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By Iosif-Daniel Rosca, micro-organisms. Plastics are also able true that poly-olefins produce
Jean-Maurice Vergnaud to reduce the loss of components such energy in burning, but it does not
as water or flavour in the packed mate- work well for PVC.
rial to a great extent. Resulting from (ii) The other way consists of reusing
INTRODUCTION this protection, plastic packages them as new packages. However, it
enable the consumer to use foodstuffs should not be ignored that very
Before 1950, food was sold mainly in nearly perfect hygienic conditions, often the old cans or bottles made
from bulk containers, the packaging and to store them without loss in qual- of plastics are commonly used to
done by the retailer after selling. For ity over an extended period of time. keep other liquids such as chemi-
example, milk was taken from a large But it is also true that plastics contain cals potentially dangerous for
milk can by a soup-ladle to be dropped low-molecular weight compounds such health. And in the same manner
in the milk-jug of the consumer. Pre- as oligomers and sometimes mono- as the additives initially in the vir-
packaging was developed in the mid mers, and additives such as plasticizers, gin polymer may migrate into the
1900s with the production of sealable lubricants, stabilizers and antioxidants, food, these chemicals may deeply
glass bottles and airtight metal cans. which are absolutely necessary either diffuse into the old polymeric
Later on, flexible materials, such as for the processing or the stability of the package, and washing even with
cellophane, were introduced instead final polymeric materials. The draw- boiling water is not able to extract
of grease-proof paper. Today, since back that results is the possible migra- them. Thus, we have to deal with a
they exhibit outstanding food protec- tion of these additives from the package potentially polluted material. And
tion properties such as air-tightness into the packaged material, leading to a finally, the only way to resolve the
and durability, plastics are used prefer- potential ingestion problem of major problem is to build new packages
entially for packaging foodstuffs. concern. For this reason, a list of non- consisting of two layers, the one
It is true that plastic packages are authorised additives has been drawn made of the recycled polymer,
capable of retarding and sometimes under the guidance of the European while the other made of virgin
preventing detrimental changes in Community (EEC) and the United polymer that will be put in contact
the packed material due to external States Food and Drug Administration with the food.
influences such as oxygen, light, and (FDA, Washington, DC, USA).
Moreover, as the use of plastic
packages is now widely spread over And following this way, as these
Iosif-Daniel Rosca is affiliated with all countries, a large amount of old multi-layer packages are obtained by
Department of Polymer Chemistry, packages is disseminated in the gar- co-extrusion or co-moulding for bot-
Polytechnic University, Bucharest, bage heaps. Thus the problem appears tles, at a temperature at which the
Romania. with the question: what to do with polymers are melted, an additional
these old plastics of various kinds? A transfer (by diffusion or perhaps by
Jean-Maurice Vergnaud is affiliated few ways are already explored, waiting convection) takes place between the
with University of St-Etienne, Route to be widely used: recycled and the virgin polymer layers.
de Chavanne, 42400 Saint-Chamond, At that time of the studies, heat transfer
France (Tel.: 4 77 31 86 73; has to be looked upon, and the effect of
fax: 4 77 31 86 73; e-mail: vergnaud. (i) One way consists of burning them the temperature-dependency of the
jean-maurice@wanadoo.fr). in the same way as crude oil; it is diffusivity estimated.1
14 ß Division of Chemical Health and Safety of the American Chemical Society 1871-5532/$32.00
Elsevier Inc. All rights reserved. doi:10.1016/j.jchas.2006.08.006
The process of material transfer from of the parameters of interest, especially where the concentration of the diffus-
the package into the food can be gen- the diffusivity and the coefficient of ing substance C depends on the time, t
erally described by either transient convection on this rate of transfer, as and distance, x.1,13
Fickian diffusion through the package well as the ratio of the volumes of At the packaging–liquid interface,
or convection in the liquid food as well liquid and packaging, is evaluated. the rate at which the substance is trans-
as at the solid–liquid (that is, package– Some results are given in the case of ferred into the liquid is constantly
food) interface; the process of transfer is a single layer package by studying the equal to the rate at which this sub-
controlled only by diffusion through the effect of the thickness of the package as stance is brought to the surface by
solid food. Various attempts have pre- well as that of the rate of stirring of the internal diffusion through the polymer
viously been made by assuming that the liquid, which acts upon the coefficient packaging, leading to the relation:
rate of convection at the solid–liquid of convective transfer. In all cases, the @C
interface is infinite, leading to the fact results are expressed in terms of pro- D ¼ hðC L;t C eq Þ (2)
@x
that the concentration of the material files of concentration of the diffusing
on the solid surface falls instanta- substance developed through the where h is the coefficient of transfer by
neously to the value at equilibrium as thickness of the package and of the convection in the liquid next to the
soon as it is in contact with the liquid, kinetics of transfer of this substance surface, CL,t the concentration of the
e.g., 0 when this liquid is initially pure.2 in the liquid.5,6 Dimensionless num- diffusing substance on the surface of
Other attempts have been made by con- bers are used, as often as it was possible the solid at time t, and Ceq is the con-
sidering the thickness of the package as so as to build general curves called centration of the diffusing substance
semi-infinite,3 essentially because this master curves, which can be used in on this surface required to maintain
assumption leads to a very simple equa- various different cases. equilibrium with the concentration of
tion. The values of the diffusivity found The problem of a bi-layer system this substance in the liquid, at time t.
in the literature collected from experi- where the package consists of the layer The value of the coefficient of con-
ments made by various authors whose made of the recycled polymer bound to vection, h, largely depends on the type
operational conditions were either dif- the virgin polymer layer is also exam- of convection; being rather low in
ferent or not clearly defined, are lying ined. This virgin layer being placed in motionless liquid, it increases notably
within a very large range.4 Thus the contact with the food plays the role of a with the rate of stirring of the liquid up
values of the diffusivity obtained for functional barrier. The effect of the to a very large value when the liquid is
the additives in Low Density Polyethy- various parameters is determined, strongly stirred.
lene (LDPE), differ from one to another without forgetting the effect of the Finally, both the Eq. (1) expressing
by not less than 100. As the time neces- mass transfer taking place between the variation of the concentrations
sary for a given transport is inversely these two layers during the stage of with time and space in the polymer
proportional to the diffusivity, it means co-extrusion.1,7–9 and the Eq. (2) defining the so-called
that the time for contamination should The function of the active packages boundary condition, are the funda-
also vary by 100 times, e.g., from 10 days is shortly considered, when the pack- mental equations of diffusion through
to 3 years. age is able to release an antibacterial a sheet of an isotropic material. There
Fortunately, at the present time, the agent,10,11 and an example of kinetics are the basic equations for calculation
theoretical treatment of the process of is given.12 of the kinetics of the transfer of a pol-
mass transfer controlled by diffusion– Finally, an attempt is made in order lutant from the polymer in the liquid,
convection with liquid food or even by to describe the operational conditions as well as of the profiles of concentra-
diffusion–diffusion when the food is necessary for predicting a standardised tion of this pollutant developed
solid is precisely described.1 Emphasis test and apparatus, which should be through the thickness of the package.
has been placed on the fact that an used by everybody working in the field Eq. (1) is a partial derivative equation,
infinite rate of convection cannot exist of food pollution. On the other hand, since the concentration C depends on
at the package–liquid interface, and the best equation leading to the safer the two parameters of time and space.
consequently we have to deal with results is drawn so that the results of
more complex equations. The question these experiments could be expressed Finite Coefficient of Convection h at the
of the volume of the package as a in valuable data.1 Solid–Liquid Interfaces and Infinite
Volume of Liquid
fraction of the volume of the liquid is
also considered. In fact, the problems The initial condition given by a uni-
of diffusion are not simple to resolve, THEORETICAL
form concentration of the diffusing
either by considering the experiments substance through the polymer thick-
or by making calculation. When the diffusivity D is constant, ness is expressed by the Eq. (3):
The purpose of this paper is to being independent of the concentra- t ¼ 0; L < x < þ L; C ¼ C in
describe precisely the process of trans- tion, the equation of transient diffusion sheet (3)
fer of the diffusing substance from the is written as follows:
polymer packaging into the liquid The solution of this problem with the
@C @2 C
food, and to present the various equa- ¼D 2 (1) above initial and boundary conditions
tions, which are widely used. The effect @t @x is given for the profiles of concentra-