Polymer Degradation and Stability 80 (2003) 373–382

www.elsevier.com/locate/polydegstab

A mechanical analysis on recycled PET/HDPE composites

Antonio F. Ávilaa,*, Marcos V. Duarteb
a
Department of Mechanical Engineering, Mechanics of Composites Laboratory, Universidade Federal de Minas Gerais, 6627 Antonio Carlos Avenue,
Belo Horizonte, MG 31270-901, Brazil
b
PETROBRAS, CEMPRES, PETROBRAS Research Center, Ilha do Fundão, Rio de Janeiro, Brazil

Received 5 July 2002; received in revised form 10 December 2002; accepted 16 December 2002

Abstract
The large amount of disposable bottles presently produced makes imperative the search for alternative procedures for recycling
or reuse of these materials, since they are not biodegradable. As chemical processing is most often costly and sometimes aggressive
to the environment, a possible solution is the recycling of such material by thermo-mechanical techniques. This paper takes into
consideration the thermo-mechanical recycling of post-consumed plastic bottles, especially the ones made of polyethylene ter-
ephtalate (PET), and its use as composite materials for engineering applications. To be able to evaluate the new composite perfor-
mance from the mechanics point of view, i.e. stiffness and machinability, two sets of tests were carried out. For the first set,
compression tests were applied. For the machinability evaluation, the final roughness was measured after the milling procedure at
different speeds and leads. Experimental data showed good performance for compression and machinability. Finally, spur gears
were cut from cylindrical specimens made of PET/HDPE blend.
# 2003 Elsevier Science Ltd. All rights reserved.
Keywords: Polymeric blends; Recycling; Machinability; PET/HDPE blend

1. Introduction emergent country with a population of three million

Polymeric matrix composites (PMC) are used in
engineering applications as they present low density and
high strength. However, they are not used in large-scale
applications due to their high cost. The large variety of
thermoplastic matrices, which allows us to experiment
with different types of resin combinations creating the
so-called melt-blended matrices, can be seen as an
alternative. These melt-blended matrices can help
reduce cost and, at the same time, increase specific
properties such as strength. One low cost source of such
type of resins is recycled thermoplastics. Post-consumed
polyethylene terephthalate (PET), for instance, has a
cost of 10 cents/kg while polystyrene (PS), high and low
density polyethylene (HDPE, LDPE), and poly-
propylene (PP) have an even lower cost, three to six
cents/kg. Their low cost is due to the large amount of
post-consumed plastic waste generated daily in large
cities worldwide. To give an example, a city in an
* Corresponding author.
E-mail addresses: aavila@dedalus.lcc.ufmg.br (A. F. Ávila),
marcos.duarte@petrobras.com.br (M. V. Duarte).
0141-3910/03/$ - see front matter # 2003 Elsevier Science Ltd. All rights reserved.
doi:10.1016/S0141-3910(03)00025-9
inhabitants produces each day around 400 t of plastic
waste [1]. As a consequence, municipalities are becom-
ing concerned about a 25% increase in plastic waste
generation per year while the landfill area is only
increasing at a 7.5% annual rate. Therefore, as Scott [2]
points out, by the year 2015 there will be no disposal
options for plastic waste.
In 1997, Jones and Baumann [3] reinforced the
importance of implementing a politics of recycling.
Nevertheless, there are many other limitations for recy-
cled materials. For instance, although there are govern-
mental regulations in countries such as Germany,
recycled materials are not used based only on their
physical properties but mainly because of their surface
appearance. In other words, many designers are afraid
of using them as they can be rejected by the market. But
this is an attitude that can change. Recently, Martins
and De Paoli [4] stated that around 15% of all rigid
plastics and films consumed in Brazil are recycled and
returned to industry. Moreover, according to Selke [5],
the total amount of plastics in the US municipal solid
waste stream is around 10%; from this amount 44% is
from containers and packaging. A large quantity of
374 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382
these containers come from soft drink bottles. The fact
that some states in the US are concerned with recycling,
(e.g. Michigan, where the recycling rate is close to
100%) proves the potential for recycling plastic waste as
well as changes in the market attitude.
One possible solution for the municipality plastic
waste problem is the recycling procedure. According to
Scott [2], plastic waste management can be done by
three different approaches. The first one is the mechan-
ical recycling approach, which is a technique similar to
procedures used to recover materials suitable for second
use. The second one is known as energy recovery, which
can be performed in two distinct ways. The first way is
incineration where the hydrocarbon polymers replace
fossil fuels. The second way can be done by pyrolysis or
by hydrogenation to low molecular weight hydro-
carbons for use either as portable fuels or as polymer
feedstock. A third approach is defined by Scott [2] as the
biological recycling. This approach takes advantage of
the polymer biodegradation, which is highly dependent
on the polymer type and environmental conditions.
However, this type of recycling most often involves not
only high costs and complex procedures but also
potential damages to the environment. Due to all these
problems, a feasible solution for the increase of plastic
waste generation is the thermo-mechanical recycling.
This technique first involves mechanical recycling where
the thermoplastics are granulated followed later by
techniques as extrusion or thermoforming.
Furthermore, as noted by Brandrup et al. [6], to be
economical a mechanical recycling procedure must be
designed in such manner that the amount of energy
needed to produce the virgin material plus the energy to
dispose of the material must be equal to the energy to
recover the post-consumer materials plus the energy
during the reprocessing itself. This balance, however,
does not take into consideration the environmental
benefits. When those environmental gains are con-
sidered, a higher energy consumption could be allowed
during the mechanical recycling. This increase in cost
could be compensated by indirect cost reductions in
landfills, for example. Unfortunately, the large majority
of the population does not consider the indirect cost
reduction as a social benefit.
Besides, all three approaches have a limitation in
common: the potentially misleading idea that during the
recycling process there is a continuous degeneration on
the materials mechanical properties. According to Paw-
lak et al. [7], the unsatisfactory mechanical properties of
recycled polymer are due to degradation during the
reprocessing. However, as recognized by Ávila [8], for
PET there is an increase on stiffness during the second
and third recycling process. This phenomenon can be
explained by different factors. One of these factors is the
increase of crystalline structures as mentioned by Gay-
mans [9]. With the increase in crystallinity, Gaymans [9]
also observed higher values of elasticity modulus and
yield strength. This phenomenon is particularly effective
above the glass-temperature. Moreover, according to La
Mantia and Gardette [10], the increase in crystallinity is
the result of a molecular weight reduction which is also
related to a drastic reduction of elongation to break.
The work from Van der Wal et al. [11] goes further; they
conclude that for the PP–rubber blends, there is also a
decrease on fracture strain due to the decrease on brit-
tle–ductile transition. Davis [12], however, stated that
these changes can be due to changes in microstructures.
2. Various ways to follow: an overview
The main idea is to obtain post-consumed materials
with enhanced mechanical properties and at same time
to give them new uses. Another key point is that for
structural mechanics stiffness is crucial, as the actual
stress field during loading and unloading is far from
yielding or breaking. There are several possible tracks
that can be pursued. One is based on the development
of new materials from post-consumed polymers. Con-
sidering this approach, the following statement must be
kept in mind: ‘‘the development of new multiphase
blend materials is dependent primarily on two key
requirements: control the interfacial chemistry and con-
trol of the microstructures’’ [12]. According to Utracki
[13], there are several materials parameters that could
influence morphology/viscosity ratio,1 composition,
elasticity, shear stress, and interfacial modification.
Davis [12] proved that lower viscosity ratio results in
fine dispensed-particle size. However, when the compo-
sition is considered, it is possible to conclude that the
final morphology obtained is a balance between defor-
mation and disintegration phenomena, on one hand,
and coalescence, on the other. As the fraction of the
dispersed phase increases, there is also an increase in the
particle size due to coalescence. Moreover, based on
Taylor’s law for Newtonian liquids, it is possible to
conclude that the phase size is inversely proportional to
the applied stress. An example of this behavior was
shown by Min et al. [14] for PE/PS blends. Davis [12],
however, noticed that large variations in the shear stress
are required for it to predominate over the viscosity
ratio in controlling dispersed-particle size. Moreover,
the particle size is largely determined by interfacial ten-
sion, the viscosity and elasticity ratios. An increase of
shear stress can be obtained as a result on shape changes
on the dispersed phases. This phenomenon was
observed by Gonzalez-Nunez et al. [15] for a Poly-
amide-6/HDPE blend. Another possible option is the
use of block copolymers. It is possible to obtain in an
immiscible blend smaller particle-size and narrow parti-
1
Viscosity of the dispersed phase/viscosity of the matrix.
 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382
cle-size distribution as a result of interfacial modifi-
cations caused by the use of copolymers. Finally, modi-
fications on morphology, and, consequently, on
mechanical properties can be obtained by a new process
named dynamic quenching proposed by Cassagnau and
Michel [16]. It consists on crystallizing under shear or
elongation flows a semi-crystalline polymer dispersed in
melt thermoplastic matrix. All of these methods result in
a completely new material not only from the micro-
scopic point of view but also in it phase composition.
Another approach is the so-called micro–macro
mechanics which leads basically to an enhanced mate-
rial where the major changes are at the microstructure
level. Thermo-mechanical loadings are applied, and its
effects are changes on the material microstructures and
on its macro-mechanical behavior. The work done by
Pawlak et al. [7], Ávila [17] and Mancini et. al [18] focus
on this idea. The work of Salem [19], relating the influ-
ence of strain rate on PET crystallization, is of special
interest. He concludes that there is a direct proportion-
ality between the strain rates and the amount of PET
crystalline phase. Cheremisinof and Cheremisinof [20],
in the other hand, affirms that the increase in crystalline
phase is often related to higher elastic modulus. There-
fore, the linkage between the microstructure changes
and the polymer macro-mechanical behavior has been
established. Nevertheless, during the processing of those
polymers the oxidation must be taken into considera-
tion. According to Scott [21], oxidation degradation
occurs during the thermoplastics processing, and as
consequence there is a reduction in mechanical proper-
ties. In addition, the introduction of oxidative products
can be harmful to long term durability. He suggests the
use of antioxidants and stabilizers to reduce the
mechanodegradation of polymers.
The final approach concentrates on the chemical
changes induced by the addition of fibers and fillers as
well as compatibilizers and additives. Guo and Mer-
rington [22], for example, studied the effects of compa-
tibilisers and additives on polymer blends. Their
attention focused on multi-component blends, i.e. PE,
PS, PP, polymethyl methacrylate (PMMA) and poly-
vinyl chloride (PVC), as a way of increasing the number
of thermoplastics recycled. They noticed a slight
increase in tensile strength with the compatibilizer use
[22]. Moreover, the elongation break and fracture
energy were greatly enhanced, around 50% more, with
the use of a co-polymer. Ha et al. [23] studied multi-
component blends, but they restricted their study to
ternary blends where the compatibilizer, a co-polymer,
was also present. The compatibilizer effectiveness was
studied by analyzing the blends’ morphology, the crys-
talline structure and the tensile properties. By doing it,
they were able to quantify the co-polymer efficiency. In
research by Park et al [24], various compatibilizers were
tested in a HDPE/PET blend. They concluded that the
375
HDPE/PET blend morphology is highly dependent on
interfacial bonding as it affects its stiffness and strength.
However, no attention was given to the cost/benefit
relation. By considering all work done so far, it seems
that there is no absolute agreement on which approach
is the best.
3. Experiments
Before describing the experimental procedure devel-
oped in this paper, some comments must be made. First,
the recycling process used in this paper is essentially
thermo-mechanical, and the polymers used are immis-
cible. Second, the entire analysis performed here takes
into consideration the macro-mechanical approach as
defined by Tamma and Avila [25]. This analysis is
mainly concerned with the polymer macroscopic
mechanical properties. On top of this, we are examin-
ing the effects of recycling process on the materials
properties as discussed in Ávila [8]. The objective here
is to develop a fully recycled polymeric matrix compo-
site, where no addition of any kind of stabilizer, com-
patibility or additive is applied, to be used into
engineering applications. The reader must have in mind
that the mechanical properties will be lower than the
ones with virgin materials, but the cost/effectiveness
relation is better. This new composite will have specific
applications where no high loadings/unloadings are
required.
3.1. Materials
The materials were selected after taking into con-
sideration not only their quantity in the urban plastic
waste but also their potential use on civil and mechan-
ical engineering. According to CEMPRE [26], the total
amount of plastic waste on urban solid waste in Brazi-
lian cities is around 18%. From that amount, the fol-
lowing percentages were obtained: HDPE and LDPE
36%, PET 20%, PVC 13%, PP 11%, and 20% others.
Besides the post-consumed PET in Brazil has a singular
characteristic: around 2/3 of all PET used in the manu-
facturing of soft drink bottles is green. This choice has a
cultural explanation. After using green glass bottles for
years in Brazil, when soft drink companies introduced
PET bottles, they decided to keep the green color to
avoid problems with customers. Therefore, the research
focused on green PET bottles. As most of the time bot-
tles and caps are discarded together, it was decided to
create a particulate composite material made of a PET
matrix (bottles) and HDPE whiskers (caps).
The PET and HDPE volume fractions, in weight,
considered here follow the ratio 80/20, 70/30, 60/40, and
50/50, respectively. The 50/50 ratio was discarded due
to problems of adhesion between PET and HDPE.
376 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382
3.2. Processing and recycling
Pawlak et al. [7] point out that to be able to obtain the
mechanical characterization of polymeric scraps, it is
necessary to homogenize the material. Nevertheless, as
the materials used are from post-consumed bottles, a
pre-treatment must be done before the homogenization
procedure.
The pre-treatment consists of three different steps,
namely: washing, granulation and drying. The granu-
lated material average length and thickness are 8 and 2
mm, respectively. The drying program was developed
considering the grains dimensions and their thermal-
mechanical properties. Moreover, the HDPE is assumed
as spherical or ellipsoidal inclusions on the PET matrix.
By taking into account this geometric arrangement, it is
possible to estimate the composite’s thermal properties,
i.e. thermal conductivity and thermal expansion coeffi-
cient. After determining the material properties, it is
feasible to define the drying procedure. It consists in a
gradual increase on temperature, which goes from room
temperature to 100  C at a rate of 5  C/min. When the
steady state has been reached, the temperature is kept
constant for a 24-h period. This procedure guarantees
levels of humidity inferior to one percent per volume, as
mentioned by Faria and Ávila [27].
The homogenization procedure is usually done by
extrusion. For this specific case, the extrusion opera-
tional parameters are listed on Fig. 1. The next step is
hot compression. This technique allows the manu-
facturing of complex pieces at low cost when compared
against injection molding or more sophisticated meth-
ods, for example, resin transfer molding. During hot
compression, a uniform pressure of 42 MPa at
200 4  C is applied for a period of 2.5 h. The values
are obtained by the heat transfer equations given by
Mantell and Springer [28] and preliminary tests.
3.3. Compression and machinability tests
To be able to evaluate the new composite perfor-
mance, two specific tests were carried out. The first one
was the compression test, where the composite strength
and failure mechanism were studied, and the last one
Fig. 1. Extruder’s parameters.
was the machinability test. The final goal was to evalu-
ate the composite’s surface roughness and its stiffness
and strength. For both tests, cylindrical specimens with
a 30 mm diameter and 35 mm height were manu-
factured by hot compression. For each PET/HDPE
group of blends, a set of four specimens were prepared.
The machinability test was performed by considering
not only the chip shape but also the average surface
roughness as a function of machine parameters, i.e. cut-
ting speed, radial cutting penetration, and lead. More-
over, during the compression test, the following variables
were evaluated: Young’s modulus (E), ultimate stress
(
u), and total strain (") at room temperature.
4. Analysis from experimental data
4.1. Compression tests
An INSTRON 4482 testing machine was used to per-
form the compression tests at room temperature and
with a constant speed of 1.0 mm/min. Fig. 2 shows the
PET/HDPE blend performance during the compression
tests for the 80/20 ratio, while the stiffness and strength
results are listed on Table 1.
The same methodology was applied to the 70/30 and
60/40 PET/HDPE ratio and the results are shown in
Figs. 3 and 4, and Tables 2 through 3, respectively. By
analyzing all data collected by the compression tests, it
is possible to conclude that there is more than one
mechanism involved on the recycled blends behavior.
As expected, the stiffness increases due to the larger
amount of PET, which is stiffer than HDPE; however
the ultimate stress is reduced even having a higher per-
centage of PET in weight.
Several hypothesis can be formulated to explain such
a behavior. According to Cheremisinof and Cher-
emisinof [20] PET is known by its susceptibility to
hydrolytic degradation. They also stated that the pre-
sence of moisture affects the crystallization process
through enhanced nucleation. However, the enhance-
ment on nucleation could not be explained on basis of a
decreasing in the glass-transition temperature. They also
suggested that changes in the crystallization behavior
 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382 377

Fig. 2. PET/HDPE stress–strain curve for 80/20 ratio.

could also be attributed to molecular-weight degrada-
tion of PET in the presence of moisture. Jabarin [29],
however, claims that the nucleation rate increased sig-
nificantly with the moisture, although the spherulitic
growth rate seems to be independent of the moisture
contents. The work done by Jabarin [29] and Cher-
emisinof and Cheremisinof [20] jump to the same con-
clusion, besides moisture there is another reason for
changes in the PET. Parisi and Neubauer [30] pointed
out the importance of moisture contents during the
extrusion of recyclates. They also mentioned the mole-
cular-weight degradation in presence of moisture during
the extrusion. So far, a possible explanation for the
behavior shown in Figs. 3 and 4 can be formulated
based on two associated mechanisms: the first one is the
presence of moisture that increases the nucleation rate,
but with no effect on spherulitic structures (Fig. 5). The
second mechanism is the PET molecular-weight degra-
dation in the presence of moisture. It seems that the
second one is dominant.
Another important point must be analyzed, i.e. the
specimen’s fracture. By observing Fig. 6, it is possible to
conclude that these fractures occurred in the maximum
shear stress region as expected. But the most important
point is that all specimen’s fracture seems to be brittle.
In parallel with the conclusions of van der Wal et al. [11]
for the PP–rubber blend, it is possible to suppose that a
decrease in the brittle–ductile transition region could be

Fig. 3. PET/HDPE stress–strain curve for 70/30 ratio.

378 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382

Fig. 4. PET/HDPE stress–strain curve for 60/40 ratio.

Table 1 taken in effect. Therefore, from the mechanical point of

PET/HDPE 80/20 mechanical properties view, the machinability test must be performed to
Specimen ID E [GPa]
u [MPa] "[mm/mm] obtain a complete analysis.

1 1.432 23.274 0.029 4.2. Machinability tests

2 1.454 21.861 0.029
3 1.495 24.869 0.040
4 1.461 21.110 0.031 The machinability test was performed considering a
fixed cutting tool with the following geometric para-
Average value 1.460 22.780 0.032 meters: main location angle equals to 87 , lateral loca-
tion angle of 19 and a positive relief angle. As the tool
geometry is fixed, it is possible to vary the machine
operational parameters. The most important variables
Table 2
PET/HDPE 70/30 mechanical properties

Specimen ID E [GPa]
u [MPa] "[mm/mm]

1 1.269 26.471 0.047

2 1.284 27.639 0.047
3 1.261 28.175 0.045
4 1.307 29.305 0.043

Average value 1.280 27.900 0.046

Table 3
PET/HDPE 60/40 mechanical properties

Specimen ID E [GPa]
u [MPa] "[mm/mm]

1 1.104 27.188 0.059

2 1.159 28.579 0.060
3 1.109 27.972 0.055
4 1.177 27.531 0.049

Average value 1.139 27.812 0.056

Fig. 5. The blend microstructure.
 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382 379

Fig. 6. Fracture aspect for the PET/HDPE 60/40 ratio.

Table 4
Machinability test conditions

First set condition Second set condition

Speed [m/s] 1.11 1.74 2.05 1.11 1.74 2.05

Radial cutting deepness [mm] 0.5 0.5 0.5 1.5 1.5 1.5
Lead [mm/rotation] 0.0079 0.0079 0.0079 0.207 0.207 0.207

Fig. 7. Roughness data from the first set condition.

380 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382
Fig. 8. A—Chip shape for the 60/40 ratio. B—Chip shape for 70/30
ratio.
on milling procedure are radial cutting deepness, lead
and speed. By keeping two of the machine parameters
constant and varying the third one, it is possible to
analyze how they influence the average surface rough-
ness. The analysis was performed applying two distinct
set conditions: a moderate and a severe milling condi-
tion, as shown in Table 4.
The first set average result data for the blend with
80/20 ratio show that as the speed increases, the
roughness increases, as expected, see Fig. 7. This trend
does not hold for the other blend ratios studied. The
blend with 60/40 ratio has a nearly constant roughness
as the speed increases, and the chip shape is close to a
continuous strip, as shown on Fig. 8A. As the amount
of PET and speed increases, the average roughness
value also increases and the chip shape is close to dis-
continuous flakes, see Fig. 8B. As mentioned by Lind-
berg [31], the discontinuous flakes affect the milling
procedure as it increases the tool wear. Therefore, a
continuous chip shape, which leads to smaller values of
roughness, proves to be more favorable to milling
operations.
The average roughness value for severe milling con-
dition are shown on Fig. 9. A peak in roughness can be
observed for a speed around 1.75 m/s for the 60/40 and
70/30 ratios while a substantial decrease for the 80/20
blend is noticed. After this variation, the values seem to
stabilize close to the ones from the lower speed. It seems
that the severe cutting deepness and the large values of
lead provokes a disjointing between the PET and HDPE
phases, as it can be observed by the chip shape on
Fig. 10.
The last step was the spur gear manufacturing. To be
able to achieve such goal the following geometric para-
meters were used: modulus equals to 2 mm/tooth, pitch
diameter of 34 mm, 17 teeth, pressure angle of 20 ,
working depth of 4.5 mm, and face width of 18 mm.
Fig. 11 shows the spur gear made of the 60/40 blend.
5. Closing remarks
Recycled polymeric matrix composites seems to have
potential for use not only in engineering applications
but also in our daily life. As shown before, their ulti-
mate strength ranging from 22 to 28 MPa is a clear evi-
dence of their capability. At the same time, the lower
values of roughness obtained are an encouraging data
from the manufacturing point of view.
In this sense, it is important to emphasize that, the
addition of HDPE particulates into a PET solution
reduces the effective stiffness of the blend. However, the
HDPE phase gives a major contribution to milling
operations, as it decreases the surface roughness by
allowing a higher cohesive condition between PET and
HDPE, as long as all operational conditions are kept
fixed.
A more comprehensive study is under development
where long term degradation tests are being conducted.
However, when the possible uses of this new composite
is considered, for example, gears for small mechanisms,
laminates for houses flooring, as a substitute for tiles
and small house/school appliances, the cost/benefit
relation seems very attractive specially when compared
against wood.
Finally, the environmental gains, for example, life
expansion of the existing landfills and the reduction in
the harvesting of trees, with the use of this new compo-
site seems to be one of the most important contribution
of the present research.
 A.F. Ávila, M.V. Duarte / Polymer Degradation and Stability 80 (2003) 373–382
Fig. 9. Roughness data from the second set condition.
Fig. 10. Chip shape from the second set condition.
Acknowledgements
The authors would like to acknowledge the financial
support provided by the Brazilian Research Council
(CNPq) and the Minas Gerais State Research Founda-
tion (FAPEMIG).
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