materials

Article

Influence of Interleaved Films on the Mechanical

Properties of Carbon Fiber Fabric/Polypropylene
Thermoplastic Composites
Jong Won Kim 1 and Joon Seok Lee 2, *
1
2

Regional Research Institute for Fiber & Fashion Materials, Yeungnam University, Gyeongsan 712-749, Korea;
kjwfiber@ynu.ac.kr
Department of Textile Engineering and Technology, Yeungnam University, Gyeongsan 712-749, Korea
Correspondence: leejs@ynu.ac.kr; Tel.: +82-53-810-2774

Academic Editor: Luciano Feo

Received: 2 March 2016; Accepted: 4 May 2016; Published: 6 May 2016

Abstract: A laminated composite was produced using a thermoplastic prepreg by inserting an

interleaved film with the same type of matrix as the prepreg during the lay-up process to improve the
low interlaminar properties, which is a known weakness of laminated composites. Carbon fiber fabric
(CFF) and polypropylene (PP) were used to manufacture the thermoplastic prepregs. Eight prepregs
were used to produce the laminated composites. Interleaved films with different thicknesses were
inserted into each prepreg. The physical properties of the composite, such as thickness, density, fiber
volume fraction (V f ), and void content (V c ), were examined. The tensile strength, flexural strength,
interlaminar shear strength (ILSS), impact property, and scanning electron microscopy (SEM) were
used to characterize the mechanical properties. Compared to the composite without any inserted
interleaved film, as the thickness of the inserted interleaved resin film was increased, V c decreased
by 51.45%. At the same time, however, the tensile strength decreased by 8.75%. Flexural strength
increased by 3.79% and flexural modulus decreased by 15.02%. Interlaminar shear strength increased
by 11.05% and impact strength increased by 15.38%. Fracture toughness of the laminated composite
was improved due to insertion of interleaved film.
Keywords:
interleaved film;
compression molding

thermoplastic composite;

polypropylene;

surplus resin;

1. Introduction
Carbon fiber-reinforced polymer composites with high mechanical properties and light
weight have been used widely in many engineering fields. In recent times, continuous fiber
reinforced thermoplastic (CFRTP) composites have been used more widely because of their many
advantages, such as fracture toughness and damage tolerance, ease of shape forming before
consolidation, significantly faster manufacturing, longer shelf life of the raw material, and the
ability to be reshaped and reused. These advantages are based mostly on the intrinsic properties
of thermoplastic polymers [1]. According to the development of high performance polymers,
such as polyetheretherketone (PEEK), polyethersulphone (PES), polyphenylene sulphide (PPS),
polyethyleneterephthalate (PET), polycarbonate (PC), polyamide (PA) and polypropylene (PP), the
so-called engineering plastics show significant mechanical properties [2]. In particular, a high flexural
strength, high thermal stability, ease of processing, resistance to corrosion, low density, and low
price has made PP one of the more promising materials as a matrix among the various thermoplastic
polymers available [3,4].
Prepreg materials, in which the reinforcing fibers are pre-impregnated with resin, are commonly
used to produce thermoplastic composites. The quality of the prepreg can have a significant effect on
Materials 2016, 9, 344; doi:10.3390/ma9050344

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the mechanical performance of the composite. Three of the most widely used prepregging techniques
are film prepregging, hot melt prepregging and solution dip prepregging [5]. In the case of film
prepregging, the pressure-temperature history of the polymer dominates the impregnation quality
(void content). For melting impregnation, however, this is impractical for certain polymers because of
their limited tolerance to the temperatures necessary for viscosity reduction. The 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 [6]. In addition, the use of large
pressures to impregnate the polymer film into the fiber has mechanical limitations.
Considerable research has been done to discover practical methods to produce composite parts
using thermoplastic prepregs. Currently, most promising processing methods include compression
molding, tape winding, tape laying, braiding, and pultrusion [7]. Interlayer delamination tends to
take place when two-dimensional laminated composites using film pregregs are subject to impact
and bending compression [8]. Consequently, they have relatively poor through-thickness mechanical
properties compared to that in the fiber direction. This is because the through-thickness mechanical
properties are carried predominantly by the resin matrix. Delamination can be a most serious problem
because it can reduce the mechanical properties and is difficult to detect visually [9]. Interlaminar
properties of two-dimensional laminated composites can be enhanced by toughening the matrix [10],
insertion of an interleaf layer [11,12], reinforcing with three-dimensional braided or woven fabrics [13],
stitching of reinforcements [14], reinforcing with felts [15], and the insertion of fillers, such as carbon
nanotubes, into the matrix [16,17]. In other research on the insertion of interleaved film layers,
either different polymers [18,19] or polymer films, consisting of the same polymer but with different
properties [2023], have simply been inserted during the forming process. Therefore, this study
examined the effects of the thickness of an interleaved film made of the same polymer film as the
matrix material on the mechanical properties of laminated composites using thermoplastic prepreg.
2. Experimental Section
2.1. Materials
Woven fabric (SNC1242R, Plain, density (counts/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. For the matrix, 20 m PP film (SBF-110, =0.9 g/cm3 , tensile strength = 75 MPa, Samyoung
Chemical Co., Seoul, Korea) was used, and the PP film with the same thickness was also used as the
interleaved film layer.
2.2. Preparation of the Prepreg and Laminated Composite
During the prepreg manufacturing process (Figure 1a) using carbon fiber fabric (CFF) and PP,
seven PP films were laminated inside the mold (295 295 mm2 ) both above and below the CFF. The
mold was designed to have a space between the upper and lower molds to allow surplus resin come
out. After the mold was preheated inside a hot press, at a temperature of 230 C for 10 min, the
pressure was increased slowly to 28 MPa for 10 min. This is because if a high pressure is applied
abruptly, the carbon fiber could be out of alignment, the resin cannot be impregnated into the fabric
and the voids are difficult to squeeze out from the inter-layer. After a dwell time of 10 min, the mold
was then cooled to room temperature. Subsequently, the pressure was relieved and the prepreg was
then detached from the mold. The produced prepreg had a 0.45 mm thickness with a 53.81% fiber
volume fraction (V f ).
A similar procedure was used to prepare the laminated composite through compression molding
by laminating (0 /90 ) 8 prepregs, as shown in Figure 1b. The forming cycle was carried out in the
same manner as prepreg production. Interleaved films were inserted between each prepreg while
laminating 8 prepregs and compression molding was then carried out. The thickness of the interleaved
film was varied by changing the number of interleaved films, which interleaved PP between each layer

Materials 2016, 9, 344

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consists some of them, in the manufactured specimen. The procedure was carried out identically to the
prepreg manufacturing process. As before, the pressure was increased slowly to 28 MPa to squeeze
out
the resin from the inter-layer.
Materials 2016, 9, 344
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Figure 1. Scheme of hot press processing; (a) prepregs; (b) composites.

Figure 1. Scheme of hot press processing; (a) prepregs; (b) composites.

A similar procedure was used to prepare the laminated composite through compression
2.3. Composites Characterization
molding by laminating (0/90) 8 prepregs, as shown in Figure 1b. The forming cycle was carried out
The
specimen
thickness
(mm)
was averaged
by measuring
5 places,
including
4 edges
the
in the
same
manner
as prepreg
production.
Interleaved
films were
inserted
between
each and
prepreg
center,
of each 5 specimens
thickness gauge.
Thewas
actual
density
using
while laminating
8 prepregsusing
and acompression
molding
then
carriedwas
out.determined
The thickness
of the
the
Archimedes
the ASTMthe
D 792
by measuring
the differences
between
the weight
interleaved principle
film was according
varied bytochanging
number
of interleaved
films, which
interleaved
PP
of
a
specimen
in
air
and
in
water.
The
V
of
the
specimen
was
calculated
using
a
burn-off
test
according
between each layer consists some off them, in the manufactured specimen. The procedure was
to
ASTMout
D 2584.
The specimen
was inserted
into a furnace
in an
environment
for 10
h at
500 C,
carried
identically
to the prepreg
manufacturing
process.
Asinert
before,
the pressure
was
increased
followed
drying
in a desiccator.
The from
fiber the
volume
fraction was then calculated based on the
slowly to by
28 MPa
to squeeze
out the resin
inter-layer.
specimen weight ratio before and after the burn-off test. The void volume content (V c ) was determined
2.3. Composites
using
Equation Characterization
(1) below based on the ASTM D 2734 as follows:
by measuring 5 places,
including 4 edges and the
The specimen thickness (mm) was averaged
%mmatrix %mfiber
Vc

100

(1)
`
samplegauge. The actual density was determined using the
center, of each 5 specimens using a thickness
matrix
fiber
Archimedes principle according to the ASTM D 792 by measuring the differences between the
where
the voidinvolume
content
is the
thespecimen
primary was
density
and %m
is athe
mass test
of
weightVofc aisspecimen
air and in
water. (%),
The Vf of
calculated
using
burn-off
each
constituent.
according
to ASTM D 2584. The specimen was inserted into a furnace in an inert environment for 10
tensile
strength,
flexural
andThe
interlaminar
shear
strength
were measured
h at The
500 C,
followed
by drying
in strength
a desiccator.
fiber volume
fraction
was(ILSS)
then calculated
based
using
tensile tester
(OTT-05,
Co.,after
Seoul,
to determine
the mechanical
properties
of
on thea specimen
weight
ratio Oriental
before and
theKorea)
burn-off
test. The void
volume content
(Vc) was
the
preparedusing
specimens.
The(1)
tensile
test
was performed
according
ASTM D 3039 at a crosshead
determined
Equation
below
based
on the ASTM
D 2734 to
as the
follows:
speed of 2 mm/min. A three-point-bending test was %m
carried out based
%m on the ASTM D 790 to measure
c
100
(1)
the flexural strength with a span-to-depth ratio of 16 at a crosshead speed of 1.3 mm/min. ILSS was
also measured using a three-point-bending test based on the ASTM D 2344 with a span-to-depth ratio
where
c is the void volume content (%), is the primary density and %m is the mass of each
of
4 at a Vcrosshead
speed of 1 mm/min. A drop weight impact test was conducted using a drop-weight
constituent.
impact testing machine (Ceast 9350, Instron, Norwood, MA, USA) equipped with a 12.7 mm diameter
The tensile
flexural
strength
and
shear
strength
were
measured
hemispherical
tip.strength,
The test was
conducted
with
aninterlaminar
impact velocity
of 2.57
m/s2(ILSS)
, 15.13 kg
mass
and an
2
using
a
tensile
tester
(OTT-05,
Oriental
Co.,
Seoul,
Korea)
to
determine
the
mechanical
properties
of
impact energy of 50 J. The specimen was prepared in 100 100 mm . The cross section of prepared
the
prepared
specimens.
The
tensile
test
was
performed
according
to
the
ASTM
D
3039
at
a
composite was observed by scanning electron microscopy (SEM, S-4100, Hitachi, Tokyo, Japan).
crosshead speed of 2 mm/min. A three-point-bending test was carried out based on the ASTM D 790
3.
Results and
Discussion
to measure
the flexural
strength with a span-to-depth ratio of 16 at a crosshead speed of 1.3 mm/min.
ILSS was also measured using a three-point-bending test based on the ASTM D 2344 with a
3.1.
Thickness and
Density
span-to-depth
ratio
of 4 at a crosshead speed of 1 mm/min. A drop weight impact test was
conducted
using
a
drop-weight
testingofmachine
(Ceastlaminated
9350, Instron,
Norwood,
MA, USA)
Figure 2 shows the thicknessimpact
and density
the prepared
composite
determined
by
equipped
with
a
12.7
mm
diameter
hemispherical
tip.
The
test
was
conducted
with
an impact
varying the thickness of the interleaved films between each of the 8 prepregs, ranging from
0 m
velocity
of 2.57
m/s2, 15.13 thickness
kg mass and
anthickness
impact energy
50 J. Theassuming
specimen that
was the
prepared
in
to
140 m.
The theoretical
is the
of the of
composite
inserted
2. The cross section of prepared composite was observed by scanning electron
100

100
mm
films are not squeezed out during compression molding. The actual thickness is the thickness of
microscopy (SEM, S-4100, Hitachi, Tokyo, Japan).

3.1. Thickness and Density

Figure 2 shows the thickness and density of the prepared laminated composite determined by
varying the thickness of the interleaved films between each of the 8 prepregs, ranging from 0 m to
Materials 2016, 9, 344
4 of 12
140 m. The theoretical thickness is the thickness of the composite assuming that the inserted films
are not squeezed out during compression molding. The actual thickness is the thickness of the
composite
measured
after
thethe
films
were
squeezed
out
the composite
measured
after
films
were
squeezed
outunder
underhigh
highpressure
pressureduring
during compression
compression
molding.
molding. Thickness
Thickness of
of the
the composite
composite without
without interleaved
interleaved film
film was
was 3.52
3.52 (0.11)
(0.11)mm.
mm. When
When aa 20
20 m
m
interleaved
film
was
inserted
between
each
of
the
eight
prepregs,
the
thickness
of
the
composite
was
interleaved film
the eight prepregs,
the composite was
3.65
which is
is similar
similartotothe
thetheoretical
theoreticalthickness
thickness
3.66
mm.
It because
is because
resin
is squeezed
3.65 mm which
ofof
3.66
mm.
It is
no no
resin
is squeezed
out
out
if interleaved
is thin.
However,
a gap
between
theoretical
thickness
and
real
thickness
grew
if interleaved
filmfilm
is thin.
However,
a gap
between
theoretical
thickness
and
real
thickness
grew
as
as
interleaved
film
became
thicker.ItItisisbecause
becausemore
moresurplus
surplusresin
resinwas
was squeezed
squeezed out under high
thethe
interleaved
film
became
thicker.
high
pressure. Additionally,
Additionally, change in the composite thickness was small over interleaved
interleaved film thickness
of
decreased from
from 1.32
1.32 g/cm
g/cm33 to
g/cm33while
of 80 m. Density decreased
to 1.29 g/cm
whilethickness
thicknessof
of the
the interleaved
interleaved film
increased
sinceVVf fofofthe
thecomposite
composite
decreased
from
insertion
ofinterleaved
the interleaved
film. was
There
was
increased since
decreased
from
insertion
of the
film. There
almost
almost
no difference
in above
density
80 m similar
because,
to the thickness,
of the
inserted
no difference
in density
80above
m because,
to similar
the thickness,
most of themost
inserted
interleaved
interleaved
films were
squeezed
from the mould.
films were squeezed
out
from theout
mould.

Figure
Figure 2.
2. Thickness
Thickness and
and density
density of
of the
the laminated
laminated composites
composites at
at various
various interleaved
interleaved film thicknesses.

3.2.
3.2. Fiber
Fiber Volume
Volume Fraction
Fraction and
and Void
Void Content
Content
Figure
Figure 33 shows
shows V
Vff and
and VVccofofthe
thecomposite
compositeat
atvarious
variousinterleaved
interleavedfilm
film thicknesses
thicknesses up
up to
to 140
140 m
m
between
between each
each of
of the
the eight
eight prepregs.
prepregs. As
As thickness
thicknessof
ofinterleaved
interleavedfilm
filmincreased
increasedfrom
from00m
mto
to140
140m,
m,
V
Vff decreased
decreased from
from 55.01%
55.01% to
to 48.52%.
48.52%. ItIt is
is because
because inserted
inserted interleaved
interleaved film
film increased
increased the
the volume
volume of
of
composite
matrix.
Also,
up
to
the
film
thickness
of
40
m,
surplus
resin
remained
within
the
composite matrix. Also, up to the film thickness of 40 m, surplus resin remained within the composite
composite
without
beingout
squeezed
so that Vf decreased sharply. In contrast, the decrease range
without being
squeezed
so that Vout
f decreased sharply. In contrast, the decrease range of Vf declined
of
V
f
declined
due
to
squeezed
out
surplus
resinSimilar
over 80to
m.
to Vf, Vfrom
c decreased
2.48%
due to squeezed out surplus resin over 80 m.
V f ,Similar
V c decreased
2.48% from
to 1.13%
as
to
1.13%
as
thickness
of
the
interleaved
film
increased.
It
is
because,
based
on
Equation
(1),
the
thickness of the interleaved film increased. It is because, based on Equation (1), the amount of resin
amount
resina increased
from
decrease
in interleaved
Vf. When 20film
mwas
interleaved
was inserted,
it
increasedoffrom
decrease in
V f . aWhen
20 m
inserted,film
it decreased
slightly
decreased
slightly
from
2.48%
to
2.40%.
As
shown
in
Figure
2,
it
is
because
no
surplus
resin
was
from 2.48% to 2.40%. As shown in Figure 2, it is because no surplus resin was squeezed out. However,
squeezed
out.
However,
the
film
of 20 m
and 80
m,
it decreased
from
between the
film
thicknessbetween
of 20 m
and
80 thickness
m, it decreased
greatly
from
2.40%
to 1.54%.greatly
It is because
2.40%
to
1.54%.
It
is
because
surplus
resin
was
squeezed
out
together
with
voids
during
the
forming
surplus resin was squeezed out together with voids during the forming process under high pressure.
process
under
high pressure.
After
decrease
range
void was
because void
content
After that,
the decrease
range of
voidthat,
wasthe
small
because
voidof
content
wassmall
low. Therefore,
insertion
of
was
low. Therefore,
insertion
interleaved
out ofcould
surplus
resin more
so that
interleaved
film causes
squeezeofout
of surplusfilm
resincauses
so thatsqueeze
void content
decrease
orvoid
less.
content could decrease more or less.

Materials 2016, 9, 344

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2016, 9,
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12
55 of

Figure 3.
3. Fiber
Fiber volume
volume fraction
fraction and
and void
void content
content of
of the
the laminated
laminated composites
composites at
at various
various interleaved
interleaved
fraction
Figure
film thicknesses.
thicknesses.
film

3.3. Tensile
Tensile Properties
Properties
3.3.
Tensile
Figure 44 shows
shows the
the tensile
tensile strength
strength and
and tensile
tensile modulus
modulus of
of the
the laminated
laminated composite
composite according
according
Figure
Figure
to
thickness
of
the
interleaved
film.
The
tensile
strength
and
tensile
modulus
showed
a
tendency
to
to thickness
thickness of the interleaved
interleaved film. The
The tensile
tensile strength
strength and tensile
tensile modulus
modulus showed
showed a tendency
tendency to
decrease with
with increasing
increasing thickness
thickness of
of the
the interleaved
interleaved film.
film.
decrease

Figure 4.
4. Tensile
Tensile strength
strength and
and tensile
tensile modulus
modulus of
of the
the laminated
laminated composites
composites at
at various
various interleaved
interleaved
Figure
Tensile
film thicknesses.
thicknesses.
film

Tensile strength
strength declined
declined from
from 796.82
796.82 MPa
MPa to
to 727.04 MPa
MPa while thickness
thickness of the
the interleaved film
film
Tensile
Tensile strength
declined from
796.82 MPa
to 727.04
727.04 MPa while
while thickness of
of the interleaved
interleaved film
increased
to
140
m.
Although
V
c decreases, it is mainly because of a decrease in Vf. However, tensile
increased
Vc decreases,
it is mainly because of a decrease in Vf. However, tensile
increased to
to 140
140 m.
m. Although
Although V
c decreases, it is mainly because of a decrease in V f . However, tensile
properties were
were mostly
mostly lower
lower than
than
that of
of general
general carbon
carbon fiber
fiber composites.
composites. It
It seems that
that aa small
small
properties
that
properties were mostly lower than that of general carbon
fiber composites.
It seems seems
that a small amount
amount
of
air
flew
in
during
the
heating
process
at
500
C
for
5
h
under
an
inert
environment
to
amount
of in
airduring
flew in
the
heating
process
at 5500
C foran5inert
h under
an inert to
environment
to
C for
of air flew
theduring
heating
process
at 500
h under
environment
desize carbon
desize
carbon
fiber
composite,
so
that
the
strength
of
the
carbon
fiber
declined
[7].
The
tensile
desize
carbon fiber
composite,
so that
thecarbon
strength
ofdeclined
the carbon
declined
[7]. The
tensilea
fiber composite,
so that
the strength
of the
fiber
[7]. fiber
The tensile
modulus
showed
modulus
showed
a
similar
tendency
to
the
tensile
strength
changing
from
15.03
GPa
to
13.61
GPa
as
modulus showed a similar tendency to the tensile strength changing from 15.03 GPa to 13.61 GPa as
the
thickness
of
the
interleaved
film
increased.
This
is
because
strain
to
break
increased
due
to
the thickness of the interleaved film increased. This is because strain to break increased due to aa
decrease of
of V
Vff..
decrease

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12
to the tensile strength changing from 15.03 GPa to 13.61 GPa as the thickness of
interleaved film increased. This is because strain to break increased due to a decrease of V f .
3.4. Flexural Properties
3.4. Flexural Properties
Figure 5 shows the flexural strength and flexural modulus of the laminated composites for
various
interleaved
film
thicknesses
eachmodulus
of the eight
contrast for
to various
tensile
Figure
5 shows the
flexural
strengthbetween
and flexural
of the prepregs.
laminated In
composites
properties,
strength between
increasedeach
slightly
MPa In
to contrast
120.58 MPa
as thickness
of
interleaved flexural
film thicknesses
of thefrom
eight116.18
prepregs.
to tensile
properties,
interleaved
film increased.
Vf decreased,
it istobecause
load as
to break
increased
according
to
flexural strength
increasedAlthough
slightly from
116.18 MPa
120.58 MPa
thickness
of interleaved
film
aincreased.
decrease Although
of Vc and an
of itthickness.
Inload
caseto
ofbreak
flexural
modulus,
it decreased
greatly from
V f increase
decreased,
is because
increased
according
to a decrease
of V c
9.58
GPa
to 8.14ofGPa
as thickness
interleaved
film increased.
It greatly
is because,
stiffness
and an
increase
thickness.
In case of
of flexural
modulus,
it decreased
fromas
9.58
GPa to declined
8.14 GPa
from
a decrease
of Vf, displacement
increased
more than
to break
in the
load-displacement
as thickness
of interleaved
film increased.
It is because,
as load
stiffness
declined
from
a decrease of V f ,
curve.
Above increased
an interleaved
film load
thickness
of 80
m,load-displacement
the decrease range
of flexural
modulus
was
displacement
more than
to break
in the
curve.
Above an
interleaved
small
because
V
f
hardly
changes
here.
Thus,
a
slight
increase
of
flexural
strength
and
a
large
decrease
film thickness of 80 m, the decrease range of flexural modulus was small because V f hardly changes
of
flexural
show that
the fracture
toughness
of the
composite
increased
fromshow
insertion
of
here.
Thus,modulus
a slight increase
of flexural
strength
and a large
decrease
of flexural
modulus
that the
interleaved
film [2426].
fracture toughness
of the composite increased from insertion of interleaved film [2426].

Figure
Figure 5. Flexural
Flexural strength
strength and
and flexural
flexural modulus
modulus of
of the laminated
laminated composites
composites at
at various
various interleaved
interleaved
film
film thicknesses.
thicknesses.

3.5.
3.5. Interlaminar
Interlaminar Shear
Shear Strength
Strength
Figure
laminated composites
Figure 66 shows
shows the
the ILSS
ILSS of
of the
the laminated
composites for
for various
various interleaved
interleaved film
film thicknesses
thicknesses
between
each
of
the
eight
prepregs.
The
ILSS
also
showed
a
tendency
to
increase
as
thickness
between each of the eight prepregs. The ILSS also showed a tendency to increase as thickness of
of
interleaved
interleaved film
film increased.
increased. Compared
Compared to
to the
the laminated
laminated composite
composite without
without an
an interleaved
interleaved film,
film, the
the
ILSS
ILSS increased
increased from
from 8.32
8.32 GPa
GPa to
to 9.24
9.24 GPa
GPa when
when the
the interleaved
interleavedfilm
filmthickness
thicknessincreased
increasedto
to140
140m.
m.
The
reason
why
ILSS
increased
greatly
seems
to
be
that
resin
layer
between
carbon
fiber
The reason why ILSS increased greatly seems to be that resin layer between carbon fiber layers
layers
prevented
prevented delamination.
delamination.
Figure
Figure 77 shows
shows photographs
photographs of
of cross
cross sections
sections of
of the
the specimen
specimen after
after the
the ILSS
ILSS test.
test. As
As shown
shown in
in
Figure
7a,
in
case
of
the
composite
without
interleaved
film,
matrix
cracks
between
carbon
fibers
and
Figure 7a, in case of the composite without interleaved film, matrix cracks between carbon fibers
delamination
between
resinresin
layers
occur.
In contrast,
as as
shown
ininFigure
and delamination
between
layers
occur.
In contrast,
shown
Figure7b,
7b,only
onlymatrix
matrix cracks
cracks
between
carbon
fibers
could
be
observed
at
interleaved
film
thickness
of
120
m
[27].
between carbon fibers could be observed at interleaved film thickness of 120 m [27].

Materials 2016, 9, 344

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ILSS of the laminated composites at various interleaved film

film thicknesses.
thicknesses.
Figure 6.
6. ILSS
Figure
of the laminated composites at various interleaved film thicknesses.

Figure 7. Photographs of cross sections of delamination with (a) no interleaved film; and (b) 120 m
Figure 7. Photographs of cross sections of delamination with (a) no interleaved film; and (b) 120 m
Figure
7. Photographs
of cross
interleaved
film from ILSS
test.sections of delamination with (a) no interleaved film; and (b) 120 m
interleaved film from ILSS test.
interleaved film from ILSS test.

3.6. Drop Weight Impact Property

3.6. Drop Weight Impact Property
3.6. Drop Weight Impact Property
Figure 8 shows the impact load-time diagrams of the impact test of the laminated composites
Figure 8 shows the impact load-time diagrams of the impact test of the laminated composites
Figure 8interleaved
shows the impact
load-time diagrams
of the
impact
test of
laminated
for various
film thicknesses.
The impact
load
tended
to the
increase
fromcomposites
4932.07 Nfor
to
for various interleaved film thicknesses. The impact load tended to increase from 4932.07 N to
various
film thicknesses.
The impact
to increase
from 4932.07
to laminated
5690.85 N
5690.85 interleaved
N as interleaved
film thickness
rose toload
120 tended
m during
the forming
processN of
5690.85 N as interleaved film thickness rose to 120 m during the forming process of laminated
as
interleaved
thickness
rose
to 120 m
during
the forming
process ofbylaminated
composites.
composites.
Atfilm
interleaved
film
thickness
of 40
m, impact
load increased
12% to 5525.14
N but
composites. At interleaved film thickness of 40 m, impact load increased by 12% to 5525.14 N but
At
interleaved
film
thicknessabove
of 40 the
m,thickness.
impact load
increased
12% to difference
5525.14 N in
but
there load
was
there
was no big
difference
Thus,
there is by
a distinct
impact
there was no big difference above the thickness. Thus, there is a distinct difference in impact load
no
big difference
above the
thickness.
Thus,
there is adifferences
distinct difference
impact
between
between
non-interleaved
and
interleaved.
However,
resultinginfrom
theload
thickness
of
between non-interleaved and interleaved. However, differences resulting from the thickness of
non-interleaved
and
interleaved.
However,
differences
resulting
from
the
thickness
of
interleaved
interleaved film could not be identified. This is because, by insertion of interleaved film, existence of
interleaved film could not be identified. This is because, by insertion of interleaved film, existence of
film
could
notimproved
be identified.
This
is because,
of interleaved
film, existenceinoffracture
a resin
a resin
layer
impact
resistance
of by
theinsertion
composite.
Therefore, improvement
a resin layer improved impact resistance of the composite. Therefore, improvement in fracture
toughness was shown.
toughness was shown.

Materials 2016, 9, 344

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layer improved impact resistance of the composite. Therefore, improvement in fracture toughness
Materials 2016, 9, 344
8 of 12
was shown.
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8 of 12

Figure 8. Impact load-time diagrams from the impact test of the laminated composites at various

Figure 8. Impact load-time diagrams from the impact test of the laminated composites at various
interleaved film thicknesses.
interleaved film thicknesses.
Figure 8. Impact load-time diagrams from the impact test of the laminated composites at various
Figure 9film
shows
the energy-time curves from the impact test for various interleaved film
interleaved
thicknesses.

thicknesses.
every
curve of specimen
shows,
energytest
begins
to decrease
after the maximum
Figure
9 showsAsthe
energy-time
curves from
thethe
impact
for various
interleaved
film thicknesses.
energy
(E
0). This suggests that thermoplastic composite had not been destroyed completely but
9 shows
the shows,
energy-time
curves from
thetoimpact
testafter
for various
interleaved
film (E ).
As every Figure
curve of
specimen
the energy
begins
decrease
the maximum
energy
0
absorbed the
impact
of
low energy,
and the
gap between
E0 and
Ea is the
elastic
energy
(Ethe
e), in which
thicknesses.
As
every
curve
of
specimen
shows,
the
energy
begins
to
decrease
after
maximum
This suggests
that
thermoplastic
composite
had
not
been
destroyed
completely
but
absorbed
the
the laminated
from deformation
or vibration
restored completely
again to thebut
energy
(E0). Thiscomposite
suggests absorbed
that thermoplastic
composite
had not and
beenwas
destroyed
impact of
low energy,
and the
between
E0 and slightly
Ea is the
elastic
energy
(Ee ), in which
the laminated
impactor
after impact.
In gap
addition,
Ea decreased
with
increasing
interleaved
film thickness
absorbed the impact of low energy, and the gap between E0 and Ea is the elastic energy (Ee), in which
but
the
decrease
was
not
large.
composite
absorbed from deformation or vibration and was restored again to the impactor after impact.
the laminated composite absorbed from deformation or vibration and was restored again to the
In addition,
slightly
with
increasingslightly
interleaved
film thickness
but film
the decrease
a decreased
impactorEafter
impact. In
addition,
Ea decreased
with increasing
interleaved
thickness was
not large.
but the decrease was not large.

Figure 9. Energy-time curves of the laminated composites at various interleaved film thicknesses.

Figure 10 shows optical images and C-Scan images of the back of the specimen after the impact
test. The laminated composites were destroyed in different ways according to whether or not there
9. Energy-time
curvesAs
of the
laminated
composites
various
film thicknesses.
wasFigure
an9.interleaved
film
layer.
shown
in C-Scan
images,atat
in
case ofinterleaved
no interleaved
film,
damage
Figure
Energy-time
curves
of the
laminated
composites
various
interleaved
film
thicknesses.
area (blue area) of the specimen was observed in a large area and cracks that appeared from the
Figure
10 shows
optical
images
C-Scan with
images
of the back
the specimen
afterobserved
the impact
impact
were
propagated
to the
edge.and
However,
interleaved
filmofinside,
damage was

Figure
10laminated
shows optical
images
and
C-Scan in
images
of the
back
of the specimen
impact
test. The
composites
were
destroyed
different
ways
according
to whether after
or notthe
there
was laminated
an interleaved
film layer.were
As shown
in C-Scan
images, in
caseaccording
of no interleaved
film, damage
test. The
composites
destroyed
in different
ways
to whether
or not there
area
(blue area)film
of the
specimen
was in
observed
a largein
area
and
that appeared
the area
was an
interleaved
layer.
As shown
C-Scaninimages,
case
of cracks
no interleaved
film, from
damage
impact
were
propagated
to
the
edge.
However,
with
interleaved
film
inside,
damage
was
observed
(blue area) of the specimen was observed in a large area and cracks that appeared from the impact

Materials 2016, 9, 344

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over
apropagated
smaller
area.
It Itimplies
that
film
the
impact
strength
thecomposite
composite
over
a smaller
area.
impliesHowever,
thatinterleaved
interleaved
film improved
improved
impact
strength
ofof
the
were
to the
edge.
with interleaved
filmthe
inside,
damage
was
observed
over a
[2830].
[2830].
smaller
area. It implies that interleaved film improved the impact strength of the composite [2830].

Figure 10. Optical images and C-Scan images of the back of the specimen after the impact test; (a) no
Figure 10. Optical images and C-Scan images of the back of the specimen after the impact test; (a) no
interleaved
film; images
(b) 60 m
interleaved
film. of the back of the specimen after the impact test; (a) no
Figure
10. Optical
and
C-Scan images
interleaved film; (b) 60 m interleaved film.
interleaved film; (b) 60 m interleaved film.

Figure 11 shows cross section images of the specimen after the impact test. Side damage by the
Figure
11large
shows
cross
section
images of
of
the
specimen
after
the
test.
Side
damage by
by
the
impact
was
in cross
case of
no interleaved
film
11a)after
but small
with inserted
interleaved
filmthe
Figure
11
shows
section
images
the(Figure
specimen
the impact
impact
test. Side
damage
impact
was
large
in
case
of
no
interleaved
film
(Figure
11a)
but
small
with
inserted
interleaved
film
(Figure
11b).
However,
delamination
could
not
be
observed
in
both
cases.
It
is
because,
for
woven
impact was large in case of no interleaved film (Figure 11a) but small with inserted interleaved film
laminate,
initiated fromcould
the center
of observed
the impactin
directions
of
(Figure
11b).delamination
However, delamination
delamination
could
not be
be
observed
inpropagated
both cases.
Itthe
is slope
because,
for woven
woven
(Figure
11b).
However,
not
both
cases.toIt
is
because,
for
warp
and
fill
fibers
[31].
laminate,
delamination
initiated
from
the
center
of
the
impact
propagated
to
the
slope
directions
of
laminate, delamination initiated from the center of the impact propagated to the slope directions of
warp
and
fill
fibers
[31].
warp and fill fibers [31].

Figure 11. Cross section images of the specimen after the impact test; (a) no interleaved film;
(b) 60 m interleaved film.

Figure 11. Cross section images of the specimen after the impact test; (a) no interleaved film;
Figure 11. Cross section images of the specimen after the impact test; (a) no interleaved film; (b) 60 m
(b) 60 m interleaved film.
interleaved film.

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10 of 12

3.7. SEM Analysis

3.7. SEM Analysis
Figure 12 shows SEM images of cross sections of laminated composites for various interleaved
12 shows
SEMeach
images
of cross
of laminated
for resin
various
interleaved
film Figure
thicknesses
between
of the
eightsections
prepregs.
As shown composites
in Figure 12a,
layer
between
film
thicknesses
between
each
of
the
eight
prepregs.
As
shown
in
Figure
12a,
resin
layer
between
carbon fiber layers could not be observed when no interleaved film was inserted. If there is no resin
carbon
fibercould
layersnot
could
be observed
was inserted.
If there
nostress
resin
layer, load
be not
transferred
fromwhen
fiber no
to interleaved
fiber so thatfilm
delamination
occurs
dueis to
layer,
load
could
not
be
transferred
from
fiber
to
fiber
so
that
delamination
occurs
due
to
stress
concentration of resin layer. Also, voids remaining within the composite were observed since there
concentration
of resin
voids remaining
composite
were formed
observedbetween
since there
was
was no squeezed
outlayer.
resin.Also,
As shown
in Figure within
12bd,the
resin
layers were
carbon
no
squeezed
outinterleaved
resin. As shown
Figurethicker.
12bd, resin
layers
formed
carbon
fiber layers
fiber
layers as
film in
became
These
resinwere
layers
seembetween
to prevent
delamination
as
interleaved
film
became
thicker.
These
resin
layers
seem
to
prevent
delamination
which
improved
which improved fracture toughness. Also, an increase in squeezed out resin caused a decrease
in
fracture
toughness.
Also,
an
increase
in
squeezed
out
resin
caused
a
decrease
in
void
content.
void content.

Figure 12. SEM images of cross sections of the laminated composites at various interleaved film
Figure 12. SEM images of cross sections of the laminated composites at various interleaved film
thickness; (a) no interleaved film; (b) 40 m interleaved film; (c) 80 m interleaved film; (d) 120 m
thickness; (a) no interleaved film; (b) 40 m interleaved film; (c) 80 m interleaved film; (d) 120 m
interleaved film.
interleaved film.

4. Conclusions
4. Conclusions
To manufacture laminated composite with high impregnation using a thermoplastic prepreg,
To manufacture laminated composite with high impregnation using a thermoplastic prepreg,
PP film, which is same as the PP resin of the matrix material, was inserted as an interleaved film
PP film, which is same as the PP resin of the matrix material, was inserted as an interleaved film
between each of the eight prepregs during the forming process. The mechanical properties of the
between each of the eight prepregs during the forming process. The mechanical properties of
laminated composite produced with different thicknesses of the interleaved film showed the
the laminated composite produced with different thicknesses of the interleaved film showed the
following conclusions.
following conclusions.
1. When the interleaved film thickness was increased up to 140 m, as the amount of squeezed out
1.
When the interleaved film thickness was increased up to 140 m, as the amount of squeezed
surplus resin increased, the thickness of the composite specimen increased by 13.35% from 3.52
out surplus resin increased, the thickness of the composite specimen increased
by 13.35%
3. In addition,
mm to 3.99 mm. The density decreased by 2.04% from 1.32 g/cm3 to 1.29 g/cm
from 3.52 mm to 3.99 mm. The density decreased by 2.04% from 1.32 g/cm3 to 1.29 g/cm3 .
there was an 11.78% decrease in the fiber volume fraction from 55.01% to 48.52% and a 51.45%
In addition, there was an 11.78% decrease in the fiber volume fraction from 55.01% to 48.52% and
decrease in void content from 2.48% to 1.20%.
a 51.45% decrease in void content from 2.48% to 1.20%.
2. Tensile strength decreased by 8.75% from 796.82 MPa to 727.04 MPa, flexural strength slightly
2.
Tensile strength decreased by 8.75% from 796.82 MPa to 727.04 MPa, flexural strength slightly
increased by 3.79% from 116.15 MPa to 120.58 MP and flexural modulus decreased greatly by
increased by 3.79% from 116.15 MPa to 120.58 MP and flexural modulus decreased greatly by
10.03% from 9.58 GPa to 8.62 GPa. ILSS increased by 11.06% from 8.32 MPa to 9.24 MPa. Impact
10.03% from 9.58 GPa to 8.62 GPa. ILSS increased by 11.06% from 8.32 MPa to 9.24 MPa. Impact
load increased by 15.38% from 4932.07 N to 5690.85 N.
load increased by 15.38% from 4932.07 N to 5690.85 N.

Materials 2016, 9, 344

3.

11 of 12

In the case of the composite with inserted interleaved film, V f decreases and then tensile strength,
tensile modulus and flexural modulus decreased so that stiffness declined. However, fracture
toughness improved due to an increase in ILSS and impact properties.

Acknowledgments: This study was supported by the Global Excellent Technology Innovation (10044758) funded
by the Ministry of Trade, Industry and Energy (MOTIE) of Korea. Also, 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/).