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materials

Article
The Effect of the Melt Viscosity
and Impregnation of a Film on the Mechanical
Properties of Thermoplastic Composites
Jong Won Kim and Joon Seok Lee *
Department of Textile Engineering and Technology, Yeungnam University, Gyeongsan 712-749, Korea;
kjwfiber@ynu.ac.kr
* Correspondence: leejs@ynu.ac.kr; Tel.: +82-53-810-2774

Academic Editor: Reza Montazami


Received: 6 April 2016; Accepted: 1 June 2016; Published: 3 June 2016
Abstract: Generally, to produce film-type thermoplastic composites with good mechanical properties,
high-performance reinforcement films are used. In this case, films used as a matrix are difficult to
impregnate into tow due to their high melt viscosity and high molecular weight. To solve the problem,
in this paper, three polypropylene (PP) films with different melt viscosities were used separately
to produce film-type thermoplastic composites. A film with a low melt viscosity was stacked so
that tow was impregnated first and a film with a higher melt viscosity was then stacked to produce
the composite. Four different composites were produced by regulating the pressure rising time.
The thickness, density, fiber volume fraction (V f ), and void content (V c ) were analyzed to identify
the physical properties and compare them in terms of film stacking types. The thermal properties
were identified by using differential scanning calorimetry (DSC) and dynamical mechanical thermal
analysis (DMTA). The tensile property, flexural property, interlaminar shear strength (ILSS), and
scanning electron microscopy (SEM) were performed to identify the mechanical properties. For the
films with low molecular weight, impregnation could be completed fast but showed low strength.
Additionally, the films with high molecular weight completed impregnation slowly but showed high
strength. Therefore, appropriate films should be used considering the forming process time and their
mechanical properties to produce film-type composites.

Keywords: thermoplastic composite; impregnation; melt viscosity; pressure rising time;


mechanical properties

1. Introduction
The application of carbon fiber reinforced plastic (CFRP) composites has been increasing with
improved mechanical properties resulting from improved fibers and matrix materials, allowing
them to displace conventional materials, such as steel, aluminum, and titanium alloys, for primary
structures [1–3]. Fiber-reinforced thermoplastic (FRTP) composites have been applied widely to
many industries owing to their advantages, such as fracture toughness, damage tolerance, ease
of shape-forming before consolidation, significantly faster manufacturing, longer shelf life of raw
materials, and the ability to be reshaped and reused [4]. On the other hand, the largest problem of
thermoplastic composites is that the resin can barely penetrate the fiber bundles because of its high
viscosity (500–5000 Pa¨ s) at melting temperatures when compared with that of thermosetting resins
(commonly < 100 Pa¨ s) [5]. Many manufacturing processes for thermoplastic composites have been
developed to solve the problem, and the use of a prepreg is the most common way to manufacture
them [6–9].
A prepreg is where the reinforcing fibers or fabrics are pre-impregnated with resin. Thermoplastic
prepregs undergo additional forming processes where needed; more than two prepregs are laminated

Materials 2016, 9, 448; doi:10.3390/ma9060448 www.mdpi.com/journal/materials


Materials 2016, 9, 448 2 of 15

and go through compression molding to produce the composite [10–13]. The property of prepregs
could have a significant effect on the properties of the composite. The methods to produce a
prepreg include film prepregging [14], hot melt prepregging [15,16], solution dip prepregging [17],
powder prepregging [18,19], commingled prepregging [20], co-weaving prepregging [21], and in-situ
polymerization [22,23].
For film prepregging, the pressure-temperature history of the polymer have the greatest effect on
the impregnation (void content). For melting impregnation, however, this is impractical for certain
polymers because of their limited tolerance to the temperatures necessary for viscosity reduction.
Thermal degradation determined by a molecular weight reduction could be initiated within a few
degrees of the melt temperature, making the viscosity reduction difficult or impractical [24]. In
addition, there are mechanical limitations when using high pressures to impregnate a fiber. Generally,
the mechanical properties of a composite deteriorate when a resin with low melt viscosity is used to
improve impregnation owing to its low molecular weight. If a resin with a high degree of crystallization
and a high molecular weight is used to improve the mechanical properties of a composite, impregnation
decreases and reinforcement goes out of alignment owing to its high melt viscosity. In the case of using
fabric-type reinforcement, the condition becomes worse.
Common film-type prepregs are manufactured continuously through a roller or belt, and a
considerable amount of research has been processed to reduce manufacturing time without any
decrease in properties so as to lower the price. Melting the film without thermal degradation and
impregnation of the reinforcing structure should be considered throughout the film-type prepreg
manufacturing process. For films, the onset of melting, the rheological behavior at melt processing
temperatures, and the time to drive impregnation should be considered [25–27].
In this paper, three polypropylene (PP) films with different melt viscosities were used separately
to produce a composite. For the resin having low flowability with high melt viscosity, to reduce the
time of driving impregnation and to improve the impregnation of the fiber, a film with a low melt
viscosity was stacked so that tow was impregnated first; afterward, a film with a higher melt viscosity
was stacked to produce the composite. The mechanical properties were then examined.

2. Materials and Methods

2.1. Materials
Woven fabric (SNC-1242R, plain, density (count/25 mm) = 6.4, weight = 420 g/m2 , Seanal Tech-tex
Co., Gumi, Korea) using carbon fiber (Toray T-300, 12K, Tokyo, Japan) was used as the reinforcing
material. As the matrix, three PP films (SFI-151, SFI-740P, SFI-130A, Lotte Chemical Co., Seoul, Korea)
with different melting flow indices (MFI) were used. Table 1 shows characterizations of the films.

Table 1. Characterizations of films from the manufacturer’s datasheets.

Properties SFI-151 SFI-740P SFI-130A


Melting flow index (g/10 min) 8 5.5 3
Molecular weight (g/mol) 250,000 270,000 300,000
Melting point (˝ C) 166.1 162.6 160.3
Density (g/cm3 ) 0.90 0.90 0.90
Tensile stress at yield (MPa) 21 26 32
Tensile strain at break (%) >500 >500 >500
Flexural modulus (MPa) 670 980 1470
Thickness (µm) 50 50 50

2.2. Preparation of the Carbon Fiber-Reinforced Thermoplastic Composites


The three PP films were stacked both above and under the carbon fiber fabric to produce the
composite in the 4 stacking types, as shown in Figure 1. Only one type of film was used in the low melt
Materials 2016, 9, 448 3 of 15

Materials 2016, 9, 448 3 of 15


viscosity type (LV-type), middle melt viscosity type (MV-type), and high melt viscosity type (HV-type);
(HV-type);
all three allfilms
types of threewere
typesstacked
of films for
were stacked
fiber for fiber impregnation
impregnation in the order in of the
theorder of the meltin the
melt viscosity
combination film type (CV-type). Those carbon fiber fabrics were laminated in 8 layersinand
viscosity in the combination film type (CV-type). Those carbon fiber fabrics were laminated 8 layers
inserted
and inserted into a mold2 (295 × 295 mm2) for compression molding to produce the composite. After
into a mold (295 ˆ 295 mm ) for compression molding to produce the composite. After the mold was
the mold was pre-heated in a hot press at 230 °C for 5 min, the pressure rising time was regulated by
pre-heated in a hot press at 230 ˝ C for 5 min, the pressure rising time was regulated by varying the
varying the time to reach 25 MPa from 5 to 25 min. When the time was shorter than 5 min, the
time to reach 25 MPa from 5 to 25 min. When the time was shorter than 5 min, the reinforcement went
reinforcement went out of alignment as a high pressure was suddenly applied so that the fiber could
out ofnotalignment
impregnateasthe
a high pressure
fabric, and voidswas suddenly
could applied
barely exit so that the
the inter-layer duefiber could not
to squeezing. impregnate
The mold was the
fabric,then
andcooled
voidstocould
roombarely exit the
temperature. inter-layer
The duethen
pressure was to squeezing.
removed and The
themold was then
composites werecooled to room
detached
temperature. The pressure was then removed and the composites were detached from the mold.
from the mold.

FigureFigure 1. Schematic
1. Schematic diagram
diagram of of hotpress
hot pressprocessing:
processing: (a)
(a)low
lowviscosity
viscosityfilm type;
film (b) (b)
type; middle
middleviscosity
viscosity
film type;
film type; (c) high
(c) high viscosity
viscosity filmfilm type
type and(d)
and (d)combination
combination (low-middle-high
(low-middle-high viscosity) filmfilm
viscosity) type.type.

2.3. Measurement
2.3. Measurement
The specimen thickness (mm) was averaged by measuring 4 edges and the center of each
The specimen
specimen usingthickness
a thickness(mm) was
gauge. Theaveraged by measuring
fiber volume fraction (Vf)4ofedges and the was
the specimen center of eachusing
calculated specimen
usingaaburn-off
thickness gauge. The fiber volume fraction
test according to ASTM D 2584. The specimen (V f ) of the specimen was calculated using a
was inserted into a furnace in an inert burn-off
test according to ASTM
environment for 10 hDat2584. The
500 °C specimen
and dried in was insertedThe
a desiccator. intoVaf was
furnace
then in an inertbased
calculated environment
on the for
10 h at 500 ˝ C and
specimen weight ratio
dried inbefore and after
a desiccator. theVburn-off
The f was test.
then The actual
calculated density
based was
on thecalculated
specimen using the ratio
weight
Archimedes principle according to ASTM D 792 by measuring the differences between
before and after the burn-off test. The actual density was calculated using the Archimedes principle the weight of
a specimen in air and in water. The void volume content (V c) was calculated using Equation (1) based
according to ASTM D 792 by measuring the differences between the weight of a specimen in air and in
on the ASTM D 2734 as follows:
water. The void volume content (V c ) was calculated using Equation (1) based on the ASTM D 2734
as follows: %m %m
100 ρ , (1)
ρ ρ
ˆ ˙
where Vc is the void volume %mprimary
matrix %mfiber and %m is the mass of each
Vc “content
100 ´ ρ(%), ρ is the
sample ` density, , (1)
constituent. ρmatrix ρfiber
where V cTheis differential scanningcontent
the void volume calorimetry
(%),(DSC,
ρ is Q-200, TA Instruments,
the primary density, Newcastle,
and %m is DW,
theUSA)
mass of
patterns of
each constituent.specimens were monitored between 30 and 200 °C at a heating rate of 10 °C/min in a
nitrogen atmosphere. The melting enthalpy was measured, and the degree of crystallinity (Xc) was
The differential scanning calorimetry (DSC, Q-200, TA Instruments, Newcastle, DW, USA) patterns
calculated using the following equation:
of specimens were monitored between 30 and 200 ˝ C at a heating rate of 10 ˝ C/min in a nitrogen
∆H 100
atmosphere. The melting enthalpy was measured, and the degree of crystallinity (Xc ) was calculated (2)
∆H ° w
using the following equation:
where ΔHm is the melting enthalpy calculated from the curve of melting endotherm of the sample,
ΔH°m (=209 J/g) is the enthalpy of the fusion of∆H
100% 100
m crystalline PP, and w is the weight fraction of
Xc “ ˝ ˆ (2)
PP in the composite [28,29]. ∆H m w
Dynamic mechanical thermal analysis (DMTA, Q-800, TA Instruments, Newcastle, DE, USA)
where ∆Hm is the melting enthalpy calculated from the curve of melting endotherm of the sample,
was used to measure the viscoelastic properties of specimens. The single cantilever method was used
∆H m (=209 J/g) is the enthalpy of the fusion of 100% crystalline PP, and w is the weight fraction of
˝

PP in the composite [28,29].


Materials 2016, 9, 448 4 of 15

Dynamic mechanical thermal analysis (DMTA, Q-800, TA Instruments, Newcastle, DE, USA) was
used to measure the viscoelastic properties of specimens. The single cantilever method was used for
the specimens. The measurements were performed at a frequency of 1 Hz and amplitude of 1.5 µm.
The temperature range was from 30 to 170 ˝ C. The storage modulus (E’) and loss factor (tan δ) of
the specimens were measured as a function of temperature. The tensile strength, flexural strength,
Materials 2016, 9,shear
and interlaminar 448 strength (ILSS) were measured using a tensile tester (OTT-05, Oriental 4 of 15 Co.,
Seoul, Korea) to determine the mechanical properties of the specimens. The tensile
for the specimens. The measurements were performed at a frequency of 1 Hz and amplitude of 1.5
test was carried
out according
µm. The to ASTM Drange
temperature 3039 was
at afrom
crosshead
30 to 170speed ofstorage
°C. The 2 mm/min.
modulus A(E’)
three-point-bending
and loss factor (tan δ)test was
carried of
out
thebased
specimens on the
wereASTM D 790
measured as ato measure
function the flexural
of temperature. Thestrength with a flexural
tensile strength, span-to-depth
strength, ratio of
and interlaminar
16 at a crosshead speedshear strength
of 1.3 (ILSS)The
mm/min. were measured
ILSS using
was also a tensile tester
measured using(OTT-05, Oriental Co.,
a three-point-bending test
Seoul, Korea) to determine the mechanical properties of the specimens. The
based on the ASTM D 2344 with a span-to-depth ratio of 4 at a crosshead speed of 1 mm/min. The tensile test was carried
out according to ASTM D 3039 at a crosshead speed of 2 mm/min. A three-point-bending test was
impregnation inside the tow was identified by scanning electron microscopy (SEM, S-4100, Hitachi,
carried out based on the ASTM D 790 to measure the flexural strength with a span-to-depth ratio of
Tokyo, Japan).
16 at a crosshead speed of 1.3 mm/min. The ILSS was also measured using a three-point-bending test
based on the ASTM D 2344 with a span-to-depth ratio of 4 at a crosshead speed of 1 mm/min. The
3. Results and Discussion
impregnation inside the tow was identified by scanning electron microscopy (SEM, S-4100, Hitachi,
Tokyo, Japan).
3.1. Thickness and Fiber Volume Fraction
3. Results and Discussion
Figure 2 shows the thickness and fiber volume fraction of the composite compared with the
pressure rising
3.1. timeand
Thickness inFiber
eachVolume
film stacking
Fraction type. In Figure 2a, the thickness of the composite decreased
as pressure rising time increased. For the LV-type, thickness started to decrease slightly as the pressure
Figure 2 shows the thickness and fiber volume fraction of the composite compared with the
rising time increased.
pressure This
rising time happened
in each because
film stacking type.tow impregnation
In Figure and reinforcement
2a, the thickness of the composite of the composite
decreased
were almost complete during the pre-heating process such that no resin
as pressure rising time increased. For the LV-type, thickness started to decrease slightly ascame out. For thethe
HV-type,
the thickness
pressure ofrising
the composite
time increased.is believed to continuously
This happened because towdecrease
impregnationbecause the unimpregnated
and reinforcement of the fiber
from thecomposite
pre-heating were almost
process complete
continuedduring
tothe pre-heating
undergo process suchduring
impregnation that no resin came out. rising
the pressure For the process
HV-type, the thickness of the composite is believed to continuously decrease because the
owing to its high melt viscosity. At a time of 25 min, the thickness of the HV-type was much higher
unimpregnated fiber from the pre-heating process continued to undergo impregnation during the
than thepressure
LV-type, which is believed to happen since impregnation was not complete for the HV-type.
rising process owing to its high melt viscosity. At a time of 25 min, the thickness of the HV-
The CV-type
type was much highershowed
and MV-type than the aLV-type,
similarwhich
tendency. On the
is believed to other
happenhand,
since by comparing
impregnation thenot
was thickness
with thecomplete
pressure forrising time, at
the HV-type. Thea CV-type
shorter and
timeMV-type
of 5 min, the impregnation
showed of tow
a similar tendency. was
On the easier
other hand,for a low
by comparing
melt viscosity film inthethe
thickness
CV-type withthan
the pressure rising time,
the middle meltatviscosity
a shorter time
filmofin5 the
min,MV-type,
the impregnation
such that the
of tow
composite was was easier for
slightly a low melt
thinner. At viscosity
a longerfilmtime in of
the25CV-type than the middle by
min, impregnation meltthe
viscosity film in
high melt viscosity
the MV-type, such that the composite was slightly thinner. At a longer time of 25 min, impregnation
film in the outer layer of the tow was much more difficult in the CV-type than that by the middle melt
by the high melt viscosity film in the outer layer of the tow was much more difficult in the CV-type
viscosity film
than in by
that thethe
MV-type because
middle melt fiberfilm
viscosity impregnation
in the MV-type wasbecause
almostfiber
complete, such that
impregnation was the composite
almost
was slightly thicker.
complete, such that the composite was slightly thicker.

Figure 2. Cont.
Materials 2016, 9, 448 5 of 15
Materials 2016, 9, 448 5 of 15

Figure Figure 2. Thickness (a) and fiber volume fraction (b) of the composite compared with the pressure
2. Thickness (a) and fiber volume fraction (b) of the composite compared with the pressure
rising time in each film stacking type.
rising time in each film stacking type.
In Figure 2b, the fiber volume fraction increased as pressure rising time increased. This
In happened
Figure 2b,because the volume
the fiber resin, which is theincreased
fraction matrix, wasassqueezed
pressureout fromtime
rising the composite
increased. due to the
This happened
high pressure, since the fiber volume fraction is the only value that represents
because the resin, which is the matrix, was squeezed out from the composite due to the high the volume of thepressure,
reinforcement and matrix within the composite, regardless of the thickness of the composite. In the
since the fiber volume fraction is the only value that represents the volume of the reinforcement and
LV-type, the decrease in thickness and increase in fiber volume fractions were similar because almost
matrix within
no resin the
wascomposite,
squeezed out, regardless of theinto
as impregnation thickness of the was
the composite composite. In the LV-type,
almost complete. Therefore, the
thedecrease
in thickness andinincrease
decrease thicknessin fiber
was volume
caused by thefractions
amount ofwere similar
squeezed outbecause
resin. Onalmost
the othernohand,
resinthe
was squeezed
fiber
out, as volume
impregnation into the
fraction slightly composite
increased whenwas almost complete.
the thickness Therefore,
decreased, largely the decrease
in the case in thickness
of the HV-type.
The resin
was caused appeared
by the amount to of
be squeezed
squeezed outoutfrom theOn
resin. mold,
the and impregnation
other hand, the fiberinto avolume
large area of the slightly
fraction
unimpregnated tow within the composite occurred as the pressure rising time increased. An increase
increased when the thickness decreased, largely in the case of the HV-type. The resin appeared to be
in fiber volume fraction in the MV-type and CV-type was larger than in the LV-type and HV-type.
squeezed out from the mold, and impregnation into a large area of the unimpregnated tow within
This happened because the amount of squeezed out resin was larger than the impregnation of
the composite occurred
unimpregnated fiberasasthe
the pressure rising
pressure rising time
time increased. An increase in fiber volume fraction in
increased.
the MV-type and CV-type was larger than in the LV-type and HV-type. This happened because the
amount3.2.of Density
squeezed and out
Void resin
Content was larger than the impregnation of unimpregnated fiber as the pressure
rising time Figure
increased.
3 shows the density and void content of the composite compared with the pressure rising
time in each film stacking type. As shown in Figure 3a, the density of the composite generally
3.2. Density and Void
increased Content
as pressure rising time increased. In the LV-type, the reason why density showed little
change, even with a longer pressure time, is that the tow had already been sufficiently impregnated
Figure 3 shows
during the density
the pre-heating andInvoid
process. content of
the HV-type, the composite
density rose as the compared with
pressure rising theincreased
time pressure rising
time in because
each filmofstacking type. out
the squeezed As shown in Figure
resin from 3a, the density
the decreased of the
thickness andcomposite generally
impregnation into theincreased
as pressure rising time
unimpregnated towincreased. In the LV-type,
within the composite. the reason
In the MV-type why density
and CV-type, showed
density little
increased change,
slightly as even
pressurepressure
with a longer rising timetime,
increased. Thisthe
is that is due
tow to had
the impregnation
already been of the unimpregnated
sufficiently area within during
impregnated the the
tow and a decrease in thickness resulting from squeezed out resin.
pre-heating process. In the HV-type, density rose as the pressure rising time increased because of
the squeezed out resin from the decreased thickness and impregnation into the unimpregnated tow
within the composite. In the MV-type and CV-type, density increased slightly as pressure rising time
increased. This is due to the impregnation of the unimpregnated area within the tow and a decrease in
thickness resulting from squeezed out resin.
As shown in Figure 3b, the void content also decreased as pressure rising time increased. The
void content is the sum of the voids and unimpregnated area within the composite. This happened
because, according to Equation (1), more impregnation was carried out during the pressure rising
process for sufficient time so that the density of the composite increased. In the LV-type, the void
content was 4.31% at a pressure rising time of 5 min, which means that the impregnation progressed
considerably during the pre-heating process, and the decrease in void content is small because of the
small amount of squeezed out resin, even when a longer pressure rising time is applied. On the other
hand, the void content was 9.32% at a shorter pressure rising time of 5 min in the HV-type, so the
Materials 2016, 9, 448 6 of 15

unimpregnated area was considered large, and the void content was 3.77%, even at a time of 25 min. In
the case of the HV-type, the high-melt-viscosity resin has low flowability, which makes impregnation
of the tow difficult at shorter pressure rising times and also brings inadequate impregnation, even at a
longer time. Similarly, in the MV-type and CV-type, the void content decreased as pressure rising time
increased because the remaining unimpregnated area decreases and voids come out together when the
resin is 2016,
Materials squeezed
9, 448 out. 6 of 15

Figure
Figure 3.
3. Density
Density(a)
(a)and
andvoid
voidcontent
content(b)
(b)of
ofthe
thecomposite
compositecompared
comparedwith
withthe
thepressure
pressure rising
rising time
time in
in
each
each film
film stacking
stacking type.
type.

As shown Scanning
3.3. Differential in FigureCalorimetry
3b, the void content also decreased as pressure rising time increased. The
(DSC)
void content is the sum of the voids and unimpregnated area within the composite. This happened
Figure
because, 4 showstoDSC
according patterns
Equation (1),ofmore
the composites
impregnationproduced at a pressure
was carried rising
out during thetime of 25 min.
pressure A
rising
film with
process forhigher melttime
sufficient viscosity showed
so that a lower
the density of melting temperature
the composite peak,
increased. Inbut
the the gap was
LV-type, thesmall.
void
The melting point of the CV-type was similar to the MV-type. X c of the composite
content was 4.31% at a pressure rising time of 5 min, which means that the impregnation progressedmatrix, calculated
according to Equation
considerably during the(2) based on the
pre-heating melting
process, andenthalpy of DSC,
the decrease was 30.23%
in void content for the LV-type,
is small because24.86%
of the
for theamount
small MV-type, 16.17% for
of squeezed the
out HV-type,
resin, and 26.92%
even when a longerforpressure
the CV-type.
risingAtime
filmiswith higher
applied. Onmolecular
the other
hand, the void content was 9.32% at a shorter pressure rising time of 5 min in the HV-type, so the
unimpregnated area was considered large, and the void content was 3.77%, even at a time of 25 min.
In the case of the HV-type, the high-melt-viscosity resin has low flowability, which makes
impregnation of the tow difficult at shorter pressure rising times and also brings inadequate
impregnation, even at a longer time. Similarly, in the MV-type and CV-type, the void content
3.3. Differential Scanning Calorimetry (DSC)
Figure 4 shows DSC patterns of the composites produced at a pressure rising time of 25 min. A
film with higher melt viscosity showed a lower melting temperature peak, but the gap was small.
The melting point of the CV-type was similar to the MV-type. Xc of the composite matrix, calculated
Materials 2016, 9, 448 7 of 15
according to Equation (2) based on the melting enthalpy of DSC, was 30.23% for the LV-type, 24.86%
for the MV-type, 16.17% for the HV-type, and 26.92% for the CV-type. A film with higher molecular
weight showed lower
weight showed lowercrystallinity
crystallinityofofthe
thematrix.
matrix.Crystallinity
Crystallinity in in
thethe CV-type
CV-type is similar
is similar to MV-type;
to the the MV-
type; however, the shape of the curve of the melting endotherm was slightly broad.
however, the shape of the curve of the melting endotherm was slightly broad. This happened because This happened
because
three filmsthree
with films with different
different molecular molecular weights
weights were were combined
combined [30]. [30].

Figure
Figure 4. Differential
Differential scanning
scanning calorimetry
calorimetry (DSC)
(DSC) patterns
patterns of
of the
the composites
composites produced
produced at
at aa pressure
rising
rising time of 25 min.

3.4.
3.4. Dynamical
Dynamical Mechanical
Mechanical Thermal
Thermal Analysis
Analysis (DMTA)
(DMTA)
Figure
Figure 55 shows
shows thetheviscoelastic
viscoelasticproperties
propertiesofofthe thecomposites
compositesmeasured
measuredbybyDMTA DMTAproduced
produced atat
a
pressure rising time of 25 min. In Figure 5a, the storage moduli of
a pressure rising time of 25 min. In Figure 5a, the storage moduli of all specimens decreased as all specimens decreased as
temperature increased due
temperature increased due to
tothe
thesoftening
softeningofofthe thematrix
matrixatata ahigh
hightemperature.
temperature.The The HV-type
HV-type seems
seems to
to
bebe
thethe stiffest
stiffest at room
at room temperature
temperature since
since its its storage
storage modulus
modulus is the
is the highest.
highest. TheThe storage
storage modulus
modulus of
of
thethe LV-type
LV-type was was the lowest
the lowest at room at temperature;
room temperature;however,however,
the LV-type the showed
LV-typea slower
showeddownward
a slower
downward trend as temperature rose. This shows that resin with low melt
trend as temperature rose. This shows that resin with low melt viscosity could achieve high adhesion. viscosity could achieve
high adhesion.
Therefore, Therefore, heat-resistance
heat-resistance was higher thanwas other higher than other
specimens [3,29].specimens [3,29].
As
As shown in Figure 5b, the loss factor (tan δ) provides information about
shown in Figure 5b, the loss factor (tan δ) provides information about the
the internal
internal friction
friction of
of
the
the material
material and and the
the adhesion
adhesion of of the
the interface.
interface. Broad
Broad peaks
peaks ofof the
the tan
tan δδ curve
curve were
were shown
shown scattered
scattered
around
around 4040 °C.
˝ C. The
The value
value of
of the
the peak
peak of of tan
tan δδ commonly
commonly shows
shows the the glass
glass transition
transition temperature
temperature (Tg),
(Tg),
and a higher Tg was observed compared to the general PP. This might
and a higher Tg was observed compared to the general PP. This might have been observed becausehave been observed because it
it is
is fabric
fabric reinforcement
reinforcement composite—not
composite—not a shorta fiber
shortreinforcement
fiber reinforcement
composite. composite.
Films with Films with low
low molecular
molecular weight showed a high tan δ peak temperature. This implies
weight showed a high tan δ peak temperature. This implies that films will become unstable that films will become unstable
over
over the temperature. In other words, the LV-type shows high heat resistance,
the temperature. In other words, the LV-type shows high heat resistance, as in the storage modulus as in the storage
modulus curve [31,32].
curve [31,32].
Materials 2016, 9, 448 8 of 15
Materials 2016, 9, 448 8 of 15

Figure
Figure 5. Dynamical
Dynamical mechanical
mechanical thermal
thermal analysis
analysis (DMTA)
(DMTA) of of the
the composites
composites produced
produced at
at pressure
rising
rising time of 25 min. (a)
(a) Storage
Storage modulus;
modulus; (b) loss factor (tan δ).

3.5.
3.5. Tensile
Tensile Properties
Properties
Figure
Figure 66 shows
shows thethe tensile
tensile strength
strength and
and tensile
tensile modulus
modulus of of the
the composite
composite compared
compared with with the
the
pressure
pressure rising
rising time
time inin each
each film
film stacking
stacking type.
type. In
In Figure
Figure 6a,
6a, the
the tensile
tensile strength
strength generally
generally rose
rose as
as the
the
pressure rising time increased. For the LV-type, since there was no big change
pressure rising time increased. For the LV-type, since there was no big change in the fiber volume in the fiber volume
fraction
fraction of
ofFigure
Figure2b2bandandinindensity
density ofof
Figure 3a,3a,
Figure which
whichis because resin
is because which
resin melted
which during
melted the pre-
during the
heating process due to its low melt viscosity promoted impregnation at a shorter
pre-heating process due to its low melt viscosity promoted impregnation at a shorter pressure rising pressure rising time,
no more
time, impregnation
no more impregnation was was
processed, eveneven
processed, with a longer
with a longer pressure
pressure rising
risingtime,
time,and
andsurplus
surplus resin
resin
hardly
hardly came
came out,
out, such
such that
that there
there was
was almost
almost no
no change
change in in thickness
thickness ofof the
thecomposite.
composite.In Inthe
theHV-type,
HV-type,
the
the tensile
tensile strength
strength increased
increased greatly
greatly asas pressure
pressure rising
rising time
time increased.
increased. TheThe tensile
tensile strength
strength increased
increased
considerably
considerably from 525.60 MPa to 613.56 MPa when the pressure rising time increased from
from 525.60 MPa to 613.56 MPa when the pressure rising time increased from 55 min
min to
to
25
25 min.
min. As
As shown
shown inin Figure
Figure 2,2, this
this happened
happened because
because the
the thickness
thickness ofof the
the composite
composite decreased
decreased as as the
the
pressure rising time
pressure rising time increased
increased and and impregnation
impregnationthen thenincreased.
increased.The TheMV-type
MV-typeand andCV-type
CV-typeshowed
showeda
a similar tendency towards increased tensile strength as the pressure rising time increased. This is
which was 10% lower than 586.82 MPa of the LV-type. This is apparently due to high thickness, in
accordance with unimpregnation. On the other hand, at a pressure rising time of 25 min, the tensile
strength of the HV-type was 613.56 MPa, which is higher than 604.28 MPa for the LV-type. In spite of
a higher void content, a lower fiber volume fraction, and a higher thickness, the HV-type showed
higher tensile strength than the LV-type. That is, the high melt viscosity film with a large molecular
Materials 2016, 9, 448 9 of 15
weight generally had a high tensile strength, such that impregnation of the composite was almost
complete at a pressure rising time of 25 min, which indicates a contribution of the film strength. The
difference in the towards
similar tendency tensile strength
increasedoftensile
the MV-type
strength and CV-type
as the pressurewas small,
rising timeand their values
increased. This iswere
due
around the average
to the decrease of the caused
in thickness LV-typebyand HV-type.
squeezed Therefore,
out resin and thethe tensile
slight strength
increase in theisfiber
affected
volume by
composite
fraction as thickness resulting
pressure rising timefrom impregnation
became longer. throughout the pressure rising process.

Figure 6. Tensile
Tensile strength
strength (a)
(a) and
and tensile
tensile modulus
modulus (b)
(b) of
of the
the composite
composite compared withthe
comparedwith the pressure
rising time in each film stacking type.

To compare the tensile strength of the composite with the film melt viscosity, at a pressure rising
time of 5 min, the tensile strength of the HV-type with a higher melt viscosity film was 525.60 MPa,
which was 10% lower than 586.82 MPa of the LV-type. This is apparently due to high thickness, in
accordance with unimpregnation. On the other hand, at a pressure rising time of 25 min, the tensile
strength of the HV-type was 613.56 MPa, which is higher than 604.28 MPa for the LV-type. In spite of a
higher void content, a lower fiber volume fraction, and a higher thickness, the HV-type showed higher
tensile strength than the LV-type. That is, the high melt viscosity film with a large molecular weight
generally had a high tensile strength, such that impregnation of the composite was almost complete at
a pressure rising time of 25 min, which indicates a contribution of the film strength. The difference in
Materials 2016, 9, 448 10 of 15

the tensile strength of the MV-type and CV-type was small, and their values were around the average
of the LV-type and HV-type. Therefore, the tensile strength is affected by composite thickness resulting
from impregnation throughout the pressure rising process.
As shown in Figure 6b, the tensile modulus in each melt viscosity of the film showed a similar
tendency with tensile strength. On the other hand, the tensile modulus in the HV-type rose by 50%
from 21.02 GPa to 32.29 GPa, unlike that in the LV-type, MV-type, and CV-type, when the pressure
rising time increased from 5 min to 25 min. This is due to a decrease in strain at break caused by an
increase in impregnation.

3.6. Flexural Properties


Figure 7 shows the flexural strength and flexural modulus of the composite compared with the
pressure rising time in each film stacking type. As shown in Figure 7a, the flexural strength for all
four composites increased as pressure rising time increased. In the LV-type, the flexural strength
slightly increased as pressure rising time increased because the viscosity decreased enough to allow
the low melt viscosity tow to be impregnated during the pre-heating process; thus, there were no
large differences in impregnation, even with a longer pressure rising time. In the HV-type, the flexural
strength increased greatly as the pressure rising time increased. When the pressure rising time increased
from 5 min to 25 min, the flexural strength rose 39%, from 106.09 MPa to 145.84 MPa. This is a great
increase compared to a decrease in composite thickness by 8.62%. This is due to the impregnation of the
large unimpregnated area within the tow at a longer pressure rising time, and high-molecular-weight
films have higher flexural properties than low-molecular-weight films. The flexural strengths of the
MV-type and CV-type showed a similar tendency towards their tensile strengths.
To compare the flexural strength of the composite with the film melt viscosity, at 5 min, the
flexural strength of the HV-type was 106.09 MPa, which is 6.07% lower than 112.95 MPa of the LV-type.
This happened because the HV-type is thicker and has a wide unimpregnated area. On the other hand,
the difference in flexural strength was small compared to the 11.64% difference between the tensile
strength of the HV-type and LV-type. This happened because, even in the case of using high melt
viscosity film, impregnation occurs at a short pressure rising time and during the pre-heating process.
In other words, flexural strength is strongly influenced by the binding force of the impregnation of the
fiber and the matrix. At a longer pressure rising time of 25 min, the flexural strength of the HV-type
was much higher at 145.84 MPa than 115.96 MPa for the LV-type. Although Vc is high in the HV-type,
it is due to an increase in the load to break, as impregnation was almost complete and thickness
increased. That is, high mechanical properties of the film with a high molecular weight contributed
to the flexural strength of the composite. In the CV-type and MV-type, the CV-type showed a higher
flexural strength than the MV-type at all pressure rising times. Unlike in the MV-type, at a shorter
pressure rising time of 5 min, impregnation first occurs in the case of low melt viscosity film, which
means more fibers could be impregnated in the CV-type, resulting in high flexural strength. At a longer
pressure rising time of 25 min, impregnation was almost complete for both types of films such that the
outer layer of the tow in the CV-type appeared to be impregnated by high-melt-viscosity resin. As
shown in the prediction zone under 5 min, impregnation occurred more in the CV-type during the
pre-heating process than in the MV-type, and it occurs more easily during the pressure rising process
as well. Thus, the LV-type showed low flexural strength when impregnation was completed fast, but
the HV-type showed high flexural strength when impregnation was completed slowly.
As shown in Figure 7b, the flexural modulus showed a similar tendency with the flexural strength.
Especially in the HV-type, the flexural modulus increased 53.76% from 9.02 GPa to 13.87 GPa when
the pressure rising time increased from 5 min to 25 min. This happened because the composite became
stiff, as the film with high molecular weight and tow completed impregnation when the pressure rising
time increased. Therefore, the properties and impregnation of the film in the composite have a great
effect on the flexural property.
Materials 2016, 9, 448 11 of 15
Materials 2016, 9, 448 11 of 15

Figure
Figure 7.7. Flexural
Flexural strength
strength (a)
(a) and
and flexural
flexural modulus
modulus (b)
(b) of
of the
the composite
composite compared
compared with
with the
the pressure
pressure
rising
rising time in each film stacking type.

As shown in
3.7. Interlaminar Figure
Shear Stress7b, the flexural modulus showed a similar tendency with the flexural
(ILSS)
strength. Especially in the HV-type, the flexural modulus increased 53.76% from 9.02 GPa to 13.87
Figure 8 shows the ILSS of the composite compared with the pressure rising time in each film
GPa when the pressure rising time increased from 5 min to 25 min. This happened because the
stacking type. The ILSS of the four composites showed a different tendency as the pressure rising
composite became stiff, as the film with high molecular weight and tow completed impregnation
time increased. The ILSS in the LV-type showed almost no change in accordance with increases in
when the pressure rising time increased. Therefore, the properties and impregnation of the film in
pressure rising time. This is due to complete impregnation during the pre-heating process. The
the composite have a great effect on the flexural property.
ILSS slightly decreased as the pressure rising time increased because of a small amount of resin that
existed
3.7. betweenShear
Interlaminar the carbon fiber layers. ILSS in the HV-type increased continuously as pressure
Stress (ILSS)
rising time increased. This is due to a decrease in thickness and V c as impregnation increased. In
Figure 8 and
the MV-type shows the ILSS
CV-type, of the composite
however, compared until
the ILSS increased with 13
themin
pressure
in therising
MV-typetimeand
in each
9 minfilm
in
stacking type. The ILSS of the four composites showed a different tendency as the pressure
the CV-type, and then decreased thereafter. The ILSS implies the strength when the interface of the rising
time
carbonincreased. Theseparate;
fiber layers ILSS in therefore,
the LV-type showedtoalmost
it appears noatchange
increase in pressure
a shorter accordance with
rising increases
time in
due to the
pressure rising time. This is due to complete impregnation during the pre-heating process.
decrease in thickness and void content, which reduces the unimpregnated area. With a longer pressure The ILSS
slightly decreased as the pressure rising time increased because of a small amount of resin that existed
between the carbon fiber layers. ILSS in the HV-type increased continuously as pressure rising time
increased. This is due to a decrease in thickness and Vc as impregnation increased. In the MV-type
Materials 2016, 9, 448 12 of 15

and CV-type, however, the ILSS increased until 13 min in the MV-type and 9 min in the CV-type, and
then decreased thereafter. The ILSS implies the strength when the interface of the carbon fiber layers
Materials 2016, 9, 448 12 of 15
separate; therefore, it appears to increase at a shorter pressure rising time due to the decrease in
thickness and void content, which reduces the unimpregnated area. With a longer pressure rising
time,
risingthe
time,layer
thebecomes thinnerthinner
layer becomes as the as
resin
the between the carbon
resin between fiber layers
the carbon is squeezed
fiber layers out after
is squeezed out
impregnation.
after impregnation. The MV-type
The MV-typeand and
CV-type in terms
CV-type of of
in terms thethe
pressure
pressurerising
risingtime
timeshowed
showedaa similar
similar
tendency.
tendency. ILSSILSSwas wasslightly
slightly lower
lower in the
in the CV-type
CV-type than
than in thein the MV-type
MV-type as pressure
as pressure rising timerising time
increased.
increased. Here, impregnation was almost complete such that the resin within a carbon
Here, impregnation was almost complete such that the resin within a carbon fiber layer had a higher fiber layer
had a higher
stiffness in thestiffness
CV-typein than
the CV-type than in the
in the MV-type. MV-type.
However, theHowever,
differencethe
wasdifference was small.
small. Since Since
the changes
the changes in thickness and fiber volume fraction were similar, the resin layers between
in thickness and fiber volume fraction were similar, the resin layers between the carbon fiber layers the carbon
fiber
were layers
similar.were similar.

Figure 8. Interlaminar
Interlaminar shear
shear strength
strength (ILSS)
(ILSS) of
of the
the composite
composite compared
compared with
with the
the pressure
pressure rising time
in each film stacking type.

3.8.
3.8. Scanning
Scanning Electron
Electron Microscopy
Microscopy (SEM)
(SEM)
Figure
Figure 99 shows
showscross-section
cross-sectionSEM SEMimages
imagesinin accordance
accordance with
with thethe pressure
pressure rising
rising timetime in each
in each film
film stacking
stacking type.type. The LV-type
The LV-type showedshowed complete
complete impregnation
impregnation at a shorter
at a shorter pressure
pressure rising rising
time oftime of
5 min.
5The
min. The HV-type showed a large unimpregnated area at 5 min and incomplete
HV-type showed a large unimpregnated area at 5 min and incomplete impregnation, even at a impregnation, even
at a longer
longer pressure
pressure rising
rising time time
of 25of 25 min.
min. This This
shows shows thatmelt
that the the viscosity
melt viscosity
of theof theand
film filmpressure
and pressure
rising
rising time affect
time affect impregnation.
impregnation. The MV-type
The MV-type and CV-type
and CV-type showed showed similar
similar impregnation
impregnation in terms
in terms of
of the
the pressure rising time; however, impregnation in the CV-type occurred slightly
pressure rising time; however, impregnation in the CV-type occurred slightly faster as the pressure faster as the
pressure
rising timerising
wastime was increased
increased from 5 minfrom 5 min
to 13 min.toThis
13 min. This
is due to is due to impregnation
impregnation by the low bymelt
the low melt
viscosity
viscosity
film, whichfilm, which
first first occurred
occurred in the CV-type.
in the CV-type.
Materials 2016, 9, 448 13 of 15
Materials 2016, 9, 448 13 of 15

Figure 9. Cross-section SEM images in accordance with the pressure rising time in each film stacking
Figure 9. Cross-section SEM images in accordance with the pressure rising time in each film stacking
type; (a) LV-type; (b) MV-type; (c) HV-type; (d) CV-type.
type; (a) LV-type; (b) MV-type; (c) HV-type; (d) CV-type.

4. Conclusions
4. Conclusions
To produce film-type thermoplastic composites, three PP films with different melt viscosities
To produce film-type thermoplastic composites, three PP films with different melt viscosities were
were used. A film with a low melt viscosity was stacked so that tow was impregnated first; then, a
used. A film with a low melt viscosity was stacked so that tow was impregnated first; then, a film
film with a higher melt viscosity was stacked to produce the composite. The mechanical properties
with a higher melt viscosity was stacked to produce the composite. The mechanical properties of the
of the composite were identified and the following conclusions were made.
composite were identified and the following conclusions were made.
As pressure rising time increased, the thickness of the four composites decreased due to
As pressure rising time increased, the thickness of the four composites decreased due to
squeezed out resin, increased fiber volume fraction, and increased density, and the Vc decreased as
squeezed out resin, increased fiber volume fraction, and increased density, and the V c decreased
impregnation increased.
as impregnation increased.
The tensile strength increased slightly in the LV-type, but greatly in the HV-type as pressure
The tensile strength increased slightly in the LV-type, but greatly in the HV-type as pressure
rising time increased. This increased similarly in the MV-type and in the CV-type. The tensile strength
rising time increased. This increased similarly in the MV-type and in the CV-type. The tensile
was affected by the composite thickness resulting from impregnation throughout the pressure rising
strength was affected by the composite thickness resulting from impregnation throughout the pressure
process.
rising process.
In the case of flexural strength, it increased slightly in the LV-type, but greatly in the HV-type as
In the case of flexural strength, it increased slightly in the LV-type, but greatly in the HV-type
pressure rising time increased. The MV-type and CV-type showed a similar tendency, but the CV-
as pressure rising time increased. The MV-type and CV-type showed a similar tendency, but the
type had higher values at each pressure rising time. LV-type showed low flexural strength when
CV-type had higher values at each pressure rising time. LV-type showed low flexural strength when
impregnation was completed fast, but HV-type showed high flexural strength when impregnation
impregnation was completed fast, but HV-type showed high flexural strength when impregnation was
was completed slowly.
completed slowly.
The ILSS mostly decreased, except in the case of the HV-type because the resin layer between
The ILSS mostly decreased, except in the case of the HV-type because the resin layer between the
the carbon fiber layers decreased as pressure rising time increased.
carbon fiber layers decreased as pressure rising time increased.
Appropriate films should be used considering the forming process time and their mechanical
properties to produce film-type composites.
Materials 2016, 9, 448 14 of 15

Appropriate films should be used considering the forming process time and their mechanical
properties to produce film-type composites.

Acknowledgments: Authors sincerely appreciate Hae Jin Cho for his assistance on the experiments.
Author Contributions: Jong Won Kim carried out the experimental study and wrote the manuscript;
Joon Seok Lee supervised the research and design of the study.
Conflicts of Interest: The authors declare no conflict of interest.

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© 2016 by the authors; licensee MDPI, Basel, Switzerland. This article is an open access
article distributed under the terms and conditions of the Creative Commons Attribution
(CC-BY) license (http://creativecommons.org/licenses/by/4.0/).

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