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Thermoplastic Starch: A Possible Biodegradable Food Packaging Material-A

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 Journal of Food Process Engineering ISSN 1745–4530

THERMOPLASTIC STARCH: A POSSIBLE BIODEGRADABLE

FOOD PACKAGING MATERIAL—A REVIEW
BAHRAM KHAN1, MUHAMMAD BILAL KHAN NIAZI1,3, GHUFRANA SAMIN2 and ZAIB JAHAN1
1
Department of Chemical Engineering, School of Chemical and Materials Engineering, National University of Sciences and Technology, Islamabad
Pakistan
2
Department of Chemistry, University of Engineering and Technology Lahore, Faisalabad Campus, Pakistan

3
Corresponding author. ABSTRACT
TEL: 92-51-90855116;
FAX: 92 51 9085 5002; In the past years, research has been focused on biodegradable materials to replace
EMAIL: m.b.k.niazi@scme.nust.edu.pk petroleum based plastics for food packaging application. For this purpose,
biopolymers are considered the most promising material because of their
Received for Publication January 19, 2016
biodegradable nature and long shelf life properties like resistance to chemical or
Accepted for Publication June 13, 2016
enzymatic reactions. Starch is renewable, cheap, and abundantly available
doi:10.1111/jfpe.12447 biopolymer. However, the intermolecular forces and hydrogen bonds in starch
resist it to be processed as a thermoplastic material. To overcome this issue,
different plasticizers are used to have deformable thermoplastic material called
thermoplastic starches (TPSs). A plasticizer enhances the flexibility, the process
stability of starch below the degradation temperature. Plasticizer lowers the glass
transition temperature (Tg).
TPS is very promising among the biobased materials available for the production
of biodegradable plastic. TPS have some limitations; bad mechanical properties
and water sensitivity. Starch absorbs water under higher relative humidity. This
work will provide an outline about the research that has been done on TPS during
last 15 years as biodegradable food packaging material.

PRACTICAL APPLICATIONS
The basic role of food packaging material is to make it cost effective that satisfies
industry requirements and consumer desires, and provide protection from three
major classes of external influences: chemical, biological, and physical, e.g., such as
exposure to gases, barrier to microorganisms, or from mechanical damage,
respectively. These external influences may damage the quality of the food and
shelf life. For this motive, starch has become the most preferred option among the
verified classes of synthetic and natural materials. Retrogradation of starch chains
in presence of water make it impossible to be use as packaging material. To
overcome this issue, Starch has been plasticized with water and low molecular
weight additive that can interact with its backbone by hydrogen bonding to
produce thermoplastic starch (TPS). The objective of this review is to summarize
numerous studies related to interaction of plasticizers and starch for the
production of biodegradable TPS food packaging materials.

INTRODUCTION material that can meet both commercial and environmental

The usage of plastic is increasing rapidly due to its wide
range of applications such as packaging, automobile parts,
etc. (Weber et al. 2002; Xiaofei et al. 2004). Many efforts
have been being made to produce biodegradable packaging
demands (Niazi 2013).
Nowadays, researchers are trying to develop methods to
lower the cost and optimize the process performances of bio-
based products (Weber et al. 2002). Efficient packaging
materials and techniques provide surety in terms of safety

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THERMOPLASTIC STARCH
and best quality of the food items (Sunny et al. 2004). Today,
many petroleum-based materials, such as plastics, glass,
paper, and metals, are being used for food packaging. All of
these are not biodegradable. Biodegradable packaging mate-
rial can be produced by the polymers that are extracted nat-
urally, such as starch, cellulose, proteins, etc.
Carbohydrate polymers, such as, starch, cellulose, gums,
chitosan, and pectins, are being extensively used in food
packaging (Lopez et al. 2015), pharmaceutical (Carbinatto
et al. 2014), and textile industries (Dall’Acqua et al. 2004).
Carbohydrates are the hydrates of carbon comprising of sug-
ars and have the empirical formula of CnH2nOn which indi-
cates that carbon atoms are attached with water (Tomasik
and Scilling 2004). Carbohydrates in amorphous form has
high mechanical and chemical properties, hence, they pro-
vide high gas barriers (Kjellgren et al. 2006).
Starch is cheap, renewable, and abundantly available bio-
polymer but it resists to be processed as a thermoplastic
material due to intermolecular forces and hydrogen bonds.
Hence, a plasticizer (urea, glycerol, sorbitol, glycerin) in
addition of water is required to make a deformable thermo-
plastic material called thermoplastic starch (TPS). The basic
function of a plasticizer is to increase flexibility and to
enhance the process ability. The plasticizer lowers the glass
transition temperature (Tg) (Niazi 2013). The importance of
plasticizer is increasing rapidly because of various environ-
mental problems and growing cost of petroleum products.
Hence, plasticizer should be natural, inexpensive, and renew-
able so that the process can be made both cost effective and
biodegradable (Yu et al. 2006).
This article provides an overview on the properties of starch
and its applications with emphasis on TPS. Scientific work so
far done on biodegradable food packaging, usage of TPS with
various plasticizers, its modifications are also reported.
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B. KHAN ET AL.
FIG. 1. BIODEGRADABLE
POLYMERS—CLASSIFICATIONS
BIOPOLYMERS FOR FOOD PACKAGING
MATERIALS
Over the past several years, there are many biobased materi-
als, which have gathered attention in food packaging because
of their specific innovative functions such as high barrier
properties, flexibility, etc. Biodegradable polymers may be
classified into three types on the basis of their synthesis and
sources as shown in Fig. 1 (Lui 2006; Stloukal et al. 2015).
Polymers From Biomass
Most commonly available resources of polymers are from
marine and agricultural, e.g., polysaccharides—starch, cellu-
lose, gums, chitosan (Garcia et al. 2000), protein (animals–
casein, whey, gelatin; Sothornvit and Krochta 2001; Karnnet
et al. 2005 and plants—zein, soya, gluten; Orliac et al. 2003;
Bertan et al. 2005) and lipids—cross-linked tri-glyceride
(Perez-Gago and Krochta 2001).
Polysaccharide films are produced from starch, cellulose,
alginic acid, carrageenan, chitosan or pectins. Among all of
these, starch has been focused mainly for the development of
bioplastic since last many years (Ramirez et al. 2011). Cellu-
lose is the most abundantly available and an economical bio-
polymer present in plant material (Lui 2006).
Gemili et al. (2009) prepared antimicrobial packaging
materials by incorporating lysozyme into cellulose acetate
(CA) films. The structure of the films was altered from high-
ly asymmetric and porous to dense by modulating the com-
position of the initial casting solution so that a controlled
release of lysozyme could be achieved. Film prepared from
5% CA solution including 1.5% lysozyme had highest release
rate, soluble lysozyme activity and antimicrobial activity.
The porosity of the films were decreased by increasing CA
content, hence, reduced the release rate, maximum released
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B. KHAN ET AL.
lysozyme activities, and the antimicrobial activities of the
films. Whereas, immobilized lysozyme activities and the ten-
sile strength of the films were increased. The incorporation
of lysozyme did not reduce tensile strength and elongation
at break values of the films except those prepared with 15%
CA. This study indicated the good potential of asymmetric
CA films to achieve controlled release in antimicrobial
packaging.
Ghaderi et al. (2014) generated All-cellulose nanocompo-
site (ACNC) films from sugarcane bagasse nanofibers using
N,N-dimethyacetamide/lithium chloride solvent. Disk grind-
ing process was applied to downsize the average diameter of
bagasse fibers (14 lm) to 39 nm. It was perceived from X-
ray diffraction (XRD) that apparent crystallinity and crystal-
line size decreased relatively to an increased duration of dis-
solution time. It was confirmed from thermogravimetric
analysis (TGA) that thermal stability of the ACNC was less
than pure cellulose nanofiber sheet. The tensile strength of
fiber sheet, nanofiber sheet, and ACNC generated with 10
min dissolution time were 8, 101, and 140 MPa respectively.
Water vapor permeability of the ACNC film enhanced to an
increased duration of dissolution time. This analysis revealed
that ACNC has a high potential for application in cellulose-
based food packaging owing to its promising
characterization.
Protein and lipid based packaging films have high poten-
tial for proper linkages as they can develop the bonds at sev-
eral different locations (Sothornvit and Krochta 2001).
Gonzalez and Igarzabal (Gonzalez and Igarzabal 2013) pre-
pared and characterized biodegradable bilayer films from
isolated soy protein (SPI) and polylactic acid (PLA). The
films showed high transparent behavior and strong adhesion
between layers were noticed without chemical modification
of film surfaces. PLA content increased the mechanical prop-
erties of the films as compared to SPI films. Moreover, the
hydrophobic properties of PLA enhanced the performance
of film under conditions where water was involved, reducing
the swelling index and water vapor permeability. The bio-
degradation under soil burial conditions was also analyzed
checking weight loss as a function of time. It showed a two-
step degradation and a quicker degradation rate for the pro-
tein component as compared to those of PLA layer.
Polymers From Microbial Sources
Generation of bioplastics from microbial fermentation of
polysaccharides has been innovative research field nowadays
(Chenu and Roberson 1996). Polymers like polyhydroxyal-
kanoates (PHA), polyhydroxybutyrate (PHB) and polyhy-
droxybutyrate co-hydroxyvalerate (PHBv) are commonly
extracted by this method (Tao et al. 2009). PHA is linear
polyester obtained from sugar/lipids. PHB is the most
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THERMOPLASTIC STARCH
common type of PHA used in food packaging (Weber et al.
2002).
Polymers Synthesized Chemically by
Monomers From Agro-Sources
This type of polymer includes PLA (Awala et al. 2015; Stlou-
kal et al. 2015). PLA is engendering a high potential for com-
mercial production of renewable packaging material (Zhang
et al. 2013). PLA is a thermoplastic obtained from lactic acid
(Ayana et al. 2014). The film produced by PLA has good
moisture-barrier properties and has a low gas transmittance
(Weber et al. 2002; Ortenzi et al. 2015).
STARCH
Starch is a natural polymer based on glucose, which is con-
sidered as a valid choice for the biodegradable polymer
products. Starch is extracted from various plant tissues in
the form of granules having the size between 1 and 100 lm
(Sugih et al. 2009). The size and shape of granules depend
upon their sources (Bucknow et al. 2009). Granules are
insoluble in cold water but they swell and make a gel if the
outer membrane has been broken by any action such as
grinding. While if the water is warm; the part of the starch
which is soluble diffuses through the wall of granule and the
rest of the granules swell and burst (Andersen et al. 2000).
Properties of Starch
Starch contains two polysaccharides; amylose and amylopec-
tin. The ratio of these two polysaccharides depends on the
starch source. Lipids and proteins are also present in the
starch but in small amount (Liu et al. 2009a).
Amylose is a linear chain of D-glucose unit that is linked
together by a-1,-4 bonds. Length of this chain varies in sev-
eral plant species between 102 and 104 glucose units. Amylo-
pectin contains short chains of a-1,-4 linked D-glucose units
that are branched by a-1,-6 bonds. The length of this chain
usually ranges from 104 to 105 glucose units (Ponstein
1990). Relative percentages of amylose and amylopectin in
starch (cereal endosperm) range from 18 to 28% amylose
and 72 to 82% amylopectin (Buleon et al. 1998). Usually,
starch having the crystallinity between 20 and 40% is termed
as semicrystalline (Whistler and BeMiller 1984). The amor-
phous region of starch contains amylose and the branching
points of amylopectin (Liu et al. 2009b).
The properties of various starches are summarized in
Table 1 (Leach et al. 1959; Morrison et al. 1984; Whistler and
BeMiller 1984; Soulaka and Morrison 1985; Lim et al. 1994;
Jane et al. 1996; Kasensuwan and Jane 1996; Lii et al. 1996).
3
THERMOPLASTIC STARCH B. KHAN ET AL.

TABLE 1. PROPERTIES OF STARCHES

Swelling Light
Amylose power Solubility transmittance
Source of starch content (%) (g/g) (8C) (%) (8C) (%, at 650 nm) References

Normal potato 20.1–31 1159 (95) 82 (95) 96 Kasensuwan and Jane (1996), Kim et al.
(1995), and Leach et al. (1959)
Normal corn 22.4–32.5 22 (95) 22 (95) 31 Kim et al. (1995), Lim et al. (1994), and
Morrison et al. (1984)
Waxy corn 1.4–2.7 - - 46 Morrison et al. (1984)
High amylose corn 42.6–67.8 6.3 (95) 12.4 (95) - Leach et al. (1959), Lii et al. (1996), and
Morrison et al. (1984)
Normal rice 5–28.4 23–30 (95) 11–18 (95) 24 Jane et al. (1996), Juliano (1992), and Lii
et al. (1996)
Waxy rice 0–2 45–50 (95) 2.3–3.2 (95) - Jane et al. (1996), Juliano (1992), and Lii
et al. (1996)
Normal wheat 18–30 18.3–26.6 (100) 1.55 (100) 28 Deatherage et al. (1955), Morrison et al.
(1984), Soulaka and Morrison (1985),
and Whistler and BeMiller (1984)

MODIFICATION OF STARCH increasing BA content, PVA crystallites size and amount

Native starch has a limited range of applications because of
the unfavorable properties such as brittleness, uncontrolled/
high viscosity, retrogradation, and insolubility in the cold
water (Carvalho 2008). In order to mend such properties,
native starches are modified both chemically and physically
(Zhu 2015).
Cross-Linking
Cross-linking is one of the most important modifications
that can be applied to starch. Stronger covalent bonds
replace the weaker hydrogen bonding between starch chains
(Kapelko et al. 2015). Most of the glucose units in starch
have two secondary and one primary hydroxyl group that
reacts easily with several compounds such as organic chloro
compounds, acid anhydrides, epoxy, and ethylenic com-
pounds (Cysewski et al. 2006; Franssen and Boeriu 2014). As
the number of cross-links increases, it becomes more resis-
tant to gelatinization (Ratnayake and Jackson 2008). The sol-
ubility of the cross-linked starch derivatives in water is
decreased and results in higher stability (Zhong et al. 2013).
The cross-linked starches are used in several fields such as
textile, paper, food, and adhesive industry (Phadnis and Jad-
hav 1991).
Lim et al. (2015) enhanced the thermal stability and barri-
er characteristics of pure polyvinyl alcohol (PVA) by formu-
lating five different cross-linked polyvinyl alcohol/boric acid
(PVA/BA) hybrid films from a solution blending method.
Barrier properties, transparency, thermal stability, and
mechanical properties were investigated as a function of BA
content. It was noticed that the physical properties of the
PVA/BA hybrid films were dependent on the chemical struc-
ture and morphology of the films originating from the
amount of BA and change in degree of cross-linking. By
were decreased, but the cross-linking density was increased,
showing compact packing of molecules. Furthermore, by
increasing BA content, glass transition temperature and ther-
mal stability were also enhanced and the oxygen transmis-
sion rate (OTR) of pure PVA was decreased. In addition,
water resistant pressure and tensile strength were also
increased by increasing BA content. Each hybrid film showed
good transparency. These properties of the cross-linked
PVA/BA hybrid films showed that they are the potential can-
didates for packaging materials.
Tripathi et al. (2009) prepared an antimicrobial film by
blending chitosan (CS) and PVA with a cross-linker, i.e., glu-
taraldehyde. XRD and scanning electron microscopy (SEM)
were used to investigate the miscibility and morphology of
the films. Whereas. the thermal properties were analyzed by
differential scanning calorimetry (DSC) and TGA. The
microbiological screening demonstrated the antimicrobial
nature of the film against food pathogenic bacteria viz.
Escherichia coli, Bacillus subtilis, and Staphylococcus aureus.
The results indicated that the film may be a promising mate-
rial for food packaging.
Jyothi et al. (2006) cross-linked Cassava starch with epi-
chlorohydrin in three different media; water, water with
phase transfer catalyst and N,N-dimethylformamide. The
physicochemical, thermal, and retrogradation properties
were characterized. The degree of cross-linking was found to
be higher in case of N,N-dimethylformamide. The water-
binding capacities were gradually decreased as the degree of
cross linking was increased.
Esterification
In this modification, ester groups replace some hydroxyl
groups. The purpose of this is to enhance the thermal

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B. KHAN ET AL.
stability and gelatinization temperature, and to decrease ret-
rogradation (Grommers 2009). Several starch esters are
available such as starch nitrates (Caesar 1958), starch sulfates
(Cui et al. 2009), starch phosphates (Wischmann et al.
2005), starch alkenyl succinates (Niazi 2013), and fatty acid
starches (Vasiliadou et al. 2015). By esterification, starch
becomes more hydrophobic as compared to native starch
(Namazi et al. 2011).
Wang et al. (2009) modified starch by esterification. They
investigated the morphology, mechanical properties and
thermal stability of starch/natural rubber composite. The
results showed that the crystal structure of starch in the com-
posite vanished after esterification. The thermal stability and
mechanical properties of composite were enhanced with
modification of starch, primarily due to the improved phase
interface interactions between rubber and starch.
Zuo et al. (2015) investigated the influence of dry method
esterification of starch on degradation properties of starch/
PLA composite via melt extrusion method. The mass loss
rates of native starch/PLA and esterified starch/PLA were
15.46% and 19.78% after 30 days of degradation respectively.
After 60 days, the mass loss rates of native starch/PLA and
esterified starch/PLA were 18.59% and 16.62% respectively.
After 90 days, the mass loss rate was increased by 4.98% and
3.4%. The mass loss rate was increased by 3.54% and 3.17%
for 120 days. Mass loss rates showed that mainly starch was
degraded in first 30 days, leading to the slower degradation
rate of esterified starch/PLA than native starch/PLA.
Stabilization
Stabilization is performed to elude retrogradation and to
enhance the tolerance of starch to the fluctuations of the
temperature. It also increases the shelf life of starch products
(Beinecke and McFarland 2012). The bulky groups such as
octenylsuccinate are substituted onto the starch to resist the
linear, dispersed fragments to retrograde (Murphy 2000).
The number of substituted groups determines the effect of
stabilization.
Park and Goins (1995) studied the covalent bonding of 2-
(20 -octenyl) succinic acid (OSA) with starch. For free OSA,
starch was removed from aqueous dispersion by precipita-
tion with methanol and the acidified supernatant was
extracted. For total OSA, esterified OSA was hydrolyzed in
an alkaline solution and OSA was extracted following acidifi-
cation. OSA after derivatization with ethereal diazomethane
was quantified. The native starch is hydrophilic in nature
because of the polyhydroxyl groups in the chain. It does not
contain the required affinity for hydrophobic compounds
such as oil to be an effective emulsifier but by the chemical
modifications, the lipophilic functionality of starch can be
enhanced (Fisk et al. 2013).
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THERMOPLASTIC STARCH
Gomand et al. (2012) annealed potato starches with vari-
ous amylopectin/amylose ratios at stepwise increasing tem-
perature. By the small-angle X-ray scattering experiments, it
was revealed that the lamellar starch crystals gain stability
upon annealing via thickening for high-amylose starch.
Crystal thickening is associated with the co-crystallization of
amylose with amylopectin.
Pregelatinization
Several starches need cooking in order to develop required
properties (Miyazaki et al. 2006). Pregelatinization is the
process which is designed to eliminate the necessity of cook-
ing. Pregelatinization is performed to achieve wide range of
cold thickening starches (Majzoobi et al. 2011).
In spray cooking process, the starch slurry entered in a
heating chamber and then atomized. At the same moment,
hot steam is injected into the chamber to cook out the starch
(Pitchon et al. 1981). By this, a uniform gelatinized starch is
produced with minimum shear and heat damage.
In drum drying, a cooked starch sheets are prepared from
the starch slurry. It is then ground to the desired particle size
(Seib 1996). Cold water swellable starches are generated by
the solvent-based techniques. Fig. 2 (Wurzburg 1986; Liu
et al. 2009a) shows the schematic view of phase transitions
of starch during gelatinization and retrogradation. Heating
in the water damages the crystalline structure of starch gran-
ules and makes amorphous amylopectin (Xie et al. 2013).
The double-helical crystalline structure formed by the short-
branched chains present in amylopectin is destroyed by gela-
tinization. Gel balls are formed by these short-branched
chains (Yu and Christie 2005). By extrusion, V-type single
helix crystals are formed having more yield stresses and
higher moduli for amylose-rich materials. The crystallinity
of V-type crystals increases with time (Wang et al. 1991).
Peerapattana et al. (2012) studied the modification of glu-
tinous rice starch (GS) as a sustained release agent for the
preparation of tablet. The GS slurry was modified physically
by heat and dried by spray drying. The pregelatinized GS
(PGS) appeared in powder form. The flowability was poor.
Tablets having PGS and propranolol HCl were prepared by
wet granulation method. Less than 80% of propranolol HCL
was released in 10 h at drug to PGS ratio 1:2 whereas it took
14 h in ratio 1:3. It was concluded that the higher the com-
position ratio of PGS, the slower will be the release of the
drug.
Ohwoavworhua and Osinowo (2010) investigated the pre-
gelatinization of starch. It was found that pregelatinized
starch preparation takes longer time to dry. To overcome
this issue, acetone precipitation of gelatinized starch was per-
formed. Two methods, cold and hot precipitations, were
used and the results showed that acetone treated pregelati-
nized starch retained good powder properties.
5
THERMOPLASTIC STARCH
FIG. 2. STARCH THERMAL PROCESSING AND AGING (PHASE TRANSITIONS)
In conclusion, it seems obvious that each modification
has its own potential to enhance the properties of starch for
its better use in food packaging field. By these specific modi-
fications of starch, characteristics are continuously being
improved that find increasing use in wide range of packaging
applications, leading to a significant value addition. Eventu-
ally biodegradable packaging will find larger and more
receptive markets in future. It can be predicted that new ven-
tures in starch modifications and their diverse applications
and effects on food packaging will continue to be of great
importance.
THERMOPLASTIC STARCH
Native starch is brittle and hydrophilic in nature that makes
it not suitable for various applications like plastic bags, food
packaging, etc. It has poor thermal process-ability because of
its high melting point and lower thermal decomposition
temperature (Wang et al. 2003). Starch can be converted
into thermoplastic by the use of plasticizer with the com-
bined effect of temperature and shear (Wang et al. 2008). In
the thermal processing of starch-based polymers, various
physical and chemical reactions are involved such as water
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B. KHAN ET AL.
diffusion (Abd El-Mohdy et al. 2012), expansion of granules
(Liu et al. 2009a), gelatinization (Atwell et al. 1988), melting
(Abd El-Mohdy et al. 2012), crystallization (Lluch et al.
2005). By improving the properties of TPS, it can be used in
food packaging field as valid option because it is cost-
effective and abundant. TPS can be blended with various
polymers each having its own properties and potentials.
TPS/Polymer Blends
The main objective of the research was to prepare a plastic
from renewable and biodegradable resources that meets the
market needs (Xiaofei et al. 2004). Pure starch is brittle and
bad mechanical characteristics; it is blended or reinforced
with synthetic polymers (Liu et al. 2009a). Blending plays an
important role in modifying the properties of polymers
(Imre and Pukanszky 2013). A compatible blend is obtained
when two or more polymers are mixed together and the pre-
ferred properties are improved. TPS is blended with numer-
ous polymers along with plasticizers to improve water
resistant and mechanical properties and to use it as a modifi-
er to generate blends which are both biodegradable and eco-
nomical (Murphy 2000). Most common TPS/polymer
blends are as following:
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B. KHAN ET AL.
TPS/Polyethylene Blends. Polyethylene (PE) is chemi-
cally resistant and is not attacked by acid, base, or the salt.
Other properties of PE which has made it widespread are
low cost, electrical insulation, flexibility and toughness (Hua
et al. 2014; Pi et al. 2015).
Pierre et al. (1997) prepared TPS/PE [low-density PE
(LDPE) and linear low-density PE (LLDPE)] blends and
used glycerol as plasticizer. A processing method was devel-
oped to compound the blends in one continuous process in
a co-rotating twin screw extruder fed by single-screw extrud-
er. High pressure was maintained to resist early evaporation
of water. The number average diameter of dispersed phase
was increased indicating a morphological control with
respect to size and shape of dispersed phase. Blends demon-
strated high elongation properties at break even with no
addition of interfacial modifier. For a packaging material,
elasticity or elongation is very important. A material with
high elongation will absorb a large amount of energy before
breaking.
Gonzalez et al. (2003) compared morphology of TPS/
LDPE blends prepared by one-step extrusion with those
obtained by reprocessing of the original blends. It was noticed
that blends from one step extrusion process showed high
anisotropy. The TPS particles of reprocessed blends showed
no coalescence and a low degree of deformation. Results indi-
cated that one-step processing of the blends can be used to
achieve highly elongated morphological properties.
Masoomi et al. (2015) prepared LDPE/LLDPE/TPS films
to obtain environmentally friendly materials consisting of
high TPS content with desired packaging properties. Blend-
ing was performed in a twin-screw extruder followed by a
process called blowing. Blending of LDPE/LLPDE (70/30 wt/
wt) with 5 to 20 wt% of TPS and 3 wt% of PE grafted maleic
anhydride was performed. SEM results showed good disper-
sion of TPS in PE matrices. DSC analysis indicated that
starch had more pronounced effect on crystallization of
LLDPE than LDPE. The desired mechanical properties of
packaging applications were achieved when 15 wt% starch
was added.
TPS/PE blends are very much suitable for food packaging
due to their high toughness and flexibility properties. The
other useful characteristics are easy process ability, reason-
able clarity of thin films, and sufficiently low permeability to
water vapor.
TPS/Polypropylene Blends. Polypropylene (PP) has
very good electrical and insulating properties. It is resistant to
various chemicals including dilute and concentrated acids,
alcohols, bases, aldehydes, esters, ketones, etc. at high temper-
ature (Reddy et al. 2008). It is being used in packaging, con-
sumer goods, and automotive (Imre and Pukanszky 2013).
Rosa et al. (2007) studied blended TPS with recycled PP,
HDPE, and HDPE/PP. It was found that the melt flow index
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THERMOPLASTIC STARCH
was reduced in case of PP but increased in case of HDPE
and HDPE/PP blends. The tensile strength was reduced for
all polymers with the addition of 30% of TPS. But for PP, a
drastic reduction was noticed suggesting TPS behaved as
nonreinforcing filler. The decrease in mechanical properties
of all the formulations can be justified by a phase separation
between the polyolefins and TPS. SEM analysis confirmed
the poor adhesion and interfacial interaction between PP,
HDPE, and TPS.
Kaseem et al. (2012) melt blended PP with TPS using a
single screw extrusion process and molded using injection
molding process to study the mechanical and rheological
properties of TPS/PP blends. The rheological properties
indicated that the viscosity of TPS was reduced by increasing
the glycerol content in TPS and the mechanical results indi-
cated that strain at break of blends was less than that of PP;
Young’s modulus of the blends was higher than that of PP.
TPS/PP have high crystallinity that helps to enhance its ten-
sile strength, hardness, and stiffness that are important fac-
tors in food packaging.
TPS/Polystyrene Blends. The availability of PS is in the
form of grades which usually vary in impact strength
between brittle and very tough. They are mostly used in air-
craft kit, containers (Ohno et al. 2001), light fittings, vending
cups (van der Harst and Potting 2014), and coils because of
their low cost coupling with ease of processing (Lochab and
Singh 2004).
Schlemmer et al. (2007) used solvent casting technique to
prepare TPS/PS blends. Glycerol and buriti oil were used as
plasticizers. TPS addition instigated thermal degradation in
PS in a rapid rate, mainly for higher ratios of TPS. Blends
prepared with glycerol degraded in more stages and at inferi-
or temperature compared to those obtained with buriti oil.
Mihai et al. (2007) studied the fabrication of extruded
foams from TPS/PS blends. Glycerol was used as a plasticiz-
er. It was concluded that the viscosity of TPS decreases by
increasing the glycerol content, hence, the viscosity ratio
between TPS and PS phase increases. It was further found
that glycerol content in the TPS phase and the TPS content
in the overall blend have a firm effect on the blend viscosity
and, hence, on the ability to foam the material.
TPS/PVA Blends. PVA has an atactic chain structure. OH
group is of small size that allows it to fit in the crystal lattice.
PVA is used in paper (Schuman et al. 2004), textile treat-
ments (Chen et al. 2013) and wet-strength adhesives (Tang
and Alavi 2011).
The conventional plasticizer which have been used for
TPS/PVOH blends are glycerol and water but there are vari-
ous other chemicals which are also being used successfully as
plasticizers like sorbitol (Yang et al. 2006), urea (Mihai et al.
7
THERMOPLASTIC STARCH
2007), citric acid (Xiaofei et al. 2004), and complex plasticiz-
ers (Tang and Alavi 2011).
Yoon et al. (2006) investigated the effect of functional group
type of plasticizers on the properties of starch/PVA blends.
Glycerol, malic acid, tartaric acid, and succinic acid were used
as plasticizers. It was found that hydroxyl and carboxyl groups
enhanced the strength and flexibility of the films. The tensile
strength and elongation were better when the additives having
both hydroxyl and carboxyl groups were added simultaneously
than in glycerol added film with hydroxyl groups only.
Zhou et al. (2009) studied the effect of complex plasticizer,
i.e., mixture of urea and glycerol, on the starch/PVA blends. It
was found that the complex plasticizer formed stronger and
more stable hydrogen bonds with water and starch/PVA mol-
ecules than the single plasticizer. So the blends with complex
plasticizer had better mechanical characteristics.
When PVOH is blended with TPS, the development of
surface cracks is prevented because both polymers are polar
substances consisting of hydroxyl groups in their chemical
structure, these polar hydroxyl groups tend to build inter-
molecular and intramolecular hydrogen bonds that enhance
the compatibility between TPS and PVOH in the blends.
The improved mechanical characteristics and compatibility
play a vital role in building strength in food packaging films.
TPS/PLA Blends. PLA is aliphatic polyester which is
derived from sugar and corn beets (Wardman and Abdrabbo
2010). It is degraded to nontoxic compounds in landfills.
PLA is used in biomedical and pharmaceutical fields such as
tissue scaffolds (Li et al. 2014), implant devices (Fu and Kao
2010), and internal sutures because it has a low molecular
weight and low cost (Liu et al. 2013).
Martin and Averous (2001) studied the mechanical and
rheological properties of TPS/PLA blends. It was found that
the least plasticized TPS was brittle and rigid while the most
plasticized TPS was ductile and flexible. The glycerol content
controls the viscosity of TPS in the melt phase and rigidity
in the solid form. It was noticed that the lack of affinity
between the TPS and PLA was the main limitation.
Wang et al. (2008) investigated the effect of different plas-
ticizers (water, glycerol, and formamide) on the properties
of TPS/PLA blends. The plasticizers were used alone or
mixed. It was found that formamide was the best among the
three for starch. Water depolymerized and deteriorated the
properties of TPS/PLA blends. On the other hand the com-
patibility and dispersion between PLA and glycerol plasti-
cized starch was poor (Hunealt and Li 2009).
Mihai et al. (2007) studied TPS/PLA blends and com-
pared the effect of two plasticizers (sorbitol and glycerol).
The granules of starch were plasticized by glycerol, sorbitol
and with the mixture of both as well. It was found that sor-
bitol plasticized blends had more modulus and tensile
strength as compared with the other plasticized blends.
8 Journal of Food Process Engineering 00 (2016) 00–00 Copyright V
B. KHAN ET AL.
Due to its low price and availability as compared to other
biopolymers, PLA is widely used in food packaging. The
resulting TPS/PLA film material offers very good moisture
barrier properties. In addition, it can withstand the rigors of
injection molding and vacuum- or blow-forming processes.
PLA is currently being utilized in the generation of loose-fill
packaging, food packaging, and in disposable food service
tableware items as well.
BIOBASED FOOD PACKAGING
The basic function of food packaging is to protect food
products from spoiling and undesirable external influences,
to maintain the food quality and also to give consumers
nutritional or ingredient information (Coles 2003). Food
packaging must be cost effective which meets the require-
ments of the industry and consumers demand. Food must
be safe in it and should minimize the environmental impacts
(Marsh and Bugusu 2007).
To design or manufacture the packaging material, one
should follow multistep procedure and must involve careful
considerations in order to engineer the proper packaging
with all the properties which are required (Andersen and
Hodson 1997). A packaging material should follow “cradle to
grave” cycle so disposal processes at the end of its life should
also be kept under consideration (Weber et al. 2002). For bio-
degradable packaging, starch is one of the best options that
comes in mind because it is natural, renewable and inexpen-
sive (Ramirez et al. 2011). It is very advantageous as it can be
altered by both chemical and enzymatic ways (Sarkheli and
Rahbari 2015). But the applications of native starch are limit-
ed due to few negative properties like, abnormal viscosity,
retrogradation, cold water insolubility and brittleness (Wurz-
burg 1986; Weber et al. 2002; Grommers 2009).
The hydrogen bonds and interatomic forces present in
starch resists native starch to be generated as a thermoplastic
material (Panaitescu et al. 2015). So, a plasticizer is needed
to produce a deformable thermoplastic material, called TPSs
(Niazi 2013). The plasticizer will help to increase the flexibil-
ity and process ability of starch well below its degradation
temperature. Glass transition temperature (Tg) will also be
reduced by the plasticizer (Karnnet et al. 2005). To improve
the performance of TPS, various plasticizers (glycerol (Mihai
et al. 2007), urea (Ma et al. 2006), formamide (Ma and Yu
2004), amino acid (Orts et al. 2007), sorbitol (Yang et al.
2006), and citric acid (Xiaofei et al. 2004) are used.
PERFORMANCE/ATTRIBUTES
OF PLASTICIZERS
Plasticizers are usually high boiling point liquids having the
average molecular weights between 300 and 600. They con-
tain linear or cyclic chains of carbon (14–40 carbons)
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B. KHAN ET AL.
FIG. 3. MICROSTRUCTURAL CHANGES OF STARCH BY PROCESSING WITH VARIOUS PLASTICIZERS
(Wilson 1995). As the molecular size of plasticizer is low, it
occupies the intermolecular spaces between polymer chains,
hence, the secondary forces among them are reduced (Dai
et al. 2009). These molecules effect the three-dimensional
organization of molecules of polymers and reduce the
amount of energy required for the motion of molecules and
hydrogen bond formation. As a result, the free volume
increases and the mobility of molecules are observed
(Wypych 2004). The degree of plasticity of a polymer is
mainly depends upon the chemical structure of a plasticizer
that includes molecular weight, chemical composition and
the functional groups (Moreno 1992). The selectivity of a
specific system is predominantly based on the components
compatibility; amount required for plasticization, required
thermal, electrical and mechanical properties, water resis-
tance, processing characteristics, toxic nature, and cost
(Cheng et al. 2006; Cao et al. 2009).
Journal of Food Process Engineering 00 (2016) 00–00 Copyright V
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THERMOPLASTIC STARCH
Compatibility between a polymer and plasticizer is very
important for an effective plasticization. This feature can be
indicated by various parameters like hydrogen bonding,
polarity, solubility, and dielectric constant (Donhowe and
Fennema 1993; Van Oosterhout and Gilbert 2003). Perma-
nence depends upon the volatility and resistance to migra-
tion/extraction in water, oils, and solvents. Hence, the
plasticizer should be of low vapor pressure and low diffusion
rate (Tena-Salcido et al. 2008).
Fig. 3 (Tajuddin et al. 2011; Niazi 2013) shows the “open
umbrella” structures of amylopectin filled with urea and the
“coated closed umbrella” strucutres of glycerol formulated
systems.
Classification of Plasticizer
In the field of polymers, plasticizers can be explained as
internal or external. Internal plasticizers are the inherent
9
THERMOPLASTIC STARCH B. KHAN ET AL.

TABLE 2. PLASTICIZER RELATED CHALLENGES et al. 2012; Imre and Pukanszky 2013) and Table 3 (Sothornvit
Challenge References and Krochta 2001; Galdeano et al. 2008) summarize various
plasticizer related challenges and their properties respectively.
Migration from plastic Foldes (1988)
Evaporation
Liquid leaching
BARRIER PROPERTIES
Solid–solid migration
Biodegradability Sun (2004) It is very crucial to estimate the shelf-life of the product-
Flexibility at high temperature Sin et al. (2012) and package. The specific barriers required for the package sys-
Starnes (2002)
tem are related to the characteristics of the product (Subirats
Lubricity at low temperature Rahman and Brazel (2004)
Environmental effects Imre and Puk anszky (2013)
et al. 2014). Usually, plastics are permeable to the molecules
Health effects Imre and Puk anszky (2013) like gas, water/organic vapors and also liquids (Hogg et al.
Flammability Carty and White (1999) 2014). Water vapor and oxygen are the two main permeates
Compatibility with polymers Krauskopf (1988) and that are studied in packaging applications because both can
Rahman and Brazel (2004) transfer from external or internal environment through the
Enhanced lifetime of the material Rahman and Brazel (2004) wall of polymer-package, varying the quality of product and
shelf-life (Siracusa et al. 2008; Anibal and Maria 2014). Light
parts of the polymer molecules and become part of the barrier properties also play a vital role in packaging as the
product that can react with the original polymer or co- light that passes through the packaging material can catalyze
polymerized into polymer structure (Frados 1976). The the oxidation reactions and reduce the shelf-life of the prod-
structure of internal plasticizer is usually bulky that gives uct (Borghetti and Coltro 2007).
space to move easily around to resist polymer from coming
Oxygen Barrier
close together. Hence, polymers become soft by the
decreased in glass transition temperature (Tg), as a result, The oxygen barrier property of packaging plays an important
the elastic modulus also decreases (Ahmad et al. 2012). On role in the preservation of fresh food products, e.g., salad, fruit,
the contrary, external plasticizers are added to the polymers and ready to eat meals (Nouri and Nafchi 2014). Oxygen per-
as a low volatile substance (Mekonnen et al. 2013). The meability coefficient (OPC) quantifies the oxygen barrier. It is
interaction between the plasticizer molecules and polymer the amount of oxygen that permeates per unit of area and time
chains takes place but it is not chemically bonded to them through the wall of packaging material (Siracusa et al. 2008).
by primary bonds, hence, can be lost by evaporation, migra- Low OPC of a polymer packaging film indicates that the pres-
tion or extraction (Niazi 2013). sure inside the food container drops to that extent where oxi-
The classification of plasticizers can also be done as pri- dation is retarded, hence increasing the product shelf-life
mary and secondary (Frados 1976). Primary plasticizers are (Auras et al. 2003). Usually the biodegradable polymers have
those in which a polymer is soluble at a high concentration. the OPC value one or more order of magnitude below the syn-
In this type, plasticizer gel the polymer rapidly and does not thetic polymer used in the similar field (Fu et al. 2012).
exude from plasticized material. On the other hand, second-
Water Vapor Barrier
ary plasticizers are those which have low gelation capacity
and compatibility with the polymers is limited. For the For all the packed material whose physical or chemical dete-
improvement in the properties of the product and reduction rioration is related to its equilibrium moisture content, water
in the cost, they are blended with primary plasticizers vapor barrier carries great importance for the maintenance
(Chanda and Roy 1986). and extension in shelf-life (Siracusa et al. 2008). The
Table 2 (Foldes 1988; Krauskopf 1988; Carty and White mechanical properties of starch films impede their wide use.
1999; Starnes 2002; Sun 2004; Rahman and Brazel 2004; Sin They are very sensitive to the direct contact with air and

TABLE 3. PROPERTIES OF PLASTICIZERS

Molecular Shape of Hydroxyls Concentration

Plasticizer Formula weight (g/mol) the chain number (g/100 g) References

Glycerol C3H8O3 92 Straight 3 20 Galdeano et al.

Urea CO(NH2)2 60 Straight 0 16 (2008), Sothornvit
Sorbitol C6H14O6 182 Straight 6 25 and Krochta
Sucrose C12H22O11 342 Ring 8 55 (2001), and
Sothornvit and
Krochta (2001)

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B. KHAN ET AL. THERMOPLASTIC STARCH

TABLE 4. CURRENT PACKAGING APPLICATIONS OF BIOPOLYMERS

Packaging Applications Biopolymer References

Starch Peelman et al. (2013)

Chocolates Cornstarch trays
Tomatoes Corn-based packaging
Cellulose Blakistone and Sand (2008) and Peelman et al.
Potato chips Cellulose films (2013)
Pasta Cellulose based packaging
Sweets Cellulose films
Kiwi Trays wrapped with cellulose films
PHA/PHB Bucci et al. (2005), Haugard et al. (2003), Lev-
Meat PHA/PHB packaging kane et al. (2008), Peelman et al. (2013), and
Cheese PHA packaging Weber et al. (2002)
Salad PHB packaging
Juices PHB packaging
PLA Nieburg (2010), Peelman et al. (2013), Sudesh
Tea, coffee PLA coating and Iwata (2008), Weber et al. (2002), and
Yoghurt PLA jars Weston (2010)
Cheese PLA packaging
Fresh cur Fruits, vegetables, salads PLA trays
Frozen fries PLA films
Carbonated water, dinks, juices PLA bottles
Poultry PLA bowls
Herbs, pasta, fruit, vegetables, sandwiches PLA packaging
Potato chips PLA bags
Beverages PLA cups

water and are permeable to water vapor (Schimidt et al.
2013). Water vapor permeability coefficient (WVPC) quanti-
fies the water vapor barrier. WVPC indicates the amount of
water vapor that permeates in packaging per unit area and
time (Auras et al. 2003). It is important to sidestep dehydra-
tion for fresh food items but for bakery/delicatessen, it is
very important to resist the water permeation (Anibal and
Maria 2014).
Carbon Dioxide Barrier
Carbon dioxide barrier property also has an importance in
food packaging applications just like the oxygen and water
vapor barrier properties. Carbon dioxide permeability coeffi-
cient (CO2PC) quantifies the carbon dioxide barrier (Pfeiffer
et al. 2011). CO2PC indicates the amount of carbon dioxide
that permeates in the packaging per unit area and time.
Light Barrier
Radiation energy from light (either ultraviolet or visible
light) significantly affects the photosensitive products
because it accelerates the photochemical degradation reac-
tions that may deteriorates such products. Moreover, poly-
mers also undergo oxidative degradation when exposed to
light leading to discoloration or weakening of the polymers.

TABLE 5. FUNCTIONS OF PACKAGING

Function Applications Example References

Protection Impact resistant packaging Egg packs/boxes Morgan (2010) and Barlow and
Morgan (2013)
Increase in product life Different barriers, making the Containing food items in a Hopewell et al. (2009) and
atmosphere inert, reduction in handling very protective atmosphere Yu et al. (2006)
Tamper—evidence Sealing the containers Metal can lids—removable Morgan (2010) and Ohring (2015)
Handling of product Containers, small items packed in clusters Box, bottle, bag, tray Barlow and Morgan (2013),
Morgan (2010), and Kropf (2014)
Advertisement or Written statements/pictures Labels, printing Barlow and Morgan (2013),
information Morgan (2010), and Wani and
Singh (2014)
Barrier Avoiding contact of environment or Packaging in multilayer form Barlow and Morgan (2013)
atmosphere with the product and Morgan (2010)

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THERMOPLASTIC STARCH
Ultraviolet absorbers/stabilizers can be used in packaging to
avert the photo-degradation of products (Borghetti and Col-
tro 2007). Hence, light barrier properties are very important
in food packaging as light catalyzes the oxidation of food
products.
PACKAGING APPLICATIONS OF
BIOPOLYMERS
Recent studies have investigated about the possible use of
biopolymers for food packaging, primarily in comparison
with the traditional packaging materials (Table 4; Weber
et al. 2002; Haugard et al. 2003; Bucci et al. 2005; Blakistone
and Sand 2008; Sudesh and Iwata 2008; Nieburg 2010; Peel-
man et al. 2013 and Table 5; Yu et al. 2006; Hopewell et al.
2009; Morgan 2010; Barlow and Morgan 2013; Kropf 2014;
Wani and Singh 2014; Ohring 2015). At the moment, it
looks like biopolymers are mainly for the fresh food items
like fresh meat or juices (Madival et al. 2009). Fat rich items
can also be packed with biopolymer packaging. For the pre-
sent moment, the focus of biodegradable food packaging is
on short life applications, dry food items (Imre and
Pukanszky 2013) and for those long shelf life applications
which do not need high water vapor/oxygen barriers (Auras
et al. 2003).
CONCLUSIONS
Biodegradable polymers are one of the most innovative
materials being generated in the packaging field. In order to
promote biodegradable polymers, it is necessary for our
society to strongly believe in environmental health. Biopoly-
mers meet the environmental issues but they also have the
limitations in the form of thermal resistance, oxygen/water
vapor barriers and other mechanical properties related with
costs. Hence, this type of packaging requires further research
in order to improve quality, shelf-life, nutritional values and
microbial safety. Moreover, the barrier properties need to be
enhanced.
Biodegradable polymers containing starch/cellulose fibers
are most likely to make a firm growth in applications. Starch
is a renewable, cheap and abundantly available biopolymer
but requires a plasticizer in addition of water to be used as a
deformable thermoplastic material called TPSs.
Other plastics have also been used in packaging but they
cannot be degraded naturally and are left as waste causing
environmental damages. Burning and burying are two most
commonly used methods to destroy the packaging waste but
these are not suitable for plastics. Microbial polymers are
also very promising but they still need to be more cost effec-
tive. Nowadays biodegradable packaging materials are used
for those food products, which do not need high oxygen/
12 Journal of Food Process Engineering 00 (2016) 00–00 Copyright V
B. KHAN ET AL.
water vapor barrier. It can be concluded that biobased poly-
mers have great potential for the food-packaging field.
ACKNOWLEDGEMENTS
This study was supported by National University of Sciences
and Technology (NUST), Islamabad, Pakistan. There is no
conflict of interest statement in the manuscript.
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