Trends in Food Science & Technology 14 (2003) 7178

Review

Biodegradable lms
and composite
coatings: past,
present and future
R.N. Tharanathan
Department of Biochemistry and Nutrition, Central
Food Technological Research Institute, Mysore-570
013, India (tel: +91-821-514876; fax: +91-821517233; e-mail: tharanathan@yahoo.co.uk)

Food packaging is concerned with the preservation and

protection of all types of foods and their raw materials,
particularly from oxidative and microbial spoilage and also
to extend their shelf-life characteristics. Increased use of
synthetic packaging lms has led to serious ecological problems due to their total non-biodegradability. Continuous
awareness by one and all towards environmental pollution
by the latter and as a result the need for a safe, eco-friendly
atmosphere has led to a paradigm shift on the use of biodegradable materials, especially from renewable agriculture
feedstock and marine food processing industry wastes.
Such an approach amounts to natural resource conservation and recyclability as well as generation of new, innovative design and use. Their total biodegradation to
environmentally friendly benign products such as CO2, water
and quality compost is the turning point which needs to be
capitalized and encashed. Polymer cross-linking and graft
copolymerization of natural polymers with synthetic monomers are other alternatives of value in biodegradable
packaging lms. Although their complete replacement for
synthetic plastics is just impossible to achieve and perhaps
may be even unnecessary, at least for a few specic applications our attention and needful are required in the days
to come. No doubt, eventually BIOPACKAGING will be our
future.
# 2003 Elsevier Science Ltd. All rights reserved.

Introduction
Food packaging, an important discipline in the area
of food technology, concerns preservation and protection of all types of foods and their raw materials, as well
from oxidative and microbial spoilage. Petrochemical
based plastics such as polyolens, polyesters, polyamides, etc. have been increasingly used as packaging
materials, because of their availability in large quantities
at low cost and favourable functionality characteristics
such as good tensile and tear strength, good barrier
properties to O2 and aroma compounds and heat sealability. On the contrary they have a very low water
vapour transmission rate and most importantly they are
totally non-biodegradable, and therefore lead to environmental pollution, which pose serious ecological problems. Hence, their use in any form or shape has to be
restricted and may be even gradually abandoned to circumvent problems concerning waste disposal (Tharanathan & Saroja, 2001). Of late, there is a paradigm
shift imposed by the growing environmental awareness
by all to look for packaging lms and processes, which
are biodegradable and therefore compatible with the
environment. In a sense, biodegradability is not only a
functional requirement but also an important environmental attribute. Thus, the concept of biodegradability
enjoys both user-friendly and eco-friendly attributes,
and the raw materials are essentially derived from either
replinishable agricultural feedstocks or marine food
processing industry wastes, and therefore it capitalizes
on natural resource conservation with an underpinning
on environmentally friendly and safe atmosphere. An
additional advantage of biodegradable packaging
materials is that on biodegradation or disintegration and
composting they may act as fertilizer and soil conditioner, facilitating better yield of the crops. Though a bit
expensive, biopackaging is tomorrows need for packaging especially for a few value added food products.
Food, either in its processed form or in the raw
material stage, depending upon its water activity and
temperature of storage is highly perishable and therefore needs a careful technological intervention to preserve it longer. Quality food preservation is a serious
concern in the present day food processing operations.
The post harvest losses of our farm produce, for example, the fruits and vegetables are signicant, ranging
from 15 to 20%. These losses are mainly due to

0924-2244/03/$ - see front matter # 2003 Elsevier Science Ltd. All rights reserved.
doi:10.1016/S0924-2244(02)00280-7

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R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

improper handling and unsound post-harvest technologies being practiced. Transportation from the production center to far o places for marketing accounts for
additional losses due to spoilage. Availability of farm
produce with freshness, enhanced shelf-life, better avour/aroma and textural characteristics with a higher
nutritional value is the need of the day.

ability upon blending and/ or processing to result in

such packaging materials. Their functionality can be
better expressed by using in combination with other
ingredients such as plasticizers and additives. The
potential uses for such biopolymeric packaging materials are:
1. use and throw, disposable packaging materials,
2. routine consumer goods for day-to-day use, such
as plates, cups, containers, egg boxes, etc.,
3. disposable personal care napkins/ sanitary pads,
diapers, etc.,
4. lamination coating, and
5. bags for agricultural mulching (nersary).

Packaging lms
The commonly used packaging lms are shown in
Table 1. Although a total replacement of synthetic
plastics by the biodegradable materials is just impossible, at least for some specic applications such a
replacement seems obvious and useful. Towards this
end, there exists a huge business opportunity. Nevertheless, such a replacement by biodegradable materials
would also allow us preserve or extend our expensive,
dwindling petroleum resources, and helps us save on
our foreign exchange. Essential prerequisites of a good
packaging lm (Kader, 1989) are:
1. allow for a slow but controlled respiration
(reduced O2 absorption) of the commodity;
2. allow for a selective barrier to gases (CO2) and
water vapour;
3. creation of a modied atmosphere with respect to
internal gas composition, thus regulating the
ripening process and leading to shelf-life extension;
4. lessening the migration of lipidsof use in confectionery industry;
5. maintain structural integrity (delay loss of
chlorophyll) and improve mechanical handling;
6. serve as a vehicle to incorporate food additives
(avour, colours, antioxidants, antimicrobial
agents) and
7. prevent (or reduce) microbial spoilage during
extended storage.

Biodegradable composites and packaging lms

All the above prerequisites can be met with by polymer composites, whose composition and formulation
vary from commodity to commodity. Biopolymers from
agricultural feed stocks and other resources have the

Two types of biomolecules, viz., hydrocolloids and

lipids, are generally used in combination for the preparation of biodegradable packaging lms or composites. Individually they lack structural integrity and
characteristic functionality. For example, hydrocolloids,
being hydrophilic are poor moisture barriers, a property
compensated by adding lipids, which are very good
moisture barriers. Composite lms are in fact a mixture
of these and other ingredients in varying proportions,
which determine their barrier (to H2O, O2, CO2 and
aroma compounds) and other mechanical properties.
Sometimes a composite lm formulation can be tailor
made to suit to the needs of a specic commodity or
farm produce. For example, oranges having a thick peel
are prone to anaerobic conditions, which lead to an
early senescence and spoilage if the composite lm is
rich in lipids. Phase separation encountered during the
preparation of composites is overcome by using emulsifying agents. Use of plasticizers such as glycerin,
enthylene glycol, sorbitol, etc. in the lm formulations or composites is advantageous to impart pliability and exibility, which improves handling
(Garcia, Martino, & Zanitzky, 2000). Use of plasticizers reduces the brittleness of the lm by interfering
with the hydrogen bonding between the lipid and
hydrocolloid molecules.
The use of wax coating of fruits by dipping is one of
the age-old methods, that was in vogue in the early 12th
century (Krochta, Baldwin, & Nisperos-Carriedo, 1994).
This was practiced in China, essentially to retard water

Table 1. Packaging lms commonly used

Film type

Monomeric unit

Characteristics

Polyethylene
Polyvinylidene
Polyester
Polyamide (Nylon)
Cellophane

Ethylene
Vinylidene
Ethyleneglycol+terephthalic acid
Diamine+various acids
Glucose (cellulose)

Desirable
Desirable
Desirable
Desirable
Desirable

mechanical properties, heat sealable

H2O/O2 barrier, not very strong, heat sealable
mechanical properties, poor H2O/O2 barrier, not heat sealable
strength, heat sealable, poor H2O/O2 barrier
strength, good H2O/O2 barrier, not heat sealable.

R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

transpiration losses in lemon and oranges. Later fat

coating of food products, specically called larding
was in vogue in England. Sausage casing used very commonly nowadays is nothing but a material derived from a
protein source (gelatin). Usually a lm thickness of  2.5
mm is employed, and coating is done by several methods.
Films are preformed thin membranous structures, which
are used after being formed separately, whereas in coatings the thin lm is formed directly on the commodity.
Dip method coating is the commonly used method for
fruits, vegetables and meat products. In here the commodity is directly dipped into the composite coating
formulations (in aqueous medium), removed and
allowed to air dry, whereby a thin membranous lm is
formed over the commodity surface. Continuous dipping builds up decay organisms, soil and trash in the
dipping solution, which needs to be removed for better
performance characteristics.
The coating can also be done by a foam application
method. Emulsions are usually applied by this method.
In here extensive tumbling action is necessary to break
the foam for uniform distribution of the coating solution, over the commodity surface. Coating by spraying
is the conventional method generally used in most of the
cases. Due to high pressure (6080 psi) less coating
solution is required to give a better coverage. Programmable spray systems are available for automation during such operations.
Biodegradable packaging lms are generally prepared
by wet casting of the aqueous solution on a suitable
base material and later drying. Choice of the base
material is important to obtain lms, which can be
easily removed without any tearing and wrinkling.
Infrared drying chambers are advantageous in that they
hasten the drying process (Tharanathan, Srinivasa, &
Ramesh, 2002). Optimum moisture content ( 58%) is
desirable in the dried lm for its easy peel o from one
edge of the base material.
Biopolymeric lms cannot generally be extrusion
blown, like synthetic polymers, as they do not have
dened melting points and undergo decomposition
upon heating.
Film formation generally involved inter- and intra
molecular associations or cross-linking of polymer
chains forming a semi-rigid 3D network that entraps
and immobilizes the solvent. The degree of cohesion
depends on polymer structure, solvent used, temperature and the presence of other molecules such as plasticizers. The presence of lipids in the composite
formulations or lm provides an appealing glassy nish
over the commodity surface.
The various naturally occurring biopolymeric materials of use in composite lm making and coating formulations are shown in Fig. 1. Coating composites
based on such biomolecules have brought a surge of
new types of packaging materials into use. These bio-

73

molecules are compatible amongst themselves and with

other hydrocolloids, surfactants and additives, and their
aqueous solutions are usually stable at acidic and neutral pH. The composite solutions are preserved for
extended/repeated use by adding benzoic acid, sorbic
acid or their sodium salts.
Polysaccharides are known for their structural complexity and functional diversity (Tharanathan, 2002).
Primary structures of some of the polysaccharide
hydrocolloids and their derivatives are shown in Fig. 2.
Linear structure of some of these polysaccharides, for
example, cellulose (1,4-b-d-glucan), amylose (a component of starch, 1,4-a-d-glucan), chitosan (1,4-b-d-glucosamine polymer), renders their lms tough, exible
and transparent. Their lms are resistant to fats and
oils. Cross-linking, for example, of chitosan with aldehydes make the lm much more tough, water insoluble
(or swellable) and highly resistant.
Cellophane, a regenerated cellulose lm is made by
the viscose process. Some of the cellulose esters like
cellulose acetate propionate and butyrate are thermoplastic products of commercial importance. The anionic
cellulose ether, carboxymethyl cellulose (CMC), being
water soluble and compatible with other (bio-)molecules, has excellent lm forming properties (Fig. 3).
CMC lms are capable of reducing oil pick-up in deepfat-fried foods. CMC of a degree of substitution 0.7 is
usually used in such applications. The barrier and
mechanical properties of cellulose-based lms are
dependent on the molecular weight of cellulose (see
Table 2), higher the molecular weight better is the
properties (Krochta et al., 1994).
TAL-Prolong and Semperfresh are two commercially
available composite coating formulations based on
CMC (Nisperos-Carriedo, Baldwin, & Shaw, 1992).

Fig. 1. Naturally occurring biopolymers of use in biodegradable

packaging lms and composites.

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R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

Fig. 2. Chemical structures of (a) cellulose, (b) amylose, (c) chitosan and (d) pullulan.

They contain sucrose fatty acid ester, sodium salt of

CMC and emulsier. Available in powder or granular
form, their aqueous solution (0.52% concentration) is
used for shelf-life extension of banana and other fruits.
Coated banana showed decreased O2 levels and climacteric rise in ethylene production and delayed chlorophyll
loss. Coating of TAL-Prolong (1%) on mangoes showed
delayed ripening with an extended shelf-life. Nature-Seal
is another cellulose-based coating formulation used for
delayed ripening of tomatoes and mangoes.
Starch is another raw material in abundance, especially from corn, having thermoplastic properties upon
disruption of its molecular structure (Tharanathan,

1995; Tharanathan & Saroja, 2001). Preponderance of

amylose (> 70%) in amylomaize starches gives stronger,
more exible lms. Branched structure of amylopectin
generally leads to lms with poor mechanical properties
(decreased tensile strength and elongation). Substitution
of the hydroxyl groups in the molecule weaken the
hydrogen bonding ability and thereby improves freezethaw stability and solution clarity. Ether linkage tends
to be more stable than the ester linkage. Hydroxypropyl
starch composites are used for the preservation of candies, raisins, nuts and dates from oxidative rancidity
(Arvanitoyannis, Nakayama, & Aiba, 1998). Graft
copolymerization of synthetic monomers such as acrylo-

R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

75

Fig. 3. Carboxymethylcellulose, DS=10.

Table 2. Properties of cellulose-based packaging lms

Mol. wt. (Da)

Methylcellulose
13,000
20,000
41,000

O2
Water Tensile
ml.m/ vapour strength
m2 s.Pa ng. m/ (MPa)
m2 s.Pa
3.1
3.6
4.6

Hydroxypropyl cellulose
100,000
3.0
370,000
3.2
LDPE
11.32

Elongation
(%)

0.084
0.094
0.103

55.62
56.15
61.15

11.16
18.51
20.71

0.052
0.059
0.006

14.79
32.76
15.32
203.53
13.127.6 100965

nitrile (AN), a precursor of acrylic bers and plastics,

onto starch provides an excellent method for preparing
starch-polymer (S-g-PAN) composites, which are shown
to be biodegradable (Saroja, Shamala, & Tharanathan,

2000). A starch graft poly(methylacrylate) copolymer

has been developed for use in agricultural mulching, that
would degrade during growing season (Dennenberg,
Bothast, & Abbott, 1978). Utilization of the starch portion by the fungi exposes the plastic polymer for enhanced
biodegradability by microbial and oxidative degradation.
Research on biodegradable plastics based on starch
began in the 1970s and continues today at various labs
all over the world. Technologies have been developed
for continuous production of extrusion blown lms and
injection-molded articles containing 50% or more of
starch. Water sensitivity of such lms has been reduced
by lamination with poly(vinyl chloride) (Shogren,
Fanta, & Doane, 1993). Combination of urea with certain polyols provides better plasticization of starch with
good quality lms (Doane, 1992). Melted or destructurized starch, obtained by disruption of the granular
architecture resulting in loss of crystallinity, has
emerged as a new type of thermoplastic material for
commercial development. To increase the compatibility

Fig. 4. Structures of (a) high-methoxyl and (b) low methoxyl pectin.

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R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

of hydrophilic starch with the hydrophobic plastic

matrix, starch granules have been surface treated, for
example with silanes (Doane, 1992). Pro-oxidants can
sometimes be added to enhance oxidative degradation
of the synthetic polymer.
Pectin, is a complex anionic polysaccharide composed
of b-1,4-linked d-galacturonic acid residues, wherein the
uronic acid carboxyls are either fully (HMP, high
methoxy pectin) or partially (LMP, low methoxy pectin)
methyl esteried (Fig. 4). HMP forms excellent lms.
Plasticized blends of citrus pectin and high amylose
starch give strong, exible lms, which are thermally
stable up to 180 C. Pectin is also miscible with poly(vinyl
alcohol) in all proportions. Potential commercial uses
for such lms are water soluble pouches for detergents
and insecticides, ushable liners and bags, and medical
delivery systems and devices. These lms are solution
casted by air-drying at ambient temperature. Starchbased plastic foams formed by blending starch with
polylactic acid are used as loose-ll cushioning materials
to protect against shock and vibration during transportation (Fang & Hanna, 2000). Laminated lms from
pectin and chitosan together with either glycerol or lactic acid as a plasticizer have been prepared (Fishman,
Friedman, and Huang, 1994).
Starch derived products such as dextrins or glucose
are extensively used as a component of the fermentation
medium. Glucose can be fermented to lactic acid, which
can be polymerized to polylactic acid polymers and
copolymers. Their use as biodegradable plastics is of
considerable interest and demand (Narayan, 1993).
Conversion of lactic acid to its dehydrated dimer, the
lactide followed by ring opening polymerization to high
molecular weight polymers or further copolymerization
with caprolactone gives packaging lms of high value.
Bacterial fermentation of glucose, acetic acid and feed
stocks gives novel thermoplastic polyesters such as poly3-hydroxybutyrate (PHB) (Savenkova et al., 2000).
These polymers (Fig. 5) either alone or in combination

Fig. 5. General structure of polyhydroxyalkanoates.

with synthetic plastics or starch (Ke & Sun, 2000) produce excellent packaging lms.
PHB is a thermoplastic biopolyester accumulated as a
reserve of carbon and energy by a number of bacteria
(Lee, 1996). Its exceptional stereo-chemical regularity
leads to progressive crystallization with aging, thus
making it brittle. This has been overcome by incorporation of comonomers by grafting. For example,
copolymers of PHB with 3-hydroxyvalerate are produced by using specic additives in the growth medium
(Byrom, 1992). Such an approach, though improves the
properties of PHB, is not cost eective, because the
copolymer costs are higher, and its toxicity leads to
lower production yields and also its presence aects
PHB crystallization kinetics, which results in longer
processing cycle times. Nevertheless, PHB could be
toughened by the process of annealing by conditioning
in an oven, a process that widens its application possibilities (De Koning & Lemstra, 1993). To overcome the
escalating cost economics, genetically engineered plants
harboring the bacterial PHA biosynthesis genes are
being developed (Lee, 1996), which hopefully may turnout PHAs competitive with the conventional plastics.
The polymorphic Aureobasidium pullulans secretes a
polysaccharide pullulans, which is commercially a useful
hydrocolloid of value (Seviour, Stasinopoulos, Auer, &
Gibbs, 1992). It can be extruded as lms, which are
biodegradable, it is resistant to oils and grease, has
excellent O2 permeability rates and is nontoxic. It is an
a-glucan consisting of repeating maltotriose residues
joined by 1,6-linkages (Fig. 2). Pullulan is of use in biodegradable packaging lm industry.
Free standing lms have been prepared from chitosan
and its derivatives, and their mechanical, barrier and
biodegradation characteristics studied (Kittur, Kumar,
& Tharanathan, 1998). Cross-linked chitosan lms oer
greater strength and resistance for handling. By being
antifungal and antimicrobial, chitosan-based lms and
coating formulations have additional value addition
(Tharanathan & Kittur, in press). Chitosan-based composite coating formulations (Kittur, Saroja, Habibunnisa, & Tharanathan, 2001) as well as lms
(Srinivasa et al., 2002) have been shown to prolong the
shelf-life of banana, mango and capsicum. Application
of chitosan induces the production of plant defence
enzymes such as chitinase. A composite formulation
called Nutri-Save, based on derivatized chitosan, is
extensively used for shelf-life extension of apples, pears,
pomegranates, etc.
Proteinaceous hydrocolloids of plant and animal origin are used in some specic coating formulations. They
provide a good barrier to O2 and CO2, but not to water.
Nevertheless, such lms supplement the nutritional
value of coated food. Zein, the corn protein fraction,
upon casting from aqueous aliphatic alcoholic solutions
form tough, glossy and grease-resistant lms. By adding

R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

glycerine or by cross-linking the tensile strength of the

lms is further improved. Edible lms have been produced by heating sunower proteins to 85 C and solution casting (Meixueir, van Garcia, & Silvestre, 2000).
Film formation in such proteins is through intermolecular disulphide bridges and hydrogen bonds accompanied by surface dehydration. Whey proteins (20% of
total milk proteins) when appropriately processed produce
exible but brittle lms (Kaya & Kaya, 2000).
Collagen lms have traditionally been used for preparing edible sausage casing (Hood, 1987). Collagen is a
major constituent of skin, tendon and connective tissues
and it is the most prevalent and widely distributed
brous protein in the animals. Gelatin, resulting from
partial hydrolysis of collagen, produces exible tough
lms when cast together with glycerine or sorbitol. Proteinaceous lms may sometimes lead to potential allergenic reactions in some individuals because of protein
modication, deciency in essential amino acids, etc.
Wax coatings are naturally found on fruit and vegetable surfaces, where they help prevent moisture loss,
especially in the dry humid season. Preservation of fresh
and dry fruits and nuts by was coatings have been
practiced since time immemorial. Bees wax, paran
wax, candelilla wax (an oily exudate of the candelilla
plant grown in USA/Mexico), etc. are some of the wax
preparations used in such applications. They are also
used as micro-encapsulation agents, especially for spice
avouring substances.
Shellac, composed of complex mixtures of aliphatic,
alicyclic hydroxy acid polymers, is a secretion of the
insect Laecifer lacca. It is used as confectioners glaze on

77

candies. Free fatty acids have also been used in some

composites. By a careful selection of the fatty acid type
(its chain length and type of derivatization) and its
concentration, composite formulations with variable
performance characteristics can be tailor made for specic applications. Formulations prepared by composite
mixture of hydrocolloid, emulsiers and lipid molecules
have shown considerable promise for shelf-life extension
of several agri-horticultural produce (Krochta et al.,
1994).
Polyethylene terephthalate (PET), a polyester has
recently been introduced as a biodegradable packaging
material (The Science, 1997). This material can be recycled, incinerated or land-lled, but it is mainly intended
for disposal by composting, where it undergoes soil
degradation to CO2 and water. Upon complete disintegration ( 8 weeks), it enriches soil as shown by positive indications of plant germination and seedling
emergence, earthworm weight gain and mortality, and
microbial population density. By soil-enrichment methods, microbes have been isolated that degrade major
petrochemical based compounds such as phthalic acid,
isophthalic acid, terephthalic acid and their esters,
which nd extensive use in the manufacture of synthetic
plastic lms.
Addition of natural polymers like starch into polyethylene is another approach to make them biodegradable. Starch-LDPE lms (containing up to 30% starch)
have been shown to be biodegradable upon composting.
The most attractive feature of the biopolymer-based
packaging lms/composites is their total biodegradability. As a result they t perfectly well in the ecosys-

Fig. 6. The carbon cycle of biodegradable polymers.

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R.N. Tharanathan / Trends in Food Science & Technology 14 (2003) 7178

tem, and save our world from growing ecological pollution caused by non-biodegradable plastics, which are
essentially petroleum-based. A number of aerobic and
anaerobic microorganisms have been identied for biodegradation. The carbon cycle involving the biopolymer
degradation is shown in Fig. 6.

Future strategy
Synthetic polymers are gradually being replaced by
biodegradable materials especially those derived from
replenishable, natural resources. More than the origin,
the chemical structure of the biopolymer that determines its biodegradability. Use of such biopackagings
will open up potential economic benets to farmers and
agricultural processors. Bilayer and multicomponent
lms resembling synthetic packaging materials with
excellent barrier and mechanical properties need to be
developed. Cross-linking, either chemically or enzymatically, of the various biomolecules is yet another
approach of value in composite biodegradable lms.
Innovative techniques of preserving food safety and
structural-nutritional integrity as well as complete
biodegradability must be adopted. Eventually biopackaging constitutes a niche market and that will be
our future. Sustained multidisciplinary research eorts
by chemists, polymer technologists, microbiologists,
chemical engineers, environmental scientists and
bureaucrats are needed for a successful implementation
and commercialization of biopolymer-based ecofriendly packaging materials. Undoubtedly, biodegradation oers an attractive route to environmental
waste management.

Acknowledgements
The author thanks Mr. A.B. Vishu Kumar for excellent assistance in type setting the manuscript.

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