Study on Mechanical Properties of Unidirectional

Continuous Carbon Fiber-Reinforced PEEK Composites

Fabricated by the Wrapped Yarn Method

Zhiping Xu ,1 Mei Zhang,1 ShuoHui Gao,2 Guibin Wang,1 Shuling Zhang,1 Jiashuang Luan 1
1
Key Laboratory of High Performance Plastics, Ministry of Education, National & Local Joint Engineering
Laboratory for Synthesis Technology of High Performance Polymer, College of Chemistry, Jilin University,
Changchun 130012, P.R. China

2
China-Japan Union Hospital of Jilin University, Changchun Shi, Jilin Sheng, Changchun 130033, P.R. China

The purpose of this study was to investigate the
mechanical properties of unidirectional continuous car-
bon fiber-reinforced PEEK (CCF/PEEK) composites via
the wrapped yarn method and to obtain optimum fabri-
cation conditions. The composite plates were fabri-
cated at different processing conditions and their
mechanical properties (i.e., tensile, bending and short
beam shear strength performance) were investigated
in terms of thermal and fracture morphology character-
izations. As the molding temperature and molding time
increased, the mechanical properties of the compo-
sites enhanced due to the improved impregnation of
the fibers, although there was potential matrix degra-
dation. Moreover, slow cooling rate had little effect on
the mechanical properties of the composites. There-
fore, to obtain a combination of excellent mechanical
properties and high production efficiency, a relatively
high molding temperature, sufficient molding time and
moderate cooling rate were optimal for the CCF/PEEK
fabricated by the wrapped yarn method. POLYM. COM-
POS., 00:000–000, 2017. V C 2017 Society of Plastics
Engineers
INTRODUCTION
With the development of the aeronautics industry, the
demand for the larger aircraft (Airbus A380 and Boeing
747) has grown gradually, since larger aircraft are safer
and more comfortable [1]. To create larger aircraft, more
fiber-reinforced polymer composites are used for
Correspondence to: J. Luan; e-mail: luanjs@jlu.edu.cn
Contract grant sponsor: Jilin Science and Technology Development Plan
Program of China; contract grant numbers: 20150204001GX and
20160204001GX; contract grant sponsor: Key Project of Science and
Technology Development Plan, Jilin Province of China; contract grant
number: 20170204042GX.
DOI 10.1002/pc.24600
Published online in Wiley Online Library (wileyonlinelibrary.com).
C 2017 Society of Plastics Engineers
V pressure [7]. In addition, the film stacking method is
lightweighting. Thermosetting composites have been used
for about 40 years in the aerospace industry because they
exhibit excellent mechanical properties. Thermoplastic
composites have some advantages over the thermosetting
composites in some aspects [1–3]: higher toughness, higher
service temperature, shorter manufacturing cycles, easier
storage, reprocessing recycling, etc. Thus, fiber-reinforced
thermoplastic composites will gain more attention by the
aviation industry. Airbus has already implemented thermo-
plastic composite structures in the A300–600 airplanes,
such as fixed wing leading edge (named J-nose) and flap
ribs [1], top deck floor and cargo compartment [4] and
engine nacelle [5].
Early thermoplastic composites were typically prepared
by short fiber-reinforced injection molding due to good
processing properties [6]. However, the mechanical prop-
erties of short fiber-reinforced composites are signifi-
cantly lower than long or continuous fiber-reinforced
composites. As a result, more attention has been paid to
the research of the continuous fiber reinforcement. The
main focus is how to make thermoplastic matrices
completely impregnate the reinforcing fibers and uni-
formly disperse the fibers. It is difficult for the thermo-
plastic matrices to be impregnated into the reinforcing
fibers due to high melt viscosity of the matrices. To solve
these difficulties, several methods for the fabrication of
continuous fiber-reinforced thermoplastic composites have
been developed such as [7]:
1. Film stacking method [8]
Layers of reinforcing fibers or fabrics are laid between
layers of thermoplastic polymer film, and then fused
under pressure for a period of time, cooled and solidified.
It is difficult to force a highly viscous thermoplastics melt
through micron sized gaps between fibers by applying

POLYMER COMPOSITES—2017
 based on flat films that are difficult to use for the fabrica-
tion of complex structures.
2. Melt impregnation method [9–12]
In the method, the dispersed fiber tow is impregnated
with the molten matrix. The most well-known hot melt
prepreg tape is prepared by this method, and its most rep-
resentative product is APC-2. Typically, for unidirectional
AS4/PEEK (60% by volume carbon fiber), its tensile
strength and modulus are about 2,100 MPa and 145 GPa
[13], flexural strength and modulus are about 1,800 MPa
and 127 GPa, short beam shear strength is about 105 MPa
[7]. The prepreg tape is so rigid that it is difficult to pre-
pare complex structural composites through weaving,
although it can easily get a good interfacial bonding
strength due to excellent matrix wettability.
3. Powder impregnating method [14–20]
Impregnating the reinforcing fiber bundles or fabrics
with a matrix powder as a precursor and applying heat to
melt the matrix and wet the fiber with the matrix. The
problem with this kind of method lies in achieving a fine FIG. 1. The schematic diagram of the three hybrid yarns.
dispersion of the matrix powders with the filler. As a pre-
condition, this requires fine matrix powders and uniform
dispersion of the tow. However, this method has also These methods have been widely used to fabricate
some defects, such as matrix powders being easily dis- continuous fiber-reinforced thermoplastic composites
lodged from the reinforcing filaments [21], unless a heat- with improved matrix impregnation. It should be noted
resistant adhesive sticks the matrix powders to the fiber that the hybrid yarns method is gaining attention
surface, but adhesives can also influence the performance
because of its application in textile composites. Textile
of composite materials.
4. Co-woven method [22–24]
composites are more easily processed in terms of perfor-
The matrix fiber yarn and the reinforcing fiber yarn are mance and shape. However, in fact, most of the research
woven into a fabric form in which the warp of the fabric work on textile composites is based on the commingled
contains the reinforcing fiber yarn and the weft contains yarns and rarely uses co-wrapped yarns. CF/PEEK com-
the matrix fiber yarn [16]. Due to the drapability of the posites are well known as a candidate for high perfor-
fabric, a composite with a complex structure can be pre- mance composites. Many researchers have investigated
pared by this method. However, because there are many the relationship between the processing, structure and
resin-rich areas inside the composite, the properties of the properties of the CF/PEEK composites based on com-
composites are usually poor.
mingled yarns, but there is little research on the co-
5. Hybrid yarns method [25–34]
The reinforcing fibers and the matrix fibers are intimately wrapped yarns method. It should be noted that the rein-
combined in different ways to form hybrid yarns, including forcing fibers will be damaged during the manufacturing
commingled yarns, co-wrapped yarns and core-spun yarns. of the commingled yarns. While the wrapped yarn
Commingled yarns are usually achieved by intimate mixing method does not provide good fiber distribution, it is
of fibers in a nozzle by means of pressurized air [3]. possible to improve the impregnation of the matrix by
Although the commingling process is easy to provide a uni- adjusting the processing conditions. Therefore, the per-
form distribution, it can damage the reinforcing fiber fila- formance of CF/PEEK composites fabricated by the co-
ments due to the enforced transverse loads. In wrapped
wrapped yarns method is expected to be better than that
yarns, the thermoplastic matrix fibers are wrapped over the
of the commingled yarns method. It is necessary to
reinforcing fibers. Compared to the commingled yarns, co-
wrapped yarns can better protect the reinforcing fibers dur- study the relationship between the processing, structure
ing manufacturing and further processing such as weaving and properties of the CF/PEEK composites fabricated by
or braiding. However, the distribution of the reinforcing the co-wrapped yarns method.
fibers and the matrix fibers is still not very good. Thus, this The purpose of this study is to look for optimum fabri-
process typically requires a higher processing temperature cation conditions of continuous carbon fiber-reinforced
and pressure to improve impregnation. Moreover, in the PEEK (CCF/PEEK) composites based on the co-wrapped
core-spun yarns, the short thermoplastic fiber yarns are yarns method. Unidirectional CCF/PEEK composites with
spun around the core reinforcing fiber yarns. The perfor-
different molding temperatures, different molding times
mance of core-spun yarns is equivalent to that of co-
and different cooling rates were prepared by hot press
wrapped yarns. Core spinning usually requires a very high
twist to create the necessary cohesion between the sheath molding. Their tensile properties, bending properties and
and the core, which reduces the production speed can dam- short beam shear strength were investigated. The test
age the reinforcing fibers [35]. The schematic diagram of results have been further characterized thermal and frac-
the three hybrid yarns are shown in Fig. 1. ture morphology.

2 POLYMER COMPOSITES—2017 DOI 10.1002/pc

 Jilin University Super Engineering Plastics Research Co.
China and used for melt spinning. The details of melt
spinning were previously reported [36]. The fabricated
PEEK fibers had a linear density of 18 and 23 tex, and
the average diameter of the monofilament was 23 lm and
36 filaments in number. The schematic diagram of the
spinning machine is shown in Fig. 2.

FIG. 2. Schematic diagram of the melt spinning machine.
FABRICATION
Melt Spinning of PEEK
Fiber grade PEEK particles (MI 5 22 g/10 min;
Tg 5 1458C; Tm 5 3378C, were supplied by Changchun
Co-Wrapped Yarns
Co-wrapped yarns were fabricated by laboratory-
assembled equipment, and the diagram is shown in Fig.
3. The device consists of three parts: the doubling device
(Fig. 3a), the spooling device (Fig. 3b) and the co-
wrapping device (Fig. 3c). To fabricate co-wrapped yarns
the required linear density of the PEEK yarns was
obtained by the doubling process. To prepare a co-
wrapped yarn with a carbon fiber mass fraction of 60%,
the line density of the PEEK yarns was 133 tex. Then,
during the spooling process, the PEEK yarns were

FIG. 3. Schematic diagram of a self-assembly device for preparing co-wrapped yarns: (a) doubling device;
(b) spooling device; (c) co-wrapping device. [Color figure can be viewed at wileyonlinelibrary.com]

DOI 10.1002/pc POLYMER COMPOSITES—2017 3

 co-wrapped yarns are shown in Fig. 4a and b, respec-
tively. In this paper, the co-wrapped yarns (333 tex, 60
wt% carbon fiber) consisted of carbon fiber (HF20, no
sizing agent, monofilament diameter 5 7 lm, 198 tex,
3,000 filaments, tensile strength  4,000 MPa, tensile
modulus is 221–242 GPa: Jiangsu Hengshen Co., Ltd,
China) and PEEK yarns (yarn size 5 133 tex, 216 fila-
ments: Laboratory made).

Unidirectional Laminated CCF/PEEK Composite Plates

FIG. 4. The co-wrapped yarn: (a) a photograph of co-wrapped yarn
and (b) a structure diagram of co-wrapped yarn.
wrapped on a specific hollow cylindrical surface with a
line speed of 500 m/min. Finally, in the co-wrapping pro-
cess, the carbon fiber and the PEEK yarns passed
through the hollow cylinder by a drawing roller at a con-
stant rate. At the same time, the hollow cylinder rotated
counterclockwise, so that the PEEK yarns were wrapped
on the carbon fiber to obtain the co-wrapped yarns that
were then wound on a paper tube. The twist of the co-
wrapped yarn was 220 and the output speed was
11.36 m/min. A photograph and schematic diagram of
The wrapped yarns were used to fabricate unidirec-
tional laminated CCF/PEEK composite plates by hot
press molding. As shown in Fig. 5a, the co-wrapped
yarn was first wound unidirectionally around a stainless-
steel plate at specific tension. The plate was then heated
to 3608C under vacuum and cooled to room temperature
without pressure to obtain a prepreg material. The pre-
preg (Fig. 5b) was cut into a plate with 150 mm 3
150 mm dimensions and then placed in a mold of similar
geometry and placed on the platform of a hot press
machine (Model: P 400P V, COLLIN, Germany) to fab-
ricate composite plates as shown in Fig. 5c. Figure 6
shows the molding process of unidirectional CCF/PEEK
composite plates. The temperature was first increased
from 308C to the molding temperature (i.e., 370, 400,

FIG. 5. (a) Unidirectional co-wrapped yarns with a size of 150 mm 3 150 mm; (b) unidirectional prepregs
with a size of 150 mm 3 150 mm; (c) schematic of tool assembly as used for fabrication of composite
plates. [Color figure can be viewed at wileyonlinelibrary.com]

4 POLYMER COMPOSITES—2017 DOI 10.1002/pc


FIG. 6. Molding process of unidirectional CCF/PEEK composite
plates.
415, 430 and 4508C) at a heating rate of about 158C/min
without applying any pressure. When the temperature
reached the set molding temperature, a degassing step
was started, its detailed steps are as follows: the pressure
down first to 0, and then quickly up to 4MPa, and finally
repeat the process 3 times, each time 10 s. At the desired
molding temperature pressure was gradually applied at a
rate of 0.1 bar/s. When the pressure reached 4 MPa, the
mold was held at the molding temperature for a length
of time (i.e., 10, 30, 60, 90 and 120 min) and cooled and
consolidated at a specific cooling rate (i.e., 22, 210 and
2208C/min). The photograph of fabricated unidirectional
CCF/PEEK composite plate is shown in Fig. 7. The
average carbon fiber volume fraction of the fabricated
composite plates was about 52%, as obtained by the
burning method, this specific step was to stay at 5508C
for 5 h.
FIG. 7. A photograph of fabricated unidirectional CCF/PEEK compos-
ite plate with a size of 150 mm 3 150 mm.
DOI 10.1002/pc
FIG. 8. Schematic drawing of a tensile specimen of unidirectional
CCF/PEEK composite plates. [Color figure can be viewed at wileyonli-
nelibrary.com]
CHARACTERIZATION
Thermogravimetric Analysis (TGA)
To investigate the effect of processing conditions on
the thermal behavior of the PEEK matrix, the composite
plates, the unprocessed PEEK fibers, and specimens of
the composites fabricated under different processing con-
ditions were used. The thermal behavior of the PEEK
matrix of composite plates was studied by thermogravi-
metric analysis (TGA Model: Pyris 1 TGA, PE Co., Ltd,
Waltham, MA). The sample was first held at 1008C for
15 min, and then heated to 8008C at a heating rate of
108C/min, under nitrogen. The amount of each test sam-
ple was about 10 mg.
Tensile Test
Tensile testing of the fabricated unidirectional CCF/
PEEK composite plates were performed on an electronic
universal testing machine (Model: Instron 5982, INS-
TRON Co.) with a cross-head speed of 2.0 mm/min. The
test standard referenced ASTM-D3039. For each type of
composite plate, at least 5 specimens were tested, until
the ultimate strength was reached. The dimensions of the
specimen for tensile testing are shown in Fig. 8. The
length of the tensile test specimen was 150 mm, the width
was 12.5 mm and the thickness was 1.50 6 0. 055 mm. A
reinforcing sheet, 35 mm long, 12.5 mm wide and 2 mm
thick was attached to both ends of each specimen to pro-
tect the specimen. An infrared camera extensometer was
used to measure the strain during testing. Tensile strength
rt and tensile modulus Et were calculated according to
the following Eqs. 1 and 2:
Pb
rt 5 (1)
b3h
DP3l
E t5 (2)
b3h3Dl
where:
rt 5 ultimate tensile strength, MPa
Et 5 tensile modulus, GPa
Pb 5 maximum force before failure, N
b 5 the width of the specimen, 12.5 mm
h 5 the thickness of the specimen, 1.45 6 0. 075 mm
DP 5 load increment of initial straight line on Load–
Strain Curve
POLYMER COMPOSITES—2017 5

FIG. 9. Schematic drawing of a bending specimen of unidirectional
CCF/PEEK composite plates. [Color figure can be viewed at wileyonli-
nelibrary.com]
l 5 gauge length of optical extensometer, mm
Three Point Bending
Three point bending of the fabricated unidirectional
CCF/PEEK composite plates were performed on an elec-
tronic universal testing machine (Model: AG-I 20KN,
SHIMADZU Co., Japan) with a cross-head speed of
1.0 mm/min. The test standard referenced ASTM-D7264.
The dimensions of the specimen for three point bending
test are shown in Fig. 9. The length of the bending test
specimen was 75 mm, the width was 12.5 mm, the thick-
ness was 2 6 0.053 mm and the span to depth ratio was
fixed at 32:1. The measured bending strength and modu-
lus were averaged from at least 5 samples. Bending
strength rb and bending modulus Eb were calculated
according to the following Eqs. 3 and 4:
3Pb L
rb 5
2bh2
Dr
Eb 5
DE
where:
rb 5 ultimate bending stress, MPa
Eb 5 bending modulus, GPa
Pb 5 maximum force before failure, N
L 5 the span of the sample, 64 mm
b 5 the width of the sample, 12.5 mm
h 5 the thickness of the sample, 2 6 0.053 mm
Dr5 difference in bending stress between the two
selected strain points, MPa
DE5 difference between the two selected strain points
Short Beam Shear Test
Short beam shear testing of unidirectional CCF/PEEK
composite plates were performed on an electronic univer-
sal testing machine (Model: AG-I 20KN, SHIMADZU
Co., Japan) with a cross-head speed of 1.0 mm/min. The
test standard referenced ASTM-D2344. The dimensions
of the specimen for short beam shear test are shown in
Fig. 10. The length of the bending test specimen was
20 mm, the width was 10 mm, the thickness was 2 6
0.053 mm and the span to depth ratio is controlled at 5:1.
6 POLYMER COMPOSITES—2017
The measured short beam shear strength is the average of
at least 7 samples. Short beam shear strength Fsbs was
calculated according to the following Eq. 5:
Pm
Fsbs 50:753 (5)
b3h
where:
Fsbs 5 short beam shear strength, MPa
Pm 5 maximum load, N
b 5 the width of the sample, 10 mm
h 5 the thickness of the sample, 2 6 0.053 mm
Microstructure Analysis
The fracture aspect of unidirectional CCF/PEEK com-
posites was first sputtered with a thin layer of platinum and
was then used to observe the microstructure morphology
by field emission scanning electron microscopy (FESEM)
(Nova NanoSEM 450: FEI Co., the Netherlands).
RESULTS
Thermogravimetric Analysis
Figure 11 shows the TGA curves of the composites fab-
ricated at different processing conditions. Unprocessed
PEEK fibers and the composite fabricated at 4008C for 10
min hold time and 108C/min cooling rate had a 5% weight
loss temperature of 5628C. When the molding temperature
increased to 4308C and hold time and cooling rate were
(3)
constant, the curve of thermal degradation began to shift to
the left and the 5% weight loss temperature dropped to
5558C. This means that the matrix had begun to undergo
(4)
thermal degradation. Continued increase in the molding
temperature to 4508C resulted in the 5% weight loss tem-
perature decreased rapidly to 5438C. This is due to severe
degradation of the PEEK matrix. When molding tempera-
ture remained at 4308C and the cooling rate remained con-
stant, a hold time increased to 90 min resulted in the 5%
weight loss temperature shifting down to 5588C, from
5628C, indicating a slightly loss in thermal stability of the
composite. Since severe degradation of the matrix
occurred, the 5% weight loss temperature dropped to 5358C
after the hold time was increased to 120 min. However, in
FIG. 10. Schematic drawing of a short beam shear specimen of unidi-
rectional CCF/PEEK composite plates. [Color figure can be viewed at
wileyonlinelibrary.com]
DOI 10.1002/pc

FIG. 11. TGA curves of the PEEK matrix for the composites fabri-
cated at different processing conditions. [Color figure can be viewed at
wileyonlinelibrary.com]
the case where the molding temperature and the holding
time were constant, when the cooling rate was reduced to
28C/min, changes in the TGA curve were not significant,
and the 5% weight loss temperature slightly dropped to
5608C. This indicates that the cooling rate had little effect
on the thermal stability of the composites. Figure 12 shows
a picture of the composite plate fabricated at different proc-
essing conditions. It can be seen that the surface quality of
the composite plates fabricated at two different cooling
rates were very good and the color of the matrix was nor-
mal. However, when the molding temperature was 4508C
and the holding time was 120 min severe degradation of
the matrix was observed via roughness of the composite
surface and a darkening of color.
Tensile Performance
Figure 13 shows the tensile stress–strain curves of
composite plates fabricated at different molding
FIG. 12. Photographs of the composite plates fabricated at different
processing conditions.
DOI 10.1002/pc
FIG. 13. Tensile stress–strain curves of unidirectional CCF/PEEK com-
posite plates fabricated at 370, 400, 415, 430 and 4508C with the same
holding time of 10 min and the same cooling rate of 2108C/min. [Color
figure can be viewed at wileyonlinelibrary.com]
temperatures. It can be seen that as the molding tempera-
ture increased, the stress at break increased until the
molding temperature increased to 4158C where the tensile
stress at break reached the maximum value and continued
increases to the molding temperature decreased the stress
at break. In particular, when the molding temperature was
increased to 4508C, the fracture stress was drastically
reduced. Figure 14 shows the relationship between the
tensile modulus of the composite and the molding temper-
ature, which were consistent with the change of tensile
stress at break. The tensile modulus increased first and
then decreased with the increase in the molding tempera-
ture, and the tensile modulus was also the highest at a
molding temperature of 4158C.
Figure 15 shows the tensile stress–strain curves of
composite plates fabricated at different holding times. It
can be seen that the stress at break increased with the
FIG. 14. Relationship between tensile modulus and molding tempera-
ture of unidirectional CCF/PEEK composite plates. [Color figure can be
viewed at wileyonlinelibrary.com]
POLYMER COMPOSITES—2017 7
FIG. 15. Tensile stress–strain curves of unidirectional CCF/PEEK com-
posite plates fabricated at 10, 30, 60, 90 and 120 min with the same
molding temperature of 4008C and the same cooling rate of 2108C/min.
[Color figure can be viewed at wileyonlinelibrary.com]
increase in the holding time until the holding time
increased to 90 min, after which the tensile fracture stress
reached the maximum value. Continued increases in hold-
ing time to 120 min resulted in decreases in stress at
break. Figure 16 shows the relationship between the ten-
sile modulus of the composite and the holding time. With
the increase in the holding time, the tensile modulus
increased until the holding time increased to 60 min
where the tensile modulus reached the maximum value.
Further increases to holding time above 60 min resulted
in a loss of tensile modulus.
Figure 17 shows the tensile stress–strain curves of
composite plates fabricated at different cooling rates. It
can be seen that the tensile fracture stress decreased as
the cooling rate increased. When the cooling rate was
28C/min, the stress at break was about 1,440 MPa and
when the cooling rate increased to 208C/min, the stress at
break was about 1,360 MPa—a decrease in 5.5%. Figure
FIG. 16. Relationship between tensile modulus and holding time of
unidirectional CCF/PEEK composite plates. [Color figure can be viewed
at wileyonlinelibrary.com]
8 POLYMER COMPOSITES—2017
FIG. 17. Tensile stress–strain curves of unidirectional CCF/PEEK com-
posite plates fabricated at 22, 210 and 2208C/min with the same mold-
ing temperature of 4008C and the same holding time of 10 min. [Color
figure can be viewed at wileyonlinelibrary.com]
18 shows the relationship between the tensile modulus of
the composites with the cooling rate. As the cooling rate
increased, the tensile modulus decreased. When the cool-
ing rate was 28C/min, the tensile modulus was about 157
GPa, and when the cooling rate increased to 208C/min,
the tensile modulus was about 151 GPa—a decrease in
only 3.8%.
Bending Performance
Figure 19 shows the bending stress–displacement
curves of composite plates fabricated at different molding
temperatures. It can be seen that the bending stress line-
arly decreased as the displacement increases until break
occurred and the bending stress dropped rapidly to zero.
The bending fracture stress increased as the molding tem-
perature increased, and the bending fracture stress reached
a maximum of about 1,900 MPa until the molding
FIG. 18. Relationship between tensile modulus and cooling rate of uni-
directional CCF/PEEK composite plates. [Color figure can be viewed at
wileyonlinelibrary.com]
DOI 10.1002/pc
FIG. 19. Bending stress–displacement curves of unidirectional CCF/ FIG. 21. Bending stress–displacement curves of unidirectional CCF/
PEEK composite plates fabricated at 370, 400, 430 and 4508C with the PEEK composite plates fabricated at 10, 30, 60, 90 and 120 min with
same holding time of 10 min and the same cooling rate of 2108C/min. the same molding temperature of 4008C and the same cooling rate of
[Color figure can be viewed at wileyonlinelibrary.com] 2108C/min. [Color figure can be viewed at wileyonlinelibrary.com]

temperature increased to 4158C. Increased molding tem-

perature resulted in a fracture stress decline. In particular,
begun to decrease. When the holding time increased to
when the molding temperature was increased to 4508C,
120 min, the bending fracture stress was significantly
the bending fracture stress decreased to about 1,300 MPa.
reduced. Figure 22 shows the relationship between the
Figure 20 shows the relationship between the bending
bending modulus of the composites as a function of hold-
modulus of the composites with the molding temperature.
ing time. It can be seen that when the holding time was
The bending modulus and the bending fracture stress
less than 60 min, the bending modulus increased with the
were the same as the change of molding temperature. As
increase in the molding time. However, after increasing
the molding temperature increased, the bending modulus
the molding time to 90 min, the bending modulus began
increased first and then decreased, and at 4158C, the
to decrease.
bending modulus reached a maximum of about 149 GPa.
Figure 23 shows the bending stress–displacement
Figure 21 shows the bending stress–displacement
curves of the composite plates fabricated at different cool-
curves of the composite plates fabricated at different
ing rates. It can be seen that the bending stress–displace-
holding times. It can be seen that the bending fracture
ment curves of the composites fabricated at three
stress increased with the increase in the holding time
different cooling rates were almost coincident. Although
when it is less than 60 min. However, after the holding
the bending fracture stress decreased with the increase in
time increased to 90 min, the bending fracture stress had
the cooling rate, there is no obvious change. The bending

FIG. 20. Relationship between bending modulus and molding tempera-

ture of unidirectional CCF/PEEK composite plates. [Color figure can be FIG. 22. Relationship between bending modulus and holding time of
viewed at wileyonlinelibrary.com] unidirectional CCF/PEEK composite plates. [Color figure can be viewed
at wileyonlinelibrary.com]

DOI 10.1002/pc POLYMER COMPOSITES—2017 9

FIG. 23. Bending stress–displacement curves of unidirectional CCF/
PEEK composite plates fabricated at 22, 210 and 2208C/min with the
same molding temperature of 4008C and the same holding time of 10
min. [Color figure can be viewed at wileyonlinelibrary.com]
fracture stress of the composites fabricated at the three
different cooling rates was around 1,800 MPa. Figure 24
shows the relationship between the bending modulus of
the composites with the cooling rates. It can be seen that
with an increase in the cooling rate, the bending modulus
decreased from 145GPa at 228C/min to 139GPa at
2208C/min—a decrease in only 4.1%.
Short Beam Shear Strength
Figure 25 shows the short beam shear strength of the
composite plates fabricated at different molding tempera-
tures. Increasing the molding temperature resulted in an
increase in short beam shear strength increased with a
maximum value of about 72 MPa until the molding tem-
perature increased to 4158C. Molding temperatures above
4158C resulted in decreased short beam shear strengths.
FIG. 24. Relationship between bending modulus and cooling rate of
unidirectional CCF/PEEK composite plates. [Color figure can be viewed
at wileyonlinelibrary.com]
10 POLYMER COMPOSITES—2017
FIG. 25. Relationship between shear strength and molding temperature
of unidirectional CCF/PEEK composite plates. [Color figure can be
viewed at wileyonlinelibrary.com]
Figure 26 shows the short beam shear strength of the
composite plates fabricated at different holding times.
The short beam shear strength increased to 74 MPa at 60
min. Longer holding times resulted in decreased short
beam shear strengths such as 56 MPa at 120 min. Figure
27 shows the short beam shear strength of the composite
plates fabricated at different cooling rates. When the cool-
ing rate was 28C/min, the short beam shear strength of
the composite was about 72.1 MPa, and the cooling rate
increased to 208C/min, the short beam shear strength
decreased to 64.1 MPa—a decrease in 11.1%.
Fracture Morphology
Figure 28 shows the fracture morphology of the compo-
sites fabricated at three different molding temperatures. As
can be seen from Fig. 28a, when the molding temperature
FIG. 26. Relationship between shear strength and holding time of uni-
directional CCF/PEEK composite plates. [Color figure can be viewed at
wileyonlinelibrary.com]
DOI 10.1002/pc

FIG. 27. Relationship between shear strength and cooling rate of unidi-
rectional CCF/PEEK composite plates. [Color figure can be viewed at
wileyonlinelibrary.com]
was 3708C only a small amount of the PEEK resin pene-
trated into the carbon fibers due to the high viscosity of the
PEEK matrix. The impregnation of PEEK was poor and a
mass of carbon fibers were exposed, but when the molding
temperature rose to 4158C, the impregnation was improved
and the exposed carbon fiber disappeared and the PEEK
matrix exhibited ductile behavior (see Fig. 28b). However,
when the molding temperature rose to 4508C, the PEEK
FIG. 28. Fracture morphology of unidirectional CCF/PEEK composite plates fabricated at different molding
temperatures: (a) 3708C, 10 min, 2108C/min; (b) 4158C, 10 min, 2108C/min; (c) 4508C, 10 min, 2108C/
min. [Color figure can be viewed at wileyonlinelibrary.com]
DOI 10.1002/pc
matrix exhibited a brittle behavior (see Fig. 28c), which
may be due to thermal degradation of the matrix.
Figure 29 shows the fracture morphology of the com-
posites fabricated at three different holding times. As can
be seen from Fig. 29a, when the holding time was 10
min, the impregnation was remarkably improved as com-
pared with Fig. 28a due to the higher molding tempera-
ture, but there were still some exposed carbon fibers.
When the holding time was increased to 60 min, the
impregnation was further improved and the PEEK matrix
exhibited ductile behavior (see Fig. 29b). However, when
the molding time was increased to 120 min, the PEEK
matrix exhibited a brittle behavior (see Fig. 29c).
Figure 30 shows the fracture morphology of the com-
posites fabricated at two different cooling rates, which
resulted in no significant difference in the impregnation
of the carbon fibers in the composites fabricated at two
different cooling rates. Figure 30a when compared with
Fig. 30b shows that the matrix of the composites exhib-
ited a more distinct ductile behavior. This may result in a
decrease in the crystallinity of the matrix due to an
increase in the cooling rate.
DISCUSSION
As shown in Figs. 13, 14, 19, 20 and 25, when the
molding time was 10 min and the molding temperature
was 3708C, the tensile properties, the bending properties
POLYMER COMPOSITES—2017 11
 FIG. 29. Fracture morphology of unidirectional CCF/PEEK composite plates fabricated at different holding
times: (a) 4008C, 10 min, 2108C/min; (b) 4008C, 60 min, 2108C/min; (c) 4008C, 120 min, 2108C/min.
[Color figure can be viewed at wileyonlinelibrary.com]
and the shore beam shear strength of the composites were
poor due bad impregnation of the carbon fibers (see Fig.
28a). As the molding temperature increased, the viscosity
of the PEEK matrix decreased and more PEEK matrix
penetrated into the carbon fibers (see Fig. 28b). Better
impregnation resulted in better mechanical properties of
the composites. However, when the temperature rose to
4308C, the mechanical properties of the composites
started to decline. This is because the matrix had started
to degrade as seen in the TGA data (see Fig. 11), which
resulted in development of defects within the composites.
Defects can cause stress concentration under the loads
and a reduction of mechanical properties. At the tempera-
ture of 4508C premature destruction of the composite
occurred due to the severe degradation of the matrix (see
Fig. 12), which lead to a reduction in mechanical
properties.
When the molding temperature was 4008C, as shown
in Figs. 15, 16, 21, 22 and 26 with increased molding
time the mechanical properties of the composites were
increased due to the improved impregnation (see Fig. 29a
and b). When the molding time was extended to 90 min
the bending performance and the short beam shear
strength of the composites began to decline. The decline
in mechanical properties was due to the degradation of
the matrix as exhibited by TGA data (see Fig. 11). While
the tensile strength still increased, it indicated that the
bending load-related properties were more sensitive to the
degradation of the matrix than the tensile load-related
12 POLYMER COMPOSITES—2017
properties. When the molding time was increased to 120
min at 4008C serious degradation of the matrix at the sur-
face of the composites had taken place as defects (see
Fig. 12), which led to a sharp decrease in the mechanical
properties of the composites.
However when the molding temperature and the mold-
ing time were constant and cooling rates were varied
from 28C/min to 208C/min, the tensile strength and modu-
lus decreased by 5.5% and 3.8%. Also, bending strength
and modulus were only decreased by 3.0% and 4.1%,
respectively. Shear strength of short beams decreased by
11.1% as cooling rate varied from 28C/min to 208C/min.
The slight decrease in mechanical properties may be due
to a decrease in the crystallinity of the matrix. It is well
known that cooling rate influences the crystallinity of the
matrix, but this change is not obvious due to the small
range of cooling rates tested in the present study. It is
also known that the cooling rate has little effect on the
impregnation of the fibers (see Fig. 30). Thus, when the
cooling rate varied by small amounts there was little
influence on the mechanical properties of the composite.
The above results have shown that a higher molding
temperature and a longer molding time are required to
obtain the composites with excellent mechanical proper-
ties based on the co-wrapped yarn technique. The effect
of a small cooling rate changes on the mechanical proper-
ties of the composites is not significant, although the
mechanical properties of the composites decrease slightly
as the cooling rate increases. Therefore, to ensure
DOI 10.1002/pc
 FIG. 30. Fracture morphology of unidirectional CCF/PEEK composite plates fabricated at different cooling
rates: (a) 4008C, 10 min, 228C/min; (b) 4008C, 10 min, 2208C/min.
production efficiency, a relatively high cooling rate is
more suitable. It must be noted that high molding temper-
ature and excessive hold times will lead to degradation of
the matrix and influence the mechanical properties of the
composites. Hence, the 400–4158C molding temperature,
the 60 min holding time and the 2108C/min cooling rate
are recommended for the fabrication of CF/PEEK compo-
sites using the co-wrapped yarn processing method.
CONCLUSIONS
In the literature many researchers have investigated the
effects of processing conditions on the mechanical proper-
ties of CF/PEEK composites. However, it must be noted
that almost all of the research work focused on compo-
sites fabricated from the prepreg process or the com-
mingled yarns method. However, since the reinforcing
fibers have been dispersed before processing, the fabrica-
tion conditions of prepreg and commingled yarn compo-
sites cannot be compared to composites fabricated by the
co-wrapped yarns method.
In this study, the co-wrapped yarns method was
applied to the fabrication CF/PEEK composites. To find
the optimum processing conditions, the unidirectional
CCF/PEEK composite plates were fabricated under differ-
ent molding temperatures; different holding times and dif-
ferent cooling rates were studied. The mechanical
properties of the composites increase with the increasing
of molding temperatures and hold times. However, after
increasing molding temperature and molding time to
4308C and 90 min, respectively, the mechanical properties
of the composites began to decrease due to the degrada-
tion of the matrix. Moreover, the slow cooling rate has
little effect on the mechanical properties of the compo-
sites. Hence, the 400–4158C molding temperature, the 60
min hold time and the 2108C/min cooling rate are recom-
mended for the fabrication of CF/PEEK composites.
Under these conditions, the composite plates exhibited
excellent mechanical properties (i.e., 4008C–60 min–
2108C/min: Tensile strength 5 1,510 MPa, Tensile mod-
ulus 5 161 GPa; Bending strength 5 1,900 MPa, Bending
DOI 10.1002/pc
modulus 5 152 GPa; Short beam shear strength 5 75
MPa). It can be considered that the co-wrapped yarns
method can be used for the development of continuous
carbon fiber-reinforced PEEK matrix composites.
ACKNOWLEDGMENT
The authors are grateful for the financial support from
Jilin Science and Technology Development Plan Program
of China (20150204001GX) and (20160204001GX), Key
Project of Science and Technology Development Plan,
Jilin Province of China (20170204042GX).
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DOI 10.1002/pc