temperature measurements were carried out from six 0.5 l
capacity bottles, at each storage temperature, for water having
an initial carbonation range of 48005400 mg/l, depending on
the particular brand.
The following measurements were carried out at the initial time
and every 15 days:
1. The CO2 concentration measurements were carried out by an
automatic sampler (CarboQC, Anton Paar GmbH, Graz, Austria).
Carbon dioxide measurement is performed by evaluating the
total pressure of all gases dissolved in the sample upon multiple
volume expansions in a sealed chamber tted with absolute
temperature and pressure gases. The precision of the instrument was 0.05 g/l, with the accuracy of 0.01 bar.
2. The temperature was read by means of with a digital thermometer (HI9061, Hanna Instruments, Ronchi di Villafranca, Italy).
The accuracy was 0.4 C.
Bottle tare W was 14.5 or 16.5 g, depending on the particular
brand and blowing procedure, and the product was stored in a
variety of thermal conditions T. All conditions or modes are summarized in Table 1. In particular, the T1 condition corresponded
to local daily and seasonal conditions, in the late-winter/earlyspring period. All other temperature conditions were obtained by
a controlled-temperature storage.
Furthermore, each bottle type was measured to infer on the geometry non-uniformity (height, diameter, and specially the thickness).
Each bottle type was divided in several sections of curvilinear length
Ds and scrutinized, on the lled bottle after carbonation, with a preci-

3. Model formulation

Table 1
Summary of experimental conditions.
Code

Mode

W1
W2
T1
T2
T3
T4

14.5 g, weight of bottle

16.5 g, weight of bottle
variable storage temperature
10.0 C, constant storage temperature
30.0 C, constant storage temperature
40.0 C, constant storage temperature

Table 2
Bottle thickness distribution d along the curvilinear coordinate
s along bottles edge (Fig. 2), for W1 bottle.
Section no.

si  si1 (mm)

d (mm)

1
2
3
4
5
6
7

9.5
1.25
74.7
58.0
50.7
26.9
11.1

1.445
0.135
0.18
0.18
0.19
0.39
1.6

Table 3
Bottle thickness distribution d along the curvilinear coordinate
s along bottles edge (Fig. 2), for W2 bottle.
Section no.

si  si1 (mm)

d (mm)

1
2
3
4
5
6
7

12.3
9.95
76.6
57.0
51.9
26.0
10.0

1.9
0.26
0.23
0.24
0.21
0.36
1.5

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Fig. 1. A rendering of the package under scrutiny, with its dimensions.

with the environment, mass transfer of gas to the outside is established causing the reduction in shelf life. But since the actual package
thickness varies along the bottle height, the mass transfer is nonuniform along its surface.
The actual ll level (liquid/head space interface) is also represented in Fig. 2. Therefore, two domains are congured and analyzed in the model, the V h (head space) and the V w domain
(packed water).
3.1. Assumptions
1. Initially, the gas is distributed uniformly in each domain
(Fig. 2); in V w the gas concentration is set at the desired initial
carbonation, while in V h an atmospheric concentration is
assumed.
2. A diffusive ux through the polyethylene terephthalate matrix
is attributed locally depending on the actual local thickness of
the package (Tables 2 and 3).
3. The diffusion coefcient depends on storage temperature and
polyethylene terephthalate density (determined by the bottle
weight and blowing procedure), only. The adoption of actual
values for these coefcients will be discussed later in Section 4.

Fig. 2. Domains under scrutiny, with indication of the curvilinear coordinate s (not
in scale, Table 2).

4. All cases are computed by assuming the same surface mass

transfer mechanism. The driving mechanism is then the diffusion in the polyethylene terephthalate matrix, and the external
convection is not discussed in this paper.
5. Equilibrium exists at all times between head space and packed
water.
6. In case of variable environmental temperatures, the thermal
uxes are considered to be small enough to ensure that no thermal gradients are formed, then no buoyancy effects are considered in the packaging.
7. No signicant swelling of the polymer occurs when CO2 permeates through the polymer self.
8. The effects of competition on the sorption by other possible
species (e.g. N2 ) are neglected.

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3.2. Governing equations

With reference to the previous statements, the governing equation for the diffusion of CO2 is applied to yield for the gas concentration c in both domains (Bird et al., 2002):

@c
r  Di rc
@t

where i denotes the head space h or the water w, depending on the

subject V h or V w subdomain, respectively.
3.3. Initial and boundary conditions
Initial conditions:
 In the V h subdomain the gas concentration is initially set at the
atmospheric concentration, depending on its partial pressure:

c0 0:03%qa

This concentration is constant at T2, T3 and T4 modes, while it is

variable at T1 mode (due to the inherent thermal oscillation of
the environment).
 In the V w subdomain the gas concentration is due to the given
concentration carbonation level, for the product at hand.
Boundary conditions:
 At bottles cap an insulation condition is applied:

n  Dp rc 0

 At bottles boundaries, an outward ux condition is applied

depending on the diffusion coefcient in the polyethylene terephthalate material and boundary section thickness:

J n  Dp rc

4. Results and discussion

4.1. Diffusion optimization and material properties

 At the subdomain interface V h  V w , the gas ux continuity is

imposed;
 At the symmetry boundary, the proper condition is imposed as
follows:

n  rc 0

Fig. 3. Close-up of adopted grid.

The model requires the denition of the properties of water and

bottles walls, the initial concentration of gas and the diffusive
coefcients. For every storage condition, all constants depend on
storage temperature (Massman, 1998; Singh and Heldman,
2009), even for the T1 mode (Table 1).
3.4. Discretization of domains and run durations
A computational grid, whose close-up is shown in Fig. 3, is
adopted. Both subdomains are discretized by Lagrange-quadratic
elements. Several grids were tried, from a total of 5800 triangular
elements up to more than 18,000. The nal grid, yielding for gridindependency results, had some 10,000 elements, and more than
37,000 degrees of freedom.
The UMFPACK direct solver is used. The BDF method for time
dependent problems is used for the time stepping setting. The time
step is taken by the solver itself in free mode. The run was executed for a total period of 7 months, taking less than a minute on
a Supermicro PC carrying a Xeon (3 GHz) CPU, under Windows XP.

It is acknowledged in this work that the diffusion coefcient

plays an important role, as the process at hand is diffusion-driven.
In order to allow preventive model validation, the integration of
the governing Eq. (1) has been complemented by using the design
environment modeFRONTIER (modeFRONTIER, 2008) in which a
SIMPLEX (Edgar et al., 2001) multi-object optimization routine is
exploited to form the desired diffusion coefcient value. Practically, n design constraints can be analyzed by calculating the following error function f x; e:

f x; e x0  e0 2 x1  e1 2 x2  e2 2 . . . xn  en 2

with xi the i-th constraint variable (the calculated carbonic concentration) and ei the corresponding i-th experimental validating datum. In the present case, n = 15. By this routine, the CFD kernel
(COMSOL Multiphysics Users Guide, 2008) is iteratively run, until
convergence for a minimized error function f.
With this procedure, the optimal Dp value has been found for
each constant temperature and bottle weight modes.

Table 4
Diffusion coefcients of CO2 in package, air and water (m2/s) employed, for the
constant temperature modes.
Mode

Dp at W1

Dp at W2

Dh

Dw

T2
T3
T4

4.32  1014
2.51 1013
4.3  013

3.71  1014
2.16  1013
3.39  1013

1.47  105
1.667  105
1.768  105

1.44  109
2.16  109
2.52  109

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G. Carrieri et al. / Journal of Food Engineering 108 (2012) 570578

As proposed for example by Del Nobile et al., 1997, Dp varies

with temperature. Therefore, for the variable temperature T1
mode, based on the above optimized values, a tting polynomial
was found, with the coefcients of Dp aT 2 bT c determined
by means of Matlab (MATLAB, 2009). For W1 we found:

Dp 0:0025  1013 T 2 0:0038  1013 T 0:1440  1013

while for W2 we assumed, for the same temperatures but varying

with bottle weight:
13 2

Dp 0:0021  10

13

T 0:0047  10

13

T 0:1120  10

The employed diffusion coefcients for package, air and water

are summarized in Table 4. Dp values are consistent with those reported in the available literature (e.g. in Lewis et al., 2003 and
McGonigle et al., 2001), considered that Dp is generally inuenced
by the crystallinity degree upon bottle formation also.
4.2. Comparison of computations with experiments
In order to validate the model, preliminary measurements were
performed for W1T1 and W2T1 bottles (Figs. 4 and 5), and then
compared with the corresponding simulations. It is shown that

Fig. 4. Comparison between experimental data and predicted data for W1T1.

Fig. 5. Comparison between experimental data and predicted data for W2T1.

G. Carrieri et al. / Journal of Food Engineering 108 (2012) 570578

the comparison with the experiments holds well enough, even

with the variable storage temperature. The computations slightly
overestimates the loss history for the lighter W1 bottle, while for
the heavier W2 bottle the optimized diffusivity yields a certain
underestimation, its maximum value being some 23% at the nal
storage time of 210 days. The experiments also show that there
is no appreciable effect on the carbonic loss due to the bulk weight
W1 or W2. In both cases, however, the average CO2 reduction ranges
from 5300 mg/l to about 2700 mg/l (almost 50%) after the entire
storage period.
Then modelling was also conducted and validated for the W1
T3, W2T3, W1T2 and W1T4 bottles (Figs. 69). At all mode com-

575

binations, it is conrmed that the model is fairly able to simulate

the evolution at stake.
A rst interesting issue is the yield obtained by a given initial
carbonic content. For example, the W1T3 (Fig. 6) bottle has a
slightly higher initial concentration (5100 mg/l) that the W2T3
(Fig. 7) one (4860 mg/l): nevertheless, in the former case the nal
concentration is only about 1000 mg/l while in the latter it reaches
almost 1300 mg/l. In other words, a mere 5% decrement in the initial concentration helps extend the shelf life by 45 days. This difference cannot be attributed to the bottle weight, as speculated
above, but to a higher driving force (the concentration gradient
with the environment) that induces a greater carbonic depletion.

Fig. 6. Comparison between experimental data and predicted data for W1T3.

Fig. 7. Comparison between experimental data and predicted data for W2T3.

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G. Carrieri et al. / Journal of Food Engineering 108 (2012) 570578

Fig. 8. Comparison between experimental data and predicted data for W1T2.

Fig. 9. Comparison between experimental data and predicted data for W1T4.

A second evident effect is the increment of carbonic loss with

temperature, as expected. It is indeed instructive to compare, for
a given bottle weight, the concentration history with varying temperature mode: that is, the variable temperature W1T1 (Fig. 4)
with the one kept at constant temperature W1T3 (Fig. 6), and similarly the W2T1 results (Fig. 5) with the W2T3 ones (Fig. 7). It is
evident that at the warm T3 temperature the carbonic loss is much
higher: after 150 days, for example, the W1T3 (Fig. 6) and W2T3
(Fig. 7) bottles loose about 2000 mg/l (some 50%) more than the
corresponding variable temperature storage W1T1 (Fig. 4) and

W2T1 (Fig. 5). At the same storage time, the loss is even higher
and up to 3000 mg/l (almost 83%) when comparing the cold temperature W1T2 case (Fig. 8) with the hotter one W1T4 (Fig. 9).
Finally, it can be observed that the computed concentration history at the warmer T3 and T4 modes (Figs. 6, 7 and 9) are nicely
superimposed with the corresponding experimental progress. Instead, at the beginning of the T1 and T2 modes (Figs. 4, 5 and 8),
when the storage temperature is low, a discrepancy of maximum
10% is found with measurements. It is speculated that in these conditions the model cannot compensate with the additional retention

G. Carrieri et al. / Journal of Food Engineering 108 (2012) 570578

577

Fig. 10. Local evolution of carbonic concentration, ranging from 1.26 to 108 mol/m3, at W1T2 modes and for six times: from left to right, at t = 0 (bottling), and at day 1, 15,
30, 90 and 210, respectively.

Fig. 11. Local carbonic concentration, ranging from 1.26 to 108 mol/m3, at W1 mode, after 15 and 210 days: for T2 (rst and second from left) and T4 (third and fourth from
left) modes, with indication of intensity and direction of diffusive ux.

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effect by the water, as CO2 features a higher solubility at low temperatures (Steen, 2006), and therefore is poorly available to transfer through polyethylene terephthalate.
4.3. Maps of carbonation evolution
In Fig. 10 the local evolution of carbonic concentration, at W1
T2 modes and for several times is shown. A similar evolution is
found for all other explored modes. It is evident that an equilibrium is soon reached between the head space and the water (which
is evident comparing the rst two maps from left in Fig. 10). The
concentration gradient disappears completely after 3 months. At
the end of the observed storage period, the polyethylene terephthalate bottle will lose about 35% of its initial carbonation.
Finally, in Fig. 11 the effect of storage temperature on the local
concentration is inspected, for the W1 bottle at the T2 and T4
modes. From the beginning of the process (15 days), a warmer
T4 storage yields for a greater carbonic loss (third map from left)
with respect to the a cooler T2 condition (rst map from left).
The uneven pattern of ux arrows (in their intensity and direction)
also evidences that the polyethylene terephthalate thickness distributions (Table 2) and arrangement diffusivities (Table 4), makes
the carbonic loss non-uniform along the bottle height. The net carbonic loss is then accelerated at the end of the period (210 days)
for T4 (last map), rather than with T2 (second map from left), conrming what speculated earlier when examining Figs. 8 and 9.

5. Conclusions
In this work a model of shelf life of carbonated drinks has been
proposed and validated by experimental results. The model takes
into consideration the weight of bottle and storage temperature,
allowing for a good agreement with the explored two parameters.
The carbonation decrement does not appear to depend on bottle
weight, although diffusive non-uniformity is observed depending
on polyethylene terephthalate thickness distribution, given by
the bottle manufacture. An adequate initial carbonation favors
the extension of shelf life up to 20%, in the explored case. The
importance of a controlled storage temperature is conrmed, as
the diffusion of gas through polyethylene terephthalate is accelerated with temperature: a fourfold increase of temperature from
10 C yields a 83% higher gas loss.
The model created in this work can be used as a design and verication tool for predicting shelf life in any carbonic beverage, and
can be easily supplemented with the dependence on lling level
among other product and storage parameters. Its results can be
employed to rapidly establish the best used by date variation,
depending of some manufacturing practice change, so that the desired features can be ensured.

Author contributions
G.C. conceived the study that was then designed by G.R. in conjunction with M.V.D.B. G.C. carried out the experiments. All
authors participated in developing the model. G.C. carried out the
computations, set up the model validation and wrote the rst draft
of the manuscript. G.C. and M.V.D.B. participated in manuscript
revisions and discussion, coordinated and critiqued by G.R.
Acknowledgments
The authors gratefully acknowledge Dr. A. Libutti and Dr. A.V.
Lotito of Fonti del Vulture S.r.l., in Rionero in Vulture (Italy).
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