1  Polyethylene Terephthalate: Blends,

Composites, and Nanocomposites – State

of Art, New Challenges, and Opportunities

Visakh P.M.
Department of Ecology and Basic Safety, Tomsk Polytechnic University, Tomsk, Russia

O U T L I N E

1.1 Modification of Polyethylene Terephthalate 1

1.2 Reinforcement of Polyethylene Terephthalate via Addition of Carbon-Based Materials 2
1.3 Polyethylene Terephthalate-Based Blends: Thermoplastic and Thermoset 3
1.4 Polyethylene Terephthalate-Based Blends: Natural Rubber and Synthetic Rubber 4
1.5 Characterization of Polyethylene Terephthalate-Based Composites and Nanocomposites 4
1.6 Polyethylene Terephthalate: Copolyesters, Composites, and Renewable Alternatives 5
1.7 Molecular Weight Determination of Polyethylene Terephthalate 6
1.8 Degradation Kinetic Parameter Determination of Blends Containing Polyethylene
Terephthalate and Other Polymers with Nanomaterials 6
1.9 Modification of Polymer Composites by Polyethylene Terephthalate Waste 7
1.10 Highly Functionalized Polyethylene Terephthalate for Food Packaging 7
References 8

1.1  Modification of Polyethylene of biomolecules. Plasma modification of PET has

Terephthalate
Polymer films need additional surface treatments
to modify the surface properties, for better wettabil-
ity and adhesion activities [1–5]. There are different
methods to modify the surface properties of the poly-
mer films such as chemical or plasma treatments, ul-
traviolet (UV) or laser irradiation.
Polyethylene terephthalate (PET) was selected
for study on the basis of the reactivity of its es-
ter group. This polymer was studied in order that
good protein adsorption could be achieved onto
the polymer surface [6–9] by utilizing the methods
discussed hereinafter. PET has excellent mechani-
cal strength, good stability against body fluids,
and high radiation resistance for sterilization, but
its surface is not favorable for the immobilization
Poly(Ethylene Terephthalate) Based Blends, Composites and Nanocomposites. http://dx.doi.org/10.1016/B978-0-323-31306-3.00001-4
Copyright © 2015 Elsevier Inc. All rights reserved.
been studied by some workers, and changes in the
physical behavior and surface morphology have
been reported [10–12].
PET has a variable density of zones: a density
characteristic of amorphous areas and the crystalline
areas. The crystalline region variations in density are
attributed to crystal defects caused by the crystalliza-
tion conditions and the amorphous density variations
from conformational restrictions. The orientation of
the macromolecules of PET is identified in the litera-
ture to be due to trans conformer transformation in
the gauche conformer.
The interfacial tension from the PET surface is
reduced just after plasma treatment due to the rapid
migration of the polar segments towards the bulk
of the polymer. A fraction of the functional groups
is transformed into stable structures at the surface
1
2 Poly(Ethylene Terephthalate) Based Blends, Composites and Nanocomposites
itself, diminishing the surface hydrophilicity. Some
authors [13–16] have reported similar observations
for the plasma-treated PET films, and have correlated
them with the reorganization of the surface, as well
as surface contamination during storage.
UV treatment requires a light source that directs
UV or visible light onto the formulated product.
The substrates absorb the UV energy from the light
source, starting a chemical reaction that quickly
converts them onto a solid functionalized surface,
forming monomers and oligomers. Monomers are
low molecular weight materials that can be mono- or
multifunctional molecules, depending on the num-
ber of reactive groups they possess. Because reactive
functional groups of the substrates appear during ex-
posure to UV light, certain new properties are present
on the surface of the polymer.
Some authors reported studies on different poly-
mers: polypropylene, polystyrene, polycarbonate,
styrene acrylonitrile copolymer, and poly(methyl
methacrylate) UV irradiated for various times [17].
The photodegradation related to the extinction co-
efficient in the UV region generated the accumu-
lated layer of the degraded species. The individual
and combined effects of UV light combined with
ozone have been studied for many different sur-
faces, including polypropylene, polyethylene, PET,
poly(ether ether ketone), and polystyrene. The
surface energy of the polymers increases through
the breaking of the polymer chain by insertion of
oxygen-containing functional groups due to the ul-
traviolet treatment. Studies of PET treatment and
UV light treatment with excimer UV laser irradia-
tion [18] show a partial surface destruction, caused
by thermal effects due to the extremely high pulse-
energy density.
Collagen is the foundation of the extracellular ma-
trix in a variety of connective tissues including bone,
dentin, cartilage, tendons, dermis, and cornea, and
the major structural protein in animals, comprising
up to 30% of total protein weight [19,20]. The most
attractive feature of plasma and UV processing is that
by exerting proper control over the exposure condi-
tions, a tailored surface with desired chemical func-
tionality and morphology may be produced. There
are specific biological and chemical criteria that must
be taken into consideration when modifying surfaces
for biomaterial applications.
In the case of plasma treatment, while the surface
roughness is not expected to change with time, the
hydrophilicity of plasma-treated PET was found to
decrease with time by contact angle measurements.
1.2  Reinforcement of Polyethylene
Terephthalate via Addition of
Carbon-Based Materials
Carbon-based materials including carbon nano-
tubes (CNTs), carbon fiber, and graphene have ex-
traordinary thermal conductivity and mechanical and
electrical properties, thus finding applications as ad-
ditives to various structural and functional materials.
When they are incorporated into a PET polymer matrix,
the resulting composites have significantly different
electrical, mechanical, and physical–chemical prop-
erties than the original.
When CNTs, multiwalled or single walled, are in-
corporated into a PET polymer matrix, the resulting
nanocomposites can have electrical properties that
differ from pristine PET [21,22].
PET reinforced by graphene has been prepared by
a combination of solution and melt processing and
has improved mechanical properties [23]. This rein-
forcement has been predominantly attributed to the
dispersion quality resulting from the solvent exfolia-
tion of both nanotubes and graphene. PET/graphene
nanocomposites were prepared by melt compound-
ing and have enhanced the electrical conductivity
of PET, resulting in a sharp transition from electri-
cal insulator to semiconductor with a low percola-
tion threshold of 0.47 vol% [24]. PET is beginning
to show promise in industrial applications [25–27].
Although promising, the disadvantages, like insuf-
ficient mechanical properties and thermal stability
and other functional requirements in new fields, have
restricted PET’s practical application in industry. In
this regard, research has been extensively performed
to find high performance PET [28–30].
As CNTs have excellent electrical, thermal, and
mechanical properties, a number of efforts have
been made to incorporate CNTs into PET to develop
high performance nanocomposite polymers, in fields
ranging from basic science to industrial applications
[31]. Thus, CNTs can greatly make up for the dis-
advantage of PET. PET/CNT composites are pre-
pared by melt compounding metallized polyethylene
terephthalate/nanotubes (M-PET/NTs). M-PET was
also processed with the same procedure of melt com-
pounding as reference [32].
The PET nanocomposites containing isocya-
nate groups showed improved mechanical proper-
ties, including tensile strength and tensile modulus,
compared with those with pristine and acid-treated
nanotubes [33]. Various matrix polymers such as
polyethylene, polystyrene [34,35], and PET [36]
1:  Polyethylene Terephthalate 3
have been tested and various mechanical properties
such as tensile and bending strengths and moduli,
yield stress, fracture toughness, fatigue, and friction
have been investigated. It has been proved that con-
ductive polymer composites with high electrical con-
ductivity and modified mechanical properties at low
CNT loadings can be obtained by preparing in situ
microfiber-reinforced PET/CNT composites through
extrusion and hot stretching.
From the literature the effect of CNTs on the rate
of PET crystallization has been investigated through
differential scanning calorimetry in transient and
isothermal modes, carried out on nanocomposite
samples of PET, melted with single walled carbon
nanotubes at concentrations of 0–3 wt%.
The various kinds of fillers dispersed in PET can
increase the mechanical properties of polymers such
as tensile strength, modulus, and fracture toughness.
Among the fillers, CNTs have a large aspect ratio
[37,38]. By using the properties of CNTs, many
excellent properties of composite materials can be
produced. For example, the plastics reinforced with
CNTs have excellent mechanical properties, good
conductivity, corrosion resistance, and can shield ra-
dio waves.
Usually, the carbon fibers have been blended into
PET matrices using conventional mixing methods,
for example a twin-screw extruder [39–41], a high
shear mixer [42,43], as well as a two-roll mill [44].
G. Morales et al. [45] prepared CNF/PET composites
by compounding methods included ball milling, high
shear mixing in the melt, as well as extrusion using
a twin-screw extruder. G. Morales et al. [46] studied
PET/short carbon fiber composites by melt extrusion
processing. Carbon fiber-reinforced polybutylene
terephthalate (PBT) composites have shown superi-
ority due to their outstanding mechanical properties
as well as their light-weight characteristics [47].
J. Martinsson et al. [48] studied the recycled car-
bon fiber-reinforced PBT. The mechanical properties,
heat distortion temperature, and thermal stability of
PBT could be significantly improved by incorpo-
rating this surface-treated carbon fiber. Carbon-
reinforced PET materials have extensive application
in the area of health monitoring for the employment
of neural networks [49].
PET fibers are most extensively used in tex-
tiles and can be produced with Young’s modulus,
strength, and tensile toughness up to ∼10 GPa,
∼1 GPa, and 200 MJ/m3, respectively [50]. However,
one merit of PET fibers is that they can be melt-spun,
cheaply and in large quantities [51].
1.3  Polyethylene Terephthalate-
Based Blends: Thermoplastic
and Thermoset
PET blends can be typically prepared by five tech-
niques: graft copolymerization, melt solution, latex
blending, partial block, and synthesis of interpene-
trating networks. Melt blending is a simple mechani-
cal process of creating a homogeneous mixture of
two or more polymers. The major advantage of melt
blending is the absence of any solvents that might be
required in other methods of polymer blending [52].
PET possesses hydroxyl and carboxyl functional
groups at chain ends; in situ or reactive compati-
bilization is an effective approach for developing
engineering thermoplastic blends from these materi-
als. Sometimes, a reactive coupler, such as epoxide
moiety, maleic anhydride, glycidyl methacrylate, etc.,
is used to compatibilize thermoplastic PET blends.
The combination of PET with polyolefins represents
yet another important group of PET blends. The use
of recycled scrap from PET and polyolefins for eco-
logical reasons, especially from soft drinks bottles,
etc., is the main reason for developing blends of PET
with polyolefins. High-density polyethylene (HDPE)
and PET contain a major portion of postconsumer
waste and are recycled to reduce waste, especially
from packaging. Blending of these polymers is an al-
ternative method to reduce waste. However, HDPE
and PET are immiscible [53]. Through a proper
compatibilization strategy, the blends can combine
the stiffness (dimensional stability) of PET with the
good impact strength of HDPE.
Akkapeddi and Van Buskirk [54] studied the com-
patibilization of postconsumer PET/HDPE blends.
The melt blends were prepared in a single-screw
extruder and a corotating twin-screw extruder. Ini-
guez et al. [55] studied the morphological stability
of postconsumer PET/HDPE blends at different com-
positions (10–90% by volume of PET in HDPE) with
and without a compatibilizer. Kim et al. [56] studied
the compatibilization of PET/HDPE blends. High-
density polyethylene grafted with the blocked iso-
cyanate group was used as a reactive compatibilizer
for an immiscible PET/HDPE blend.
Murff et al. [57] prepared a melt blend of polycar-
bonate and PET by continuous extrusion and injec-
tion molded it into bars to study their thermal and
mechanical behavior. Huang [58] studied and dis-
cussed the mechanism, morphology, and mechani-
cal properties of PET/PA-6 (polyamide-6) blends
with low molecular weight bisphenol-A epoxy resin
4 Poly(Ethylene Terephthalate) Based Blends, Composites and Nanocomposites
(E-44) as a reactive compatibilizer. Imashiro et al.
[59] have described adding a carbodiimide compound
to recycled PET such that the intrinsic viscosity
and strength of the polyester resin during processing
are retained.
1.4  Polyethylene Terephthalate-
Based Blends: Natural Rubber
and Synthetic Rubber
PET is a very important engineering thermoplas-
tic polyester because of its excellent chemical resis-
tance, good mechanical and thermal properties, as
well as its excellent optical and barrier properties,
which make PET an ideal candidate for use as bever-
age bottle applications.
The effect of compatibilization between rubber
and a PET matrix has been observed to play an im-
portant role in the resulting blend’s behavior [60–62].
Rubber modification gives an effective method for
enhancing the impact behavior of notch-sensitive
PET [63,64]. The main role of the dispersed rubber
particles is to induce a global deformation mecha-
nism, rather than a localized type.
Based on theories of rubber toughening [65],
blend morphologies and characteristics, such as av-
erage rubber particle size and concentration of the
dispersed phase, will have distinct influences on
the final mechanical properties. The PET/NR (natu-
ral rubber) blends are normally prepared in the labo-
ratory via mixing in a Banbury mixer or Brabender
Plasti-Corder attached to a mixer or a twin-screw
compounder. The dried PET is first melted in the
mixer and then masticated NR is added [66]. Addi-
tives, such as compatibilizers or stabilizers are added
before the addition of the NR [67].
An unstable morphology and poor interfacial ad-
hesion will result in a blend with poor mechanical
properties. To viably develop a PET/NR blend with a
desired fine phase morphology, the use of a reactive
compatibilization strategy plays an important role,
when two polymers are immiscible. Blends of PET
and NR were prepared by Phinyocheep et al. [68] in
different ratios by the twin-screw extruder technique.
PET is dried in an air oven at 120°C for 10 h in order
to avoid excessive moisture-induced degradation re-
actions, before processing in a corotating twin-screw
extruder. The notch sensitivity of PET becomes
quite apparent from the very low notched Izod im-
pact strength (6.0 J/m) that was obtained by passing
the PET in the twin-screw extruder before injection
molding into test specimens.
PET/NR blends possess excellent properties, such
as reduced permanent set, improved mechanical
properties, greater resistance to attack by fluids, im-
proved high temperature utility, etc. [69], and there-
fore provide very useful and attractive applications in
different fields, for example automotive parts, build-
ing materials and construction equipment, wire and
cable insulation, etc. [70]. PET/NR blends are gener-
ally used for making automobile parts where opera-
tions such as abrasion, flexing, and tear are prominent
factors leading to the fracture of the products [71].
PET is an engineering plastic and is widely used
as an engineering thermoplastic often in packaging,
electronics, and other applications [72]. PET online
viscosity presents a substantial decrease, due to ther-
momechanical degradation at the processing condi-
tions [73]. It is important to note that the viscosity
variation with shear rate, in the physical blends, is
such that the viscosity curves lie above the PET curve.
The rubber particles infuse an increasing resistance
to flow, as observed in polymer-filler systems [74].
Lashgari et al. [75] reported that PET/ABS
(poly(acrylonitrile-co-butadiene-co-styrene)) blends
with more ABS content have higher impact resis-
tance, thus attesting to the good impact property of
ABS. On the other hand, the impact strength of the
blends increases with MAH content, a finding that
suggests that using grafted ABS, instead of neat
ABS, enhances the impact strength through the com-
patibilizing process, because of the bond formation
between functional groups of PET and ABS-g-MAH.
1.5  Characterization of
Polyethylene Terephthalate-Based
Composites and Nanocomposites
PET is a plastic resin and is the most common
type of polyester used commercially. It is also one of
the most recycled plastics in the market. Microstruc-
ture and mechanical properties of PET can be signifi-
cantly controlled by tailoring crystallization rate and
degree of crystallinity with use of additives [76–79].
The role that nanoparticles play in the crystallization
behavior of PET nanocomposites is widely reported
in the literature [80,81]. Ou et al. [82,83] in their re-
port have suggested that half-life of crystallization
can be lowered on clay intercalation in PET.
Investigations by Barber et al. [84] have shown that
the incorporation of organically modified montmoril-
lonite (MMT) clays, such as Cloisite® 30A, via solution
blending can significantly increase the crystallization
temperature while lowering the crystallization half-time.
1:  Polyethylene Terephthalate 5

Entezam et al. [85] suggested that the localization of 1.6  Polyethylene Terephthalate:
nanoclay in the blend systems can be detected by ana- Copolyesters, Composites, and
lyzing changes in crystallization temperature and crys-
tallinity of polymer components of the blend systems. Renewable Alternatives
The tensile test studies revealed that tensile strength of
PET is used for a broad range of applications, es-
the blend systems was affected by localization of nano-
pecially bottles for soft drinks. It can also be used for
clay in the matrix phase only. Davis et al. [86] reported
flexible packaging and electronics, for solar panels, or
the preparation of PET-based nanocomposite via melt
as textile fibers and fabrics, among many other appli-
blending using a corotating mini twin-screw extruder
cations [95]. PET is resistant to microbial attack and
operated at 285°C. They used 1,2-dimethyl-3-N-alkyl
does not degrade under normal environmental condi-
imidazolium salt modified MMT (hexadecyl-MMT)
tions [96], requiring instead very severe chemical deg-
as the filler. Organoclays with various contents of hy-
radation approaches [97,98]. In this case, recycling
droxyl groups and absorbed ammonium were prepared
plays an important role and has been extensively pro-
and compounded with PET, forming PET/clay nano-
moted for PET, albeit the impossibility of recovering
composites via melt extrusion [87].
it indefinitely persists. Composite materials are pre-
Nanocomposites of PET with different types of
pared using vegetable substrates, for example, fibers
organoclays were prepared using the melt mixing
from sisal [99], rice husks [100], wood flour [101],
technique by Papageorgiou et al. [88]. Two types of
and sawdust [102].
commercial inorganic clays (Laponite-synthetic hec-
Some interesting publications in the field include
torite and Kunipia-montmorillonite) were studied after
the study of Corradini et al. [103] on composites of
cation exchange with hexadecyltrimethylammonium
recycled PET and sugarcane bagasse fiber, which ap-
bromide while two commercial organo-modified
pears to be a good alternative to obtain environmental-
MMT clays (Nanomer I.30E modified with primary
ly friendly products. According to the authors, the use
octadecylammonium ions and Cloisite 10A modified
of compatibilizing agents, namely ethylene/n-butyl
with quaternary dimethyl benzyl hydrogenated-tallow
acrylate/glycidyl methacrylate, and ethylene-methyl
ammonium ions) were also investigated. Pegoretti et al.
acrylate copolymers, increased the interfacial adhe-
[89] studied the dispersion of two different types of
sion of recycled PET and sugarcane bagasse fibers.
clay in recycled PET. Various amounts (1, 3, and
Dehghani et al. [104] manufactured recycled PET/date
5 wt%) of a nonmodified natural MMT clay (Cloisite
palm leaf fiber composite materials using a twin-screw
Na+) or of an ion-exchanged clay modified with qua-
extruder followed by injection molding. The ensuing
ternary ammonium salt (Cloisite 25A) were dispersed
composites showed lower thermal stability, higher
in recycled PET by a melt intercalation process.
crystallinity, and superior mechanical properties. Fot-
Zheng and Wu [90] in their study have shown that
so Talla et al. [105] prepared PET/hemp fiber compos-
nanosilica does not behave as a nucleating agent but
ites by melt processing for engineering applications
rather retards the appearance of the microcrystalline
and investigated the effects of fiber concentration
phase that enhances spinnability. Liu and coworkers
(1, 5, 10, 15, and 20 wt%) and the use of additives,
[91–93] have carried out extensive research on silica/
namely poly(ε-caprolactone) (PCL), PCL/glycidyl
PET nanocomposites. The effect of the nanoparticles
methacrylate, PCL/pyromellitic dianhydride, and
on the crystallization temperature and the melting
PCL/clay, on mechanical and structural properties.
point of the polymer, and also on the mechanical
According to the results, the elastic modulus and max-
behavior of PET, are extensively reported by them.
imum strength of the composites increased with fiber
The PET/LDH_DBS (layered double hydroxide_ do-
concentration, while the strain at break decreased.
decyl benzene sulfonate) nanocomposite possesses
Kiziltas et al. [106,107] prepared composites
the highest thermal stability and the largest charred
using polyethylene terephthalate-co-trimethylene
residue. PET/graphene nanocomposites with uni-
terephthalate (PET-co-PTT) blends as matrix and mi-
form dispersion were prepared by melt compound-
crocrystalline cellulose as filler by melt compounding
ing by Zhang et al. [94]. Graphene nanosheets were
followed by compression molding. Ershad-Langroudi
prepared by complete oxidation of pristine graph-
et al. [108] reported the fabrication of polypropylene
ite followed by thermal exfoliation and reduction.
(PP)/recycled PET/chopped rice husk (CRH) com-
The incorporation of graphene greatly improved the
posites by melt mixing. The incorporation of recycled
electrical conductivity of PET, resulting in a sharp
PET improved the tensile modulus of the composites
transition from electrical insulator to semiconductor
and, at the same time, reduced its tensile strength. In
with a low percolation threshold of 0.47 vol%.
6 Poly(Ethylene Terephthalate) Based Blends, Composites and Nanocomposites
addition, the flexural modulus increased by 44% and
the impact strength increased threefold compared
to the PP/CRH matrix. These results pointed out the
ability of recycled PET to be used in the PP matrix as
reinforcing agent. Zou et al. [109] reported a unique
approach to reuse the waste PET/cotton blend fabrics
from the textile industry to develop composites for
various applications without the need of plasticizers,
additional matrix, or reinforcing agents. According to
this study, cotton acts as the reinforcing material and
PET, which melts during hot compression molding,
acts as the matrix; hence, there is no need to separate
cotton from PET.
The work of Canetti and Bertini [110,111] de-
scribed PET/lignin composites compounded by a
single-screw extruder. The supermolecular structure
and the thermal properties of the obtained composites
were assessed and the results revealed that the well-
dispersed lignin particles in the PET matrix enhanced
the crystallization rate, crystallinity, and crystal di-
mensions of PET by acting as a nucleating agent.
1.7  Molecular Weight Determination
of Polyethylene Terephthalate
PET is a semicrystalline polymer with excellent
chemical resistance, melt mobility, and spinnability
[112]. This polymer contains repeating units of tere-
phthalic acid and ethylene glycol. Each unit of the
polymer possesses a molecular weight of ∼200 Da.
When prepared from the reaction of terephthalic acid
and ethylene glycol, a water molecule is liberated
during the reaction, which must be removed under
high temperature and vacuum. The distribution of
molecular size depends on the synthesis of the poly-
mer. The fundamental characteristics of a polymer
determine all the other properties of the polymer,
such as cohesive forces, packaging density, potential
crystallinity, and molecular mobility of the polymer;
this means the total behavior of the polymer depends
on the molecular weight distribution [113,114].
The molecular weights of PET polymers used for
various purposes are important and affect their me-
chanical and physical properties significantly. If mo-
lecular weight is too low, the transition temperatures
and mechanical properties generally are also too low
for the polymer material to have any useful commercial
applications. A useful polymer must have transition
temperatures above room temperature, and it should
have mechanical properties sufficient to bear design
loads. Different grades of PET require different mo-
lecular weight requirements. Moreover, the molecular
weight of PET polymers significantly affects its degra-
dation and thereby its environmental fate [115].
Gel permeation chromatography (GPC) is a size
exclusion chromatography that separates analytes
basing on their molecular weight. It was first devel-
oped in 1955 by Lathe and Ruthven. The term GPC
was coined by J.C. Moore of Dow Chemical Com-
pany in 1964. GPC is accepted as a rapid and reliable
technique compared to other techniques in determin-
ing the molecular weights of polymers. GPC was a
practical method for the determination of molecular
weights of PET fibers even with 1 mg sample size.
This method is reproducible and accurate for micro-
gram analysis and can be used for comparison to de-
termine if two given PET fibers originate from the
same source. This practical method can be used for
the comparison of all kinds of polymers and plastics.
This method, although simple, may have significant
impact on the characterization of PET fibers.
PET is an unmanageable polymer for the determina-
tion of molecular weights by GPC. Initially, m-cresol
was used as the mobile phase for the elution of PET
using GPC; due to the viscous nature of this solvent,
a higher column temperature (125°C) must be used,
which leads to polymer degradation. Other solvents
used in GPC for PET are a mixture of nitrobenzene and
tetrachloroethane at room temperature; degradation of
PET was not observed for several months [116].
Sreenivasan and Nair determined the molecular
weight distribution of PET by GPC using chloroform
as a solvent. In their method, first, PET is dissolved
in 1:1 (v/v) chloroform and phenol at 50°C, and then
1 mL of this solution is diluted four times with chlo-
roform. The direct calibration method is employed
for the determination of weight average molecular
weights of the PET samples.
1.8  Degradation Kinetic Parameter
Determination of Blends Containing
Polyethylene Terephthalate and
Other Polymers with Nanomaterials
PET has been rigorously studied in the past from
a degradation standpoint where several authors have
published a number of mechanisms concerning its
degradation, which can be found in open literature.
Yet, the study of polymer blends under different heat-
ing conditions has been neglected. This route can
aid in a number of areas in engineering problems.
Municipal solid waste feed to thermochemical treat-
ment units, and in particular pyrolysis reactors, is
1:  Polyethylene Terephthalate 7
a commingled polymeric blend. Zohdy et al. [117]
studied the thermal degradation of PET in thermo-
gravimetric analyses  using a 10°C/min heating rate
and compared it with PET grafted with acrylonitrile,
styrene, and acrylamide. PET started decomposing at
around 300°C and the value of the activation energy
(Ea) was estimated at 140 kJ/mol using the Anderson
and Freeman method for zero-order kinetics.
Vassiliou et al. [118] evaluated the degradation
kinetics of PET nanocomposites prepared by in situ
polymerization with MMT modified with triphe-
nylphosphine and fumed silica nanoparticles (SiO2).
As previously indicated, studying the blends of poly-
meric materials considering their thermal degradation
and stability is scant in the literature. PET/PMMA
(polymethyl methacrylate) blends were investigated
in the past and the behavior under pyrolysis condi-
tions was established. The PET polymer in the blend
will start decomposing after the PMMA has started
degrading. This will affect both the PET and PMMA
degradation kinetics and vice versa. PET has a melt-
ing point of 260°C (≈530 K) and in pyrolysis condi-
tions it starts decomposing at around 310–450°C.
Virgin PET and PMMA were studied by Holland
and Hay [119] for their kinetic parameters in noniso-
thermal conditions estimation using different methods,
namely Ozawa, Coats and Redfern, and Friedman
methods at different heating rates (1–8°C/min). It
was reported that the apparent Ea for PMMA was
210 kJ/mol, while the apparent Ea for PET ranged
between 170 and 250 kJ/mol. Motaung et al. [120]
reported the behavior of PMMA/zirconia nanocom-
posites, where the addition of nanoparticles reduces
the activation energy at higher conversions. PMMA
activation energy was also reported in the Lopez et al.
[121] study in nonisothermal (dynamic) thermogra-
vimetry, ranging between 164 and 169 kJ/mol with
heating rates reported between 2.5 and 20 K/min.
The determination of the kinetic parameters of blends
represents a challenge in such cases, where models
available in the literature cannot represent the exact
behavior of the blend in pyrolysis conditions.
1.9  Modification of Polymer
Composites by Polyethylene
Terephthalate Waste
PET waste is among the most intensively studied
plastic waste capable of replacing natural aggregate
in cement composites [122]. An interesting method
of the concrete modification by means of PET waste
was presented Choi et al. [123]. Silva et al. [124] in-
vestigated the behavior of waste PET fibers in the ma-
terials based on Portland cement. These were mortar
samples having a composition of cement:sand = 1:3,
provided that the water:cement ratio = 0.61. A great
deal of information on recycling waste PET is provid-
ed in the context of unsaturated polyester resin syn-
thesis [125–127], which can then be used, e.g., as a
binding material in resin concretes. Rebeiz [128,129]
showed that the concrete, the binder of which is the
unsaturated polyester resin obtained from the PET
waste, has a higher strength compared with conven-
tional concretes.
Ignacio et al. [130] investigated that the type of cur-
ing system also influences concrete strength based on
the unsaturated polyester resin obtained by the PET
waste synthesis. The application of methacrylic acid
and maleic anhydride allows one to achieve higher
mechanical properties when compared to a conven-
tionally used isophthalic acid. On the other hand,
sebacic acid and maleic anhydride were used as a
curative system. Additionally, apart from endurance
tests, chemical resistance tests of obtained concrete
samples under the influence of aggressive media
were conducted by other authors [131]. The concretes
received by Tawfik and Eskander [132], the composi-
tion of which consisted of 12% by weight of unsatu-
rated polyester resins synthesized with PET waste and
88% by weight of sand and marble waste, showed
good chemical resistance to 20% sodium carbonate
(Na2CO3), 10% sodium hydroxide (NaOH), tap water,
groundwater, and seawater. Some authors [133] decid-
ed to investigate composites free of cement while us-
ing the waste material, which constitutes a significant
environmental problem. Composites made of PET
received from waste beverage bottles and sand were
tested. The bottles were crushed and converted into
fibers, which were then melted with sand at a tempera-
ture of 180–200°C. The results of the study showed
that the bending strength and compressive strength
and flexibility of the composites were improved. An
additional advantage of the obtained composites was
their marginal water absorption.
1.10  Highly Functionalized
Polyethylene Terephthalate
for Food Packaging
The high gas-barrier properties for food packag-
ing can be added to plastic packaging materials either
by coating a thin dense layer onto the polymer or by
8 Poly(Ethylene Terephthalate) Based Blends, Composites and Nanocomposites
mixing the rigid filler materials into the polymer ma-
trix. Garbassi and Occhicllo [134] reported the SiOx
deposition from siloxane monomers such as hexa-
methyldisiloxane (HMDSO) and tetramethyldisilox-
ane in the presence of O2 and/or CF4. The preliminary
data showed that the barrier properties of the coat-
ing from HMDSO/O2/CF4 mixtures were similar to
or better than those of the coating from HMDSO/O2.
Bieder et al. [135] reported the water vapor per-
meability of SiOx films deposited on PET films by
plasma-enhanced chemical vapor deposition with the
mixture of HMDSO and O2.
Schmachtenberg et al. [136] reported the SiOx
deposition on PET films using the HMDSO/O2 plas-
ma excited by a microwave energy source, studied
in contrast to the usual radio frequency excitation.
Deilmann et al. [137] also reported the correlation
between the O2 permeation and the layer composition
along with the activation energy of the permeation.
Furthermore, Deilmann et al. [138] also investi-
gated the influence of the coating composition on
the permeation barrier properties of SiOx films and the
mechanism of the residual permeation. Schneider
et al. [139] reported the use of the electron cyclo-
tron resonance (ECR) plasma source for SiOx barrier
coatings on PET foils in order to improve the O2 bar-
rier properties. Sufficient gas-barrier improvement
could be achieved by a diamond-like carbon (DLC)
film coated on PET bottles with a thickness of less
than 10 nm. A thinner DLC film could exhibit more
colorless clarity and higher transparency than the
rather thick current DLC film with a slightly brown
color, which has limited the applications of the cur-
rent DLC only to some specific product categories by
Yamamoto et al. [140]. Inorganic filler/PET compos-
ites have attracted interest as a way to improve the
mechanical properties and gas-barrier properties of
polymer matrix [141,142].
Among the various kinds of clays with layered
structures, MMT has been widely used in the PET/
clay composites for food packaging [143]. MMT
is the natural clay of phyllosilicate minerals, which
consist of multiple layers of silicate aluminum ox-
ide with the dimension of 100 × 100 × 1 nm. Wang
et al. [144] reported that MMT/PET composites with
1 wt% of MMT showed 25% higher tensile modu-
lus than pure PET. Other properties such as bending
modulus and bending strength were also increased.
The enhancement of the mechanical properties is due
to the large specific area and surface-active centers
promoting the physical or chemical interactions be-
tween MMT and the polymer matrix. In consequence,
MMT adhered strongly to the polymer matrix, which
could disperse the mechanical energy into the sur-
rounding matrix. It was also found that MMT could
act as a nucleating agent and help the crystallization
of the polymer matrix.
Ghasemi et al. [145] reported the effects of uniaxial
drawing of MMT/PET composites on the mechanical
and gas-barrier properties of the composites. After
drawing up to 65% of strain, O2 permeability was
decreased by 23% and the tensile modulus was in-
creased by about 20% as for the MMT/PET compos-
ites with 3 wt% of MMT. However, at the same time,
the clarity of the composite was decreased by about
15% due to the increase in the crystallinity caused by
the existence of MMT.
Yuan et al. [146] reported AT/PET composites, in
which AT was modified by organic phosphonium for
the intercalation and by a silane coupling agent for the
decrease of AT aggregations. PET was then synthe-
sized through in situ polycondensation in the presence
of modified AT. Yoo et al. [147] also reported the MW-
CNT/PET composite with functionalized multiwalled
carbon nanotube (MWCNT) with improved mechani-
cal properties. In their studies, COOH, benzyl, and phe-
nyl groups were introduced to MWCNT by acid treat-
ment. The modulus of the MWCNT/PET composites
with the phenyl-CNT concentration of 3 wt% increased
to 1200 MPa, while that of pure PET was 800 MPa.
Yesil and Bayram [148] reported the MWCNT/
PET composite with acid-functionalized MWCNT.
Here, the surface of the MWCNT was functionalized
by treatment with a strong acid mixture of HNO3
and H2SO4. The MWCNT was then modified with
sodium dodecyl sulfate (SDS), polyethylene glycol
(PEG), and bisphenol A diglycidyl ether (DGEBA).
The number of carboxylic acid groups on the MW-
CNT surface was decreased by the modification pro-
cesses, and thus it was assumed that the carboxylic
acid groups were actually reacted with PEG, DGE-
BA, and SDS.
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