ANTIMICROBIAL POLYMERS

Spectrum of pathogenic microorganisms, thermally stable during polymer processing, does not alter
the quality of the product by providing odor or taste, and cost effective. Different chemicals such as
organic and inorganic acids, chlorine dioxide, silver ions and nanoparticles, zinc oxide, magnesium
oxide, chitosan, alcohols, ammonium compounds, or amines have been successfully incorporated
as antimicrobial substances into plastic materials. However, the current trend nowadays is the
preference for natural over synthetic chemistries; therefore, much attention is being paid to the use
of bacterial starter cultures, bio preservatives, and plant extracts as antimicrobial hurdles as they
present a perceived lower risk to the consumers. The bio preservatives suggested as antimicrobials
include bacteriocins such as nisin and pediocin and antimicrobial enzymes such as lysozyme,
lactoperoxidase, chitinase, and glucose oxidase

Chlorine dioxide received FDA acceptance as a packaging material antimicrobial agent. It is an

antimicrobial gas released from a basic chlorine-containing chemical upon exposure to moisture. Its
main advantage is that it functions away from the plastic, and thus, it is one of the few packaging
antimicrobials that do not require direct contact with the food. Other possible antimicrobial
substances are food preservatives such as sorbates, benzoates, propionates, and parabens, all of
them covered by FDA regulations. Sorbate-releasing plastic films are a good example of successful
research and development of antimicrobial packaging. Films containing sodium propionate have
also been proved useful in prolonging the shelf life of bread by retarding microbial growth.

ENGINEERING PROPERTIES OF POLYMERIC-BASED ANTIMICROBIAL FILMS FOR FOOD PACKAGING

Wide ranges of antimicrobial substances have been tested in laboratories for their potential
applications in the antimicrobial food packaging. These substances include organic acids (benzoic
acid, sorbates), enzymes (lysozyme, glucose oxidase), bacteriocins (nisin, pediocin), fungicides,
polymers (predominantly chitosan), natural extracts, antibiotics, triclosan, and silver compounds.
Food-packaging films with antimicrobial activity can be divided into two groups: films that allow the
antimicrobial to migrate into the food films that do not release antimicrobial substances and that
inhibit microbial growth on the food surface.

Few biopolymers, which are produced by chemical synthesis from bio-derived monomers, have
been used in the production of antimicrobial films. Synthetic polymers that have been used to
develop antimicrobial food packaging films include PE, PP, PS, EVA, PVC, PA, and PBAT. PLA is
synthesized from bio-derived monomers and can be applied as film for antimicrobial food
packaging. The Tg, Tm, and crystallization temperature (Tc) are important thermal properties
related to polymers used for food packaging, since they suggest the level of association between
polymeric chains. These properties are also important for characterizing plastics for their use in food
packaging and provide important information about some criteria that must be taken into account
during processing. Differential scanning calorimetric (DSC) is used to determine the thermal
parameters of a polymer and characterize the crystallization mechanism of semicrystalline
polymers. The degree of crystallinity (v) is an important physical parameter that relates to the
morphology and mechanical properties of the polymer.
ANTIMICROBIAL SUBSTANCES FOR FOOD PACKAGING PRODUCTS: THE CURRENT SITUATION

The extension of shelf life values may be obtained by means of the inhibition of commensal and
pathogen life forms in food intermediates (before the final packaging) and final products. This
approach requires adequate instruments, including thermal treatments, physical modifications, the
addition of traditional food chemicals (olive oils, vinegar, etc.) for preservation purposes (and
hedonistic reasons), and the use of selected antimicrobials.

.One of the most promising research fields in this ambit concerns the possible use of “hybrid”
approaches involving strong chemical agents such as chlorine dioxide/ozone in association with
natural biocide substances and other plant extracts. Antibiotic substances are widely used in the
food industry and related food/nonfood sectors. The second of the above-mentioned risks is related
to the use of devices able to remove bioavailable oxygen from the inner atmosphere of the package.
By the microbiological viewpoint, the use of similar agents may be considered as an antimicrobial
strategy against aerobic bacteria. However, the indirect effect in certain situations could predictably
be the possible spreading of anaerobic microorganisms. Consequently, the survival and growth of
antimicrobial-susceptible life forms may theoretically be observed when the antibiotic system
inhibits only a notable portion of the existing microbial flora into the food container. Many
antimicrobial substances can be used at present with regard to active packaging systems, provided
that national authorities approve their use. In general, these compounds may be subdivided into
eight main categories: organic acids, enzymes, bacteriocins, fungicides, natural substances,
polymers, oxygen scavengers, and other agents. Four strategies are considered in the realization of
antimicrobial food packaging systems, with the exclusion of polymers with intrinsic antimicrobial
properties:

(a) Addition of the antimicrobial agent in sachets.

(b) Direct addition to the polymeric matrix.
(c) Coating and/or absorption on the polymeric (packaging surface) intended for food contact and
Immobilization of the antimicrobial agent in the packaging matrix by means of chemical covalent
bonds.

BIOCIDE POLYMERS: A MECHANISTIC OVERVIEW

Generally, polymeric antibiotics are prepared through polymerizing monomers with biocidal agents
as functional groups and are expected to behave similarly to these small-molecule counterparts.
Dombrosk and Donaruma synthesized a series of polymeric antibiotics with sulfonamides by
condensation polymerization with the comonomer dimethylolurea Even though the precise
structures of the polymers were unclear, these polymers were shown to be stable under strong
hydrolysis conditions and exhibited comparable biocidal activity compared to the sulfonamide
monomers at the same dosage.The authors also investigated the effects of different comonomers,
dimethylolurea, and formaldehyde, on the biocidal activity of sulfonamide copolymers. It was found
that the copolymers containing dimethylolurea had superior performance compared with those
copolymerized with formaldehyde under identical testing conditions, indicating that the biocidal
action depends on comonomers in addition to the content of sulfonamide.
However, not all-polymeric antibiotics exhibit strong biocidal performance compared to their small
molecule counterparts. One possible reason for this is that the polymerization reactions may
interfere with the mechanisms of action of biocidal functional groups, as was reported who
prepared a series of polymerizable vancomycin derivatives through modifications toward different
sites on vancomycin molecules. A new class of polymeric antibiotics has been designed by
immobilizing photo-sensitizers as the antibiotics.Photo-sensitizers generally possess conjugate
chemical structures, which contain delocalized electrons with high density. The delocalized
electrons are excited after being stimulated by light and return to ground energy level to emit
energy.

THE INFLUENCE OF HIGH PRESSURE TREATMENT AND THERMAL PASTEURIZATION ON THE

SURFACE OF POLYMERIC PACKAGING FILMS

Evaluate the influence of HPP and thermal pasteurization on the surface topography and surface
energy of polymeric films, AFM, profile method and surface energy measurements were used. The
combination of atomic force microscope and profile method enables the assessment both with high
resolution at a small measurement area (AFM) and with a lower resolution at a large measuring
length. The surface energy measurement complements the obtained information with data about
polar and dispersive parts as well as the total surface energy. The commercially available foils were
additionally tested by DSC and tensile testing. With this, potential interrelations between high
pressure and thermal induced changes of topography and material properties can be identified.

The stability of the molecular orientation within the oriented polymer films is dependent on internal
stresses (in turn dependent on process management and thermal history) and the opportunity to
reduce these tensions. Hence even at temperatures below the thermodynamic melting temperature
a shrinking of stretched films may occur. The findings indicate that because of the compression and
decompression by HPP, these opportunities to reduce the tension within oriented polymer films are
facilitated; hence, a slight shrinking occurs. A comparison of the thermally pasteurized biaxially
oriented samples supports this assumption.

Based on the findings for single-layer films we selected two laminated multi-layer films with a
pasteurization sensitive layer and heat sealable layer to test commercially available multilayer films.
For these films further analyses (DSC and tensile testing) in addition to AFM and profile method
were performed. Unfortunately the PEpeel layer of the PP-BO/PEpeel multi-layer turned out to be
not suitable for HPP. In contrast to the single-layer films, there is no effect of high pressure induced
or thermal pasteurization on the arithmetic mean roughness obtained by profile method.

MECHANICAL AND THERMAL BEHAVIOUR OF FLEXIBLE FOOD PACKAGING POLYMERIC FILMS

MATERIALS UNDER HIGH PRESSURE/TEMPERATURE TREATMENTS

The effect of high-pressure processing on mechanical and thermal properties of four complex
packaging materials (polyethylene/ethylene vinyl alcohol/ polyethylene: PE/EVOH/PE; metallized
polyester/polyethylene: PETmet/PE; polyester/ polyethylene: PET/PE; polypropylene SiOx
recovered: PPSiOx) was studied. Pouches of the different materials containing distilled water or
olive oil as food simulants, as well as empty ones, were subjected to 400 MPa for 30 min, at
temperatures of 20 or 60°C. Delamination and wrinkling were a general consequence of the high-
pressure processing of multilayer polymeric systems. However, no signifi cant changes were
observed regarding the mechanical properties of PE containing laminates after pressurization.
PPSiOx underwent signifi cant modifi cations as SiOx completely broke down. Neither thermal
property was affected by pressure, as it was the processing temperature that induced tempering
effects on the crystallization behaviour of polymeric components. Only PE/EVOH/ PE, when in
contact with water as a simulant, presented a decrease in the melting point temperature.

Investigated the effect of HPP on the mechanical and physical characteristics of eight high-barrier
multilayer fi lms (polyester/SiOx recovered /low-density polyethylene: PET/SiOx/ LDPE;
polyester/Al2O3 recovered/low-density polyethylene: PET/Al2O3/LDPE; polyester/polyvinylidene
chloride/nylon/highdensitypolyethylene/polypropylene:PET/PVDC/nylon/HDPE/PP;polyethylene/n
ylon/ethylene vinyl alcohol/polyethylene:PE/nylon/EVOH/PE; polyethylene/ nylon/polyethylene:
PE/nylon/PE; metallized polyester/ethylene-vinyl acetate/linear
lowdensitypolyethylene:metallizedPET/EVA/LLDPE;polypropylene/nylon/polypropylene:
PP/nylon/PP; and polyester/polyvinylidene chloride/ ethylene-vinyl acetate: PET/PVDC/EVA).

POLYMERIC ENCAPSULATES OF ESSENTIAL OILS AND THEIR CONSTITUENTS: A REVIEW OF

PREPARATION TECHNIQUES, CHARACTERIZATION, AND SUSTAINABLE RELEASE MECHANISMS.

Starch is a readily available polymer of plant origin commonly used for encapsulation process.used
starch for the first time for the encapsulation of pesticidesused starch in the encapsulation of
flavoring agents. The modification also alters the DE (Dextrose Equivalent value) of products, which
represent the degree of hydrolysis, this in-turn regulates the retention capacity of volatile
compounds. Maltodextrins, cyclodextrins, and dextrin whites are the major hydrolysates derived
using acid treatment or enzyme modification of the starch and have been widely used for the
encapsulation of EOs and other flavoring agents. EOs encapsulation due to low solubility and rapid
solidifying/lack of emulsifying properties, hence used in combination with other polymers like gum
arabic, chitosan, proteins.

ANTIMICROBIAL ECO-FRIENDLY POLYMERIC FILMS FOR FOOD PACKAGING APPLICATIONS

Addition of sachets / pads containing volatile agents into packages is the most successful
commercial application of antimicrobial packaging. Oxygen absorbers, moisture absorbers and
ethanol vapor generators are the main types of sachets used commercially. Oxygen and moisture
absorbers are used especially in bakery, pasta and meat packaging to prevent oxidation and water
condensation. Although oxygen absorbers are not an antimicrobial agent, a reduction of headspace
oxygen in the package inhibits the growth of aerobes, particularly molds. Moisture absorbers reduce
water activity and also indirectly affect microbial growth on the food.

PE is a polymerized ethylene resin, used especially for containers, kitchenware, and tubing, or in the
form of films and sheets for packaging. The mechanical properties of PE depend significantly on
variables such as the extent and type of branching, the crystal structure, and the molecular weight.
Han and Floros extruded an antimicrobial film using LDPE resins and potassium sórbate powder. Its
tensile properties, transparency and antimicrobial activity were measured to examine the
performance as a packaging material. Incorporation of potassium sórbate in the film did not affect
the tensile properties.

MODELING AND SENSITIVITY ANALYSIS OF MASS TRANSFER IN ACTIVE

MULTILAYER POLYMERIC FILM FOR FOOD APPLICATIONS

The barrier performance of multilayer polymeric films for food applications has been significantly
improved by incorporating oxygen scavenging materials. The scavenging activity depends on
parameters such as diffusion coefficient, solubility, concentration of scavenger loaded and the
number of available reactive sites. These parameters influence the barrier performance of the film
in different ways. Virtualization of the process is useful to characterize, design and optimize the
barrier performance based on physical configuration of the films. Also, the knowledge of values of
parameters is important to predict the performances. Inverse modeling and sensitivity analysis are
sole way to find reasonable values of poorly defined, unmeasured parameters and to analyze the
most influencing parameters. Thus, the objective of this work was to develop a model to predict
barrier properties of multilayer film incorporated with reactive layers and to analyze and
characterize their performances. Polymeric film based on three layers of Polyethylene terephthalate
(PET), with a core reactive layer, at different thickness configurations was considered in the model.
A one dimensional diffusion equation with reaction was solved numerically to predict the
concentration of oxygen diffused into the polymer taking into account the reactive ability of the
core layer. The model was solved using commercial software for different film layer configurations
and sensitivity analysis based on inverse modeling was carried out to understand the effect of
physical parameters. The results have shown that the use of sensitivity analysis can provide physical
understanding of the parameters which highly affect the gas permeation into the film. Solubility and
the number of available reactive sites were the factors mainly influencing the barrier performance
of three layered polymeric film. Multilayer films slightly modified the steady transport properties in
comparison to net PET, giving a small reduction in the permeability and oxygen transfer rate values.
Scavenging capacity of the multilayer film increased linearly with the increase of the reactive layer
thickness and the oxygen absorption reaction at short times decreased proportionally with the
thickness of the external PET layer.

ANTIMICROBIAL AND IMPROVED BARRIER PROPERTIES OF NATURAL PHENOLIC COMPOUND-

COATED POLYMERIC FILMS FOR ACTIVE PACKAGING APPLICATIONS

Functional antimicrobial low-density polyethylene (LDPE) films with coatings containing different
amounts of pyrogallol (PGL), a natural phenolic substance, and polyurethane were prepared. To
examine the applicability of the prepared LDPE/PGL films in packaging, the films were characterized
by scanning electron microscopy, Fourier transform infrared, thermogravimetric analysis, and X-ray
diffraction. The role of the coating, the barrier and color properties, and the antimicrobial activity
of the films were evaluated. The thermal stability of the LDPE/PGL films was affected by the PGL
concentration. Coatings with pyrogallol caused the barrier properties for water, and oxygen was
increased from 0.78–0.32 to 470 ± 23.2–273 ± 57.1 (g mm)/(m2 h kPa), respectively. These findings
indicate that the barrier properties of the LDPE/PGL films were highly improved compared to those
of neat LDPE. Moreover, the LDPE/PGL films exhibited acceptable antimicrobial activity against
Staphylococcus aureus (Gram-positive) and Escherichia coli (Gram-negative), especially for S.
aureus. Further studies are necessary to increase the thermal stability of the pyrogallol coatings with
the LDPE substrate in order to improve their performance and extend their packaging applications

NEW GENERATION OF THE POLYMERIC PACKAGING MATERIALS SUSCEPTIBLE TO ORGANIC

RECYCLING

Among biodegradable polyesters, aliphatic biopolyesters (polyhydroxyalkanoates, PHAs) are

polymer materials of natural origin with broad scope of application. PHAs are typical thermoplasts,
which conquer our everyday life as disposable packaging materials, but which also have strong
position among materials used for medical applications. These materials are of renewable (non
fossil) source, and after finished lifetime they undergo organic recycling. Alternatively to
composting, poly(3-hydroxyalkanoates) can also be recycled to valuable resources using relatively
simple methods. This article, in a perspective of recently carried out comprehensive research of new
generation packaging materials made of organically recyclable polymers, presents possibilities of
application of PHA and their synthetic analogs in that scope

LDPE-BASED BLENDS AND FILMS STABILIZED WITH NONRELEASING POLYMERIC ANTIOXIDANTS

FOR SAFER FOOD PACKAGING

Several novel random copolymers of ethylene and 1‐olefin counits bearing a highly efficient phenolic
antioxidant moiety placed at different distances from the polymerizable double bond were prepared
in the presence of a metallocene catalyst. These copolymers were melt‐blended with an antioxidant‐
free LDPE in an internal batch mixer to obtain innovative materials containing nonreleasing
polymeric antioxidants suitable for safer food packaging applications. Blends and films, obtained by
compression molding, were tested for their thermal and thermo‐oxidative stability by
thermogravimetric analysis both in dynamic and isothermal conditions. Films containing the
macromolecular antioxidants showed a longer induction time before O2 uptake starts and,
consequently, a higher degradation temperature than neat LDPE or LDPE containing a low molecular
weight commercial additive. Aging tests demonstrated that the new polymeric antioxidants also
exert a valid protection against photo‐oxidation. Eventually, migration tests demonstrated the
absence of any trace of products containing the antioxidant moiety when the films were kept in
contact with a food simulant.

DEVELOPMENT OF NEW, NONABSORBABLE POLYMERIC ANTIOXIDANTS FOR USE IN FOODS

Antioxiflant Activity The antioxidant activity of BHT, BHA, TBHQ, and various polymeric antioxidants
in vegetable oil was determined using the official active oxygen method (AOM) procedure (30). In
addition, oils were aged at 80 C in a forced-draft oven and peroxide values (PV) determined (31).
Endpoints in both instances were taken as the number of hours to reach 70 and 100 meq peroxide
per kg of oil. Unless otherwise specified, the antioxidants were tested at levels up to 200 ppm in oil;
polymeric antioxidants were also tested at equivalent (% by wt) aromatic hydroxyl content. In all
instances, 200 ppm citric acid was added to the oils to chelate trace metals which act as prooxidant
catalysts. Antioxidant activity was also measured in an emulsified oil-water system using the
hemoglobin peroxidation procedure described by Cort (32). In our modification of the Cort
technique, the antioxidants were not added to preformed emulsions from alcohol stock solutions.
Rather, the antioxidants were added to the oil phase from GMO concentrates, after which the
system was emulsified as described.
EXPERIMENTAL AND THEORETICAL STUDY OF THERMODYNAMICS AND TRANSPORT PROPERTIES
OF MULTILAYER POLYMERIC FOOD PACKAGING

The quality of the packaged food is directly related to the foodstuffs and packaging material
attributes. There are interaction processes between the packaging, food, and environment
(sorption, permeability, and migration) that can affect the quality and characteristics of the package
and the foodstuffs, especially in the case of plastic packaging. Multilayer structures are one of the
more significant developments in which each layer contributes with its specific properties to the
new complex structure. The multilayer material is usually an excellent barrier to moisture, oxygen,
carbon dioxide, and nitrogen while they provide adequate mechanical protection to the contained
product. The use of multilayer materials significantly increases the shelf life and quality of various
packaged foods such as meat, fish, poultry, cheese, snacks, and ready-made meals. LDPE is widely
used as one of the components in multilayer structures because of its unique properties of
moisturebarrier and heat sealability. Many of those components are additives such as antioxidants,
lubricants and stabilizers, which must be added to polymers in order to improve some properties,
such as thermal stability, flexibility, mechanical properties, among others.

POLYMERIC-BASED FOOD PACKAGING FOR HIGH-PRESSURE PROCESSING

High-pressure processing (HPP) of foods mainly utilizes flexible packaging materials for commercial
products. There are a number of integrity requirements for these packaging materials that must be
complied with for acceptance and use in different product applications. These include visual
integrity, gas permeability, seal and physical strength properties, and global migration of packaging
components into the food, some of which are specific to either refrigerated or shelf-stable products.
HPP is known for its potential in manufacturing novel value-added foods retaining heat labile
nutrients, flavors, and aromas, with products ranging from individual to institutional size packages.
Continuous or semi-continuous HPP systems are used only in a few cases to directly process
pumpable products, which then need to be aseptically packaged. In batch HPP systems, the product
is generally treated in its final primary package; commonly, the food and its packaging are treated
together; thus, the entire package remains a ‘‘secure unit’’ until the consumer opens it. In-container
processing requires packages in form of pouches, large bulk bags, or container-lid combination. The
packaging used for treated foods must be able to accommodate up to a 19% reduction in volume
and return to its original volume without loss of seal integrity or barrier properties. Packaging
materials, which are oxygen impermeable and opaque to light, have been developed for keeping
colors and flavors fresh in certain HPP treated foods. Some multilayer structures also may be
suitable for pre-packaged highpressure-treated foods. At least one interface in the package should
be flexible enough to transmit the pressure.

POLYMERS FOR INNOVATIVE FOOD PACKAGING

Polymers have long been a vital part of food packaging due to their mechanical strength, inexpensive
cost, and ease of processing and manufacturing. Food packaging provides not only a method for
transporting food safely, but extended self-life as well as protection from harmful bacteria,
contamination, and degradation that would occur otherwise. Over the past several years,
modifications in polymers, glass, and paper packaging materials have made it possible to store,
protect, and preserve food from spoiling and damage. With declining petroleum supplies and an
abundance of non-biodegradable plastics in landfills across the country, the need for
environmentally friendly, cheaper, and more effective methods of packaging are required to extend
shelf life and preserve the quality of the food while also improving the barrier and mechanical
properties. With growing concern for the environment, biodegradable polymers are now being
investigated for 7 food packaging while still maintaining mechanical strength and functionality. Each
food packaging plastic is used in a certain way due to their unique properties. A plastic such as PET
has very good tensile and yield strength properties as well as being transparent after processing but
melts very easily, making it ideal for cold beverages which need a strong material to contain the
liquid while preventing chemical interactions. Though all the mechanical properties are pertinent to
how strong the material is and what kind of support and strength it will have, the tensile strength is
the most commonly looked at aspect of a material since it will indicate the materials resistance to
stress and strain. Of the barrier properties, oxygen and water transfer are the most important
aspects to food packaging since an increase in oxygen or water can often speed up the decay of
food. It is also important to note that none of the current packaging plastics address other packaging
problems such as biodegradability, prevent or warn of contamination, or preservation of the food.

EFFECTS OF HIGH PRESSURE TREATMENTS ON POLYMERIC FILMS FOR FLEXIBLE FOOD PACKAGING

Novel processing methods for food preservation have been recently developed to improve safety,
quality and shelf life of packaged foods. Among these treatments, high pressure processing (HPP) is
steadily gaining as a food preservation method that maintains the natural sensory and nutritional
attributes of food with minimal quality loss. Packaged foods processed using this technique maintain
most of their original texture and nutritional and sensory qualities with extended shelf life. HPP
preserves food and only minimally alters its qualities as compared with thermal treatment, chemical
conservation or irradiation. The HP is applied to a confining fluid, contained in a HP vessel, which, in
turn, transmits the pressure loading to foodstuff contained in a proper packaging structure.
Packaged food product, compression fluid, packaging materials and, if present, headspace gas phase
all undergo compression heating that leads to marked increase of temperature above its initial value
during the compression stage. The amount of adiabatic heating depends on the specific foodstuff
HPP preserves food and only minimally alters its qualities as compared with thermal treatment,
chemical conservation or irradiation.composition and on the type of packaging material and of
pressure-transmitting fluid.
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