Professional Documents
Culture Documents
DOI 10.1007/s11947-013-1106-8
REVIEW
Received: 16 February 2013 / Accepted: 1 April 2013 / Published online: 18 April 2013
# Springer Science+Business Media New York 2013
Abbreviations
AC
Acrylonitrile
AG
Alcoholic grade
Al
Aluminum
BADGE Bisphenol A diglycidyl-ether
DEHP
Ethylhexyl phthalate
ESBO
Epoxidised soybean oil
FS
Food simulants
GC
Gas chromatography
GC-MS Gas chromatographymass spectroscopy
IR
Spectroscopy
LC
Liquid chromatography
LC-MS Liquid chromatographymass
spectroscopy
LDPE
Low-density polyethylene
OM
Overall migration
PET
Polyethylene teraphthalate
PO
Polyolefin
PS
Polystyrene
PVC
Polyvinyl chloride
PVdC
Polyvinylidene chloride
SM
Specific migration
Nowadays, packaging is applied on a huge variety of products. The protection of goods during all stages of the supply
chain is mainly based on packaging (Brody et al. 2008).
According to Robertson (2006) without packaging, materials handling would be a messy, inefficient and costly
exercise and modern consumer marketing would be virtually important.
22
Migration
Migration Mechanism
The migration of substances from packages into foodstuffs
is characterised by high complexity. Diffusion is mainly
responsible for this type of migration, i.e. the macroscopic
movement of molecular structures from higher to lower
concentrations, while adsorption can be another way of
leading to this type of migration (Simoneau 2008).
Diffusion is the mass transfer due to random movement of
molecules from regions of high concentration to regions of
low concentration until equilibrium is reached (Miltz et al.
1997). The diffusion rate is expressed mathematically with the
following equation known as the second law of Fick:
@Cp =@t D @ 2 Cp =@x2
23
24
Plasticisers
Light stabilisers find many applications in improving the longterm weathering properties of plastic polymers such as polyolefins. Polymeric hindered amines, (e.g. Tunuvin 622 and
Chimasorb 944) are widely applied in polyolefins as light
A plasticiser is defined as a substance which after incorporation into a material (usually a plastic or elastomer) can
make it more flexible and facilitate its processing. Most
plasticisers belong to the group of esters of phthalic acid
(phthalates) and adipic acid. The di-2-ethylhexyl phthalate,
the dioctyl phthalate and the di-2-ethylhexyl adipate are
systematically applied (Rahman and Brazel 2004).
Figure 2 diagrammatically represents the migration route
of di-n-octyl phthalate into Semolina powder and a solidfood simulant. Many studies report that plasticisers can act as
migrants and can be transported from packages to foods (Biles
et al. 1997; Castle et al. 1988a; Castle et al. 1988b; Castle et al.
1988c; Castle et al. 1988d; Castle et al. 1988e; Castle et al.
1988f; Castle et al. 1990a; Castle et al. 1990b; Castle et al.
1993; Losada et al. 1997; Macias-Matos et al. 1990; Page and
Lacroix 1995; Startin et al. 1987). According to Pedersen et al.
(2008): phthalates are used in cap-sealing resins and sealing
gaskets of bottled food, PVC films and some plastic packaging. Phthalates used as plasticisers for polymers are
Plastic Packaging
stabilisers (Lee et al. 2008; Careri et al. 2002). An ultraperformance liquid chromatography (UPLC) with ultraviolet
spectrophotometry detection system (UPLC-UV-visible) was
used by Noguerol-Cal et al. (2010) for the determination of
the light stabilisers Chimassorb 944 and Tinuvin 770. The
method provided quite reliable results offering a chance for
the development of an effective tool for verifying compliance
with legal limits.
Antioxidants
Exposing polymers to UV light and air can lead to significant degradation of the materials due to oxidation reactions.
Antioxidants can be used to reduce the rate of oxidation and
enhance the stabilisation of the material of interest, through
degrading themselves. Tinuvin P, Tinuvin 326, Tinuvin 776
DF, Tinuvin 234, Chimasorb 81, Irganox 1076, Irganox
1330, Irganox 1010, Irganox168 and Irganox P-EPQ are
included among the most widely known chemical antioxidant substances (Lau and Wong 2000). The most significant
natural antioxidants that are either contained or subsequently added to foods are substances such as: tocopherols and
tocotrienols (vitamin E) ascorbate (vitamin C), vitamin A
and carotenoids (-carotene, lycopene, lutein etc.), Se (and a
variety of other metals which are considered to play a key role
for the action of antioxidant enzymes), phytochemicals with
antioxidant activity, dietary and other supplements (CoQ10,
glutathione, lipoic acid etc.) and food antioxidants such as
butylated hydroxyanisole, butylated hydroxytoluene, propyl
gallate and tertiary butylhydroquinone (Papas 1999). Figure 3
presents the migration kinetics of Irganox 1076 from LDPE
into a food simulant and meat.
Solvents
During printing plastic packages, the inks are used in the
form of dissolutions or dispersions in solvents, which can
afterwards evaporated or removed by penetration, distillation and contact usually in specific types of ovens (Boon
2008). However, it is possible that a quantity of residual
solvent remains. The solvents most usually used are low
molecular weight, organic substances composed of hydrocarbons, alcohols, glycol ethers, ketones and esters, which
may present migration into foods by directly contacting
them or through the free space in the interior of the package.
The quantity of solvents entering a food product is highly
dependent on portioning of the solvent between the package
materials and the food (Robertson 2006).
25
Fig. 3 Migration over time of Irganox 1076 from LDPE into Tenax
(at 23 C) (Reinas et al. 2012) and pork minced meat (at 25 C) (Beld
et al. 2012)
26
Metal Packaging
Tin
Tin is currently found in low quantities in a variety of
canned foods and beverages, especially in foodstuffs packaged in unlacquered or partially lacquered tinplate cans.
Although some case reports of acute gastrointestinal disorders after consuming foods with a level of 100500 mg kg1
tin have been published (Benoy et al. 1971; Omori et al.
1973), these studies present several insufficiencies.
Controlled clinically performed experiments on acute effects of tin ingested after migration from packages indicate
that there is a threshold concentration for adverse effects
(AEs) of >730 mg kg1 (Boogaard et al. 2003). The tin layer
adheres significant protection against corrosion and in many
cases coating is not used since tin can act as an effective
oxygen scavenger. Nevertheless, the use of coating is usually applied since uncoated tin can lead to the occurrence of
numerous interactions between the metal surfaces (Oldring
and Nehring 2007).
27
Lead
Despite its toxicity, lead is often used in metal packages.
It was shown that lead is one of the most important
contaminants derived from packaging materials. The
highly toxic effects of lead, and specifically of organolead species (such as neonate) can significantly affect the
central nervous system. It is often supported that infants
are much more susceptible to the toxic effects of lead in
comparison to adults, with a higher percentage of lead
being retained to bones and brain of infants. Subacute
ingestion of lead by children can lead to encephalopathy,
convulsions and mental retardation (Robertson 2006;
Skrzydlewska et al. 2003).
Aluminum
According to Elinder and Sjgren (1986), aluminum (Al)
is commonly used in food contact materials. Different
elements such as Mg, Fe, Si, Mn, Cu and Zn can be found
in Al alloys used in contact with foods (European
Committee or Standardisation CEN 2004a; European
Committee or Standardisation CEN 2004b). Al is detected
at low quantities in numerous plants and animals despite
the fact that it is the most abundant and widely distributed
metal, constituting 8.4 % of the Earths crust (Taylor
1964). However, it is important to mention that Al does
not constitute part of any known animal metabolism, in
contrast to a vast number of less widely distributed metals
involved in enzymes and other metabolic processes. High
intake and increased tissue amounts of this metal have
been connected to numerous disorders, such as dialysis
encephalopathy, osteodystrophy and microcytic anemia.
Apart from the unavoidable daily intake of Al via food,
exposure to Al can occur due to migration from cooking
utensils, storage containers and packages. Due to this fact,
pure Al is not used for the manufacturing of food-contact
packages and a certain amount of alloying elements, such
as Fe, Cu, Zn, Mn and Cr, may be added. However, all
these elements plus the Al can be found into foods if
corrosion occurs (Robertson 2006; Rodushkin and
Magnusson 2005).
Chromium
According to Kim et al. (2008), passivation is a Cr treatment
widely applied to make the tin layer in tinplate cans less
susceptible to oxidation damage and improve the enamel
adherence. Chromium is characterised by relative toxicity
and undesired organoleptic properties and according to
Skrzydlewska et al. (2003), its presence as Cr(VI) can have
severe effects on living organisms since it is known as both
carcinogenic and mutagenic.
28
29
Migration Testing
Determination methods of migrating compounds from packaging materials to foods greatly depend on the extraction
capability of the under study compound. This property can
be quantitatively determined by exposing the packaging
material in contact with food for specific time and temperature and determination of migrating compound to food
(Arvanitoyannis and Stratakos 2011). However, the determination of migration under real conditions is quite difficult.
It is because of this reason that in most cases simulation of
migration conditions takes place. For example, for a food of
lengthy preservation the migration studies are carried out for
lesser time at higher temperature. Furthermore, standard
compounds known as food simulants are used (instead of
foods) for facilitating the investigations (Stoffers 2005).
Food Simulants
Due to the extremely complex chemical and physical structure of foods, migration tests are usually performed using
FSs. The latter are either liquid or solid substances that have
a simple and known composition making tests easier and
better interpreted. A variety of different FSs have been
used from time to time and some of them are now
official simulants indicated by mandatory regulations
(Lee et al. 2008).
According to EU Directive 85/572 and Grob (2008), the
above-mentioned FS are classified based on the assumption
that they have similar properties to those of one or more
categories of foods. Although the FS are distinguished in
several categories (see the following paragraphs) there are
foods which are mixtures of fatty and aqueous foods.
Water
The use of water is common for aqueous foods with a
pH higher than 4.5. This group of foods includes nonalcoholic beverages or alcoholic beverages of an alcoholic strength lower than 5 % vol. such us water, ciders
fruit or vegetable juices of normal strength or concentrated, musts, fruit nectars, lemonades and mineral waters, syrups, bitters, infusions, coffee, tea, liquid
chocolate, beers, pastry, cakes and other bakers fresh
wares, moist, honey, molasses and sugar syrups, fruits
after processing, vegetables as purees, fish, crustaceans,
molluscs, meat, processed meat foods, cheeses, ice
creams, eggs and many products in aquatic medium.
Acetic Acid
A 3 % concentration of acetic acid solution in water
is commonly used for acidic aqueous foods (pH below
4.5) such as vinegar and non-alcoholic beverages or
alcoholic beverages of an alcoholic strength lower than
5 % vol. such us yoghurt, buttermilk and similar foods
with or without fruit and fruit products.
Ethanol
Ten percent aqueous ethanol is commonly applied
for the production of alcoholic products. The concentration of the solution is adapted to the alcoholic grade
(AG) of the food provided the AG exceeds 10 %v/v. As
an example the aqueous ethanol can be used to simulate
alcoholic beverages of an alcoholic strength equal to or
higher than 5 % vol (winers, spirits, liqueurs etc.).
Oil
Olive oil and other oils, such us sunflower oil
and synthetic mixtures of triglycerides are commonly used for the production of fatty foods. Animaland vegetable-derived fats and oils, many kids of
sauces (mayonnaise, mustard), milk, processed meat
products and products in oily medium are grouped
in this category.
The most recent EU regulation 10/2011 for packaging materials made of plastic refers to three categories of FS, except for water and addition of
different concentrations of ethanolic solution.
Acetic acid (3 %v/v)
Ethanol (10, 20 and 50 %v/v)
Vegetable oil
30
t5 min
5 min<t1/2 h
T5 C
5 C<T20 C
20 C<T40 C
40 C<T70 C
70 C<T100 C
100 C<T121 C
1/2 h<t1 h
T5 C
5 C<T20 C
20 C<T40 C
40 C<T70 C
70 C<T100 C
100 C<T121 C
1 h<t2 h
T5 C
5 C<T20 C
20 C<T40 C
40 C<T70 C
70 C<T100 C
100 C<T121 C
2 h<t24 h
T5
C5 C<T40 C
T>40 C
t>24 h
T5 C
5 C<T40 C
T>40 C
Legislation
Initially, the commission established a general framework
directive for determining the key requirements that should
be met for all materials and articles, as well as prerequisites
and processes that should be taken into account when drafting
certain directives, such as directives related to specific groups
of materials (e.g. plastics, ceramics etc.) or specific substances
(e.g. vinyl chloride). The framework Directive 76/893/EEC of
26 November 1976 (since superseded by 89/109/EEC of 21
December 1988) set up two general principles. The one is the
principle of the inertness of the material and the purity of
the food, and the second is the positive labelling.
100 C
Depend on the simulant, in accordance
with Directive 82/711/EEC
24 h at 5 C
24 h at 5 C
Conditions adjusted by national regulations
10 days at 5 C
10 days at 40 C
Conditions adjusted by national regulations
The management of migration presents the same problems and is a matter of the same principles like those applied
in accordance with ISO 9001:2008 for the continuous improvement of food products. Figure 4 diagrammatically presents the basic interactions between all factors involved in
the commercial development of foods.
Specific Migration Testing
Determination of specific migration is carried out by measuring every time the migration of a specific chemical
31
simulations should be maintained below specific limits identified in the positive list. Directive 85/572/EC includes all
simulants that can be applied for migration simulations as
well as a table of correlations between food categories and
their food-simulating liquids.
Subject
10/2011
Regulation on plastic materials and articles intended to come into contact with food.
76/893/EEC Relating to plastics materials and articles intended to come into contact with foodstuffs.
78/142/EEC Approximation of the laws of Member States relating to materials and articles contain vinyl chloride monomer and are intended to come into
contact with foodstuffs.
80/590/EEC Determining the symbol that may accompany materials and articles intended to come into contact with foodstuffs.
80/766/EEC Community method of analysis for the official control of the vinyl chloride monomer level in materials and articles which are intended to come
into contact with foodstuffs.
81/432/EEC Community method of analysis for official control of vinyl chloride released by materials and articles into foodstuffs.
82/711/EEC Basic rules necessary for testing migration of the constituents of plastics materials and articles intended to come into contact with foodstuffs.
84/500/EC Approximation of the laws of Member States relating to ceramic articles intended to come into contact with foodstuffs.
85/572/EEC List of simulants to be used for migration of constituents of plastic materials and articles intended to come into contact with foodstuffs.
89/109/EEC Approximation of the laws of the Member States related to materials and articles intended to come into contact with foodstuffs.
90/128/EEC Relating to plastic materials and articles intended to come into contact with foodstuffs.
92/39/EEC Amending Directive 90/128/EEC relating to plastics materials and articles intended to come into contact with foodstuffs.
93/8/EEC
Amending Council Directive 82/711/EEC laying down the basic rules necessary for testing migration of constituents of plastics materials and articles
intended to come into contact with foodstuffs.
93/9/EEC
Amending Directive 90/128/EEC relating to plastics materials and articles intended to come into contact with foodstuffs.
93/10/EEC Relating to materials and articles made of regenerated cellulose film intended to come into contact with foodstuffs.
93/11/EEC Concerning the release of the N-nitrosamines and N-nitrosatable substance from elastomer or rubber teats and soothers.
95/3/EEC
Amending Directive 90/128/EEC relating to plastics materials and articles intended to come into contact with foodstuffs.
96/11/EEC Amending Directive 90/128/EEC relating to plastic materials and articles intended to come into contact with foodstuffs.
97/48/EEC Amending for the second time Council Directive 82/711/EEC laying down the basic rules necessary for testing migration of the constituents
of plastics materials and articles intended to come into contact with foodstuffs.
2002/72/
Relating to plastic materials and articles intended to come into contact with foodstuffs.
EEC
1935/2004 Regulation on materials and articles intended to come into contact with food and repealing Directive 80/590/EEC and 89/109/EEC.
1895/2005 Regulation on the restriction of use of certain epoxy derivatives in materials and articles intended to come into contact with food.
2023/2006 Regulation on good manufacturing practice for materials and articles intended to come into contact with food.
2007/42/
Relating to materials and articles made of regenerated cellulose film intended to come into contact with foodstuffs.
EC
282/2008
Regulation on recycled plastic materials and articles intended to come into contact with foods and amending Regulation (EC) No. 2023/2006.
450/2009
Regulation on active and intelligent materials intended to come into contact with food.
EEC
Directives
Recycled plastic
Active and intelligent
materials
Plastics
All materials
All materials
All materials
Regenerated cellulose
Plastics
Plastics
Regenerated cellulose
Elastomers
Plastics
Plastics
Plastics
Plastics
Plastics
Ceramics
Plastics
All materials
Plastics
Plastics
Plastics
All materials
Plastics
Plastic materials
Plastics
Material
32
Food Bioprocess Technol (2014) 7:2136
Conclusions
The migration phenomenon is of high importance nowadays
especially due to the continuously increasing requirements
of consumers for safer products, and the establishment of
international regulations to meet these requirements.
Migration in both directions (from packaging to food and
conversely) can affect both the organoleptic characteristics
(quality) and the safety of products. This complex process
can be affected by several factors such as the nature of the
food, the packaging material, time and temperature conditions etc. Migration can be affected by the characteristics of
both the package and the contained food, while the characteristics and the nature of the migrant itself can significantly
affect the migration route.
The food simulants are extensively used for examining
the migration phenomenon, mainly due to the high variety
of food products that need to be examined. A variety of food
simulants have been applied for testing the migration phenomenon. The international legislation defines specific
simulants that can be used under certain time-temperature
conditions for the conduction of migration testing.
The extreme variety of potential migrants indicates the
need for establishment of not only internationally recognised
testing tools, but also appropriate risk management procedures (better identification of potential consumers and establishment of maximum permitted limits, assessment of safety
for all potential migrants etc.).
33
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