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Injection Molded Short Glass and Carbon Fibers Reinforced Polycarbonate

Hybrid Composites: Effects of Fiber Loading

Article  in  Journal of Reinforced Plastics and Composites · September 2010

DOI: 10.1177/0731684409358282

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 Injection Molded Short Glass and Carbon
Fibers Reinforced Polycarbonate Hybrid
Composites: Effects of Fiber Loading

Y. J. PHUA AND Z. A. MOHD ISHAK*

School of Materials and Mineral Resources Engineering
Engineering Campus, Universiti Sains Malaysia, Seri Ampangan 14300 Nibong
Tebal, Penang, Malaysia

R. SENAWI
Polyloy Engineering Plastics Sdn. Bhd, Simpang Empat, 14100 Penang, Malaysia

ABSTRACT: Hybrid composites of polycarbonate (PC) reinforced with short glass fibers (GF) and
short carbon fibers (CF) were prepared by twin-screw extrusion and injection molding techniques.
Composites were produced in different ratios of GF and CF by maintaining the total fiber loading
at 40 wt%. The mechanical properties such as tensile, flexural strength, and impact of these compo-
sites were investigated. It was noted that an increase in GF content led to a higher strength of
the hybrid composites as compared to CF. Morphological analysis by using scanning electron
microscope reveals that CF had poor fiber—matrix interactions with PC, which brought about the
decrement of stress-transfer efficiency. A poor fiber—matrix interaction is believed to be the main
cause of the lower strength enhancement by CF than expected. Heat deflection temperatures of
composites increased with the increment of GF content. From dynamic mechanical thermal analysis,
high-storage modulus is observed at the temperature below Tg. Meanwhile, it was observed that
surface and volume electrical resistivity decreased by increasing the CF content owing to its
conductivity.

KEY WORDS: polycarbonate, carbon fiber, glass fiber, hybrid composites.

INTRODUCTION

YBRID COMPOSITE IS defined as a composite material in which two or more rein-

H forcements are incorporated into the matrix [1]. Through this approach, it is possible
to combine the advantages of different fibers while simultaneously mitigating their less
desirable properties. Normally, one of the fibers is a high strength, high modulus fiber such
as carbon, and the second fiber usually is a low modulus and less expensive fiber such as
E-glass. Hybrid composites are becoming more popular because the composite properties
can be tailor made to requirement.

*Author to whom correspondence should be addressed. E-mail: zarifin@eng.usm.my

Journal of REINFORCED PLASTICS AND COMPOSITES, Vol. 29, No. 17/2010 2592
0731-6844/10/17 2592—12 $10.00/0 DOI: 10.1177/0731684409358282
ß The Author(s), 2010. Reprints and permissions:
http://www.sagepub.co.uk/journalsPermissions.nav
Injection Molded GF and CF Reinforced PC Composites 2593

In this study, hybrid composites of polycarbonate (PC) reinforced with short glass and
carbon fibers have been produced. Carbon fibers (CF) are widely used as reinforcements
for polymeric matrices in various applications due to their high modulus and
strength, accompanied with the excellent electrical and thermal properties. However,
their high cost, poor toughness, and processability had restricted their usage in some of
the applications [1—4]. Certain fraction of CF can be replaced by glass fibers (GF) in
producing the composites in order to maintain the strength and modulus of the compo-
sites, and yet provide adequate electrical conductivity to the composites, which are rele-
vant in electrical applications. Thus, the study presented here was prompted by the balance
between the cost, processability, and properties of the short GF and CF reinforced PC
hybrid composites. There are various types of hybrid composite. The one produced in this
study is an intimately mixed hybrid, where the constituent fibers are made to mix as
randomly as possible so that no overconcentration of any one type is present in the
material [1].
PC is a particular group of amorphous thermoplastic polymers with glass transition
temperature (Tg) of 145 C. Their interesting features such as high toughness, good thermal
properties, excellent dimensional stability, and good optical properties, position them
between commodity and engineering plastics. The major problem in handling PC is its
low hydrolytic stability. The drying process of PC resin is extremely crucial before pro-
ceeding to any other processes in order to avoid void formation, which is detrimental to
the mechanical properties of final products [4,5].
Generally, mechanical properties such as strength and modulus can be enhanced by
incorporating GF and CF. The additional function of CF is to provide electrical conduc-
tivity to the PC matrix [1,4]. Thus, the major function of CF in this hybrid composite is to
provide electrical conductivity, whilst the responsibility of increasing the mechanical prop-
erties lies on GF, which has a lower price.
Electrical conductivity of a composite is directly proportional to the concentration of
CF in that particular composite [2,4]. High CF loading leads to a higher conductivity.
Critical concentration of CF, which enables a polymer composite to convert from an
insulator to a conductor, is known as ‘percolation threshold’ [2]. A continuous network
of CF formed along the polymer matrix allows the charge carriers to move throughout the
polymer matrix. The electrical conductivity in CF is achieved through the transition of
electrons from one CF to the other, by over-crossing the gap between fibers [2—4].
However, if the CF content is too low in a composite, continuous network could not
be formed and restricted the electrical charges to flow in the composite. In this research,
the electrical properties of composites are characterized by using surface and volume
resistivity tests.

EXPERIMENTAL

Materials

PanliteÕ L-1225L PC resin was produced by Teijin Kasei America, Inc., USA. Chopped
CF K223Y1 used in this study was supplied by Mitsubishi Chemical Corp, Japan. The
diameter of the filament is 13 mm and the length of fibers is 6 mm. E-glass chopped strand
ECS-13-4.5 was supplied from Shenzhen Yataida High-Tech. Co., Ltd, China with diam-
eter of 13 mm and 4.5 mm length.
2594 Y.J. PHUA ET AL.

Preparation of Composites

GF/CF reinforced PC hybrid composites were prepared by using twin-screw extruder

(Sino PSM30). PC was fed through the main feeder while fibers were placed in the side
feeder. Before processing, PC resin was dried for at least 4 h at 120 C in a vacuum oven.
The extrusion process was carried out at compounding temperatures ranging from 260 C
to 280 C. After that, extrudates were pelletized by using a pelletizer. The pellets were
then injection molded into standard tensile bars and flexural specimens with Sumitomo
injection molding machine. The injection temperature was fixed at 275 C. Table 1 shows
the formulation of composites produced in this study. The total fiber content was main-
tained at 40 wt%.

Characterizations

MECHANICAL PROPERTIES
Tensile test was carried out at ambient temperature with an Instron-5582 machine,
according to ASTM D638 (Type I) at a crosshead speed of 5 mm/min. Flexural measure-
ments were performed on the same Instron machine according to ASTM D790 using
three-point bending configuration with a support span length of 50 mm and a crosshead
speed of 1 mm/min. Charpy impact tests were carried out at room temperature as referred
in ASTM D6110-04 for both notched and unnotched samples. The tests were conducted by
using Zwick Pendulum Impact Tester (USA) with striker energy of 7.5 J. Five specimens of
each compound were tested.

FRACTOGRAPHY STUDIES
The fracture surface of selected PC composites was examined in a scanning electron
microscope (FESEM) Zeiss Supra 35VP LEO machine. Prior to the SEM observations,
the fracture surface was sputter-coated with a thin layer of gold to avoid electrical charging
during examination.

FIBER LENGTH DISTRIBUTION

Chemical digestion test was used to determine the fiber length distribution in the com-
posites. A small piece of molded composite sample was dissolved in chloroform and fil-
tered. The residue was then dispersed in glycerol. A drop of mixture was dripped on a glass
plate and observed under Rax Vision Optical Microscope to determine the fiber length
distribution. One hundred counts were carried out in each determination.

Table 1. Formulation of compound.

PC (wt%) GF (wt%) CF (wt%)

100 — —
60 40 —
60 — 40
60 20 20
60 25 15
60 30 10
Injection Molded GF and CF Reinforced PC Composites 2595

ELECTRICAL PROPERTIES
Electrical conductivity characterization was determined by the surface resistivity of the
composites, which was carried out by using VoyagerÕ surface resistivity meter. Surface
resistivity ranged from 104 to 105 X/m2 indicating that the sample is electrically conductive.
Surface resistivity of 106—1011 X/m2 indicates that the material is antistatic, while material
with surface resistivity higher than 1012 X/m2 indicates that it is an insulator. Volume
resistivity test was performed by using Advantest R8340 ultrahigh resistance meter with
a voltage of 0.5 V.

HEAT DEFLECTION TEMPERATURE

Heat deflection temperature (HDT) test was performed under ASTM D648 by using
Ray-Ran HDT-Vicat Softening Point Tester (model RRHDV4). In the HDT test,
1.82 MPa load was subjected edgewise to the specimens with span length of 100 mm and
ramp rate of 120 C/h.

DYNAMIC MECHANICAL THERMAL ANALYSIS

Dynamic mechanical thermal analysis (DMTA) was performed using Mettler Toledo
DMTA Analyzer Model MA861e. DMTA spectra were taken in a three-point bending
mode, in temperature ranging from room temperature to 200 C under nitrogen atmo-
sphere at a heating rate of 5 C/min and frequency of 10 Hz.

RESULTS AND DISCUSSION

Electrical Properties

Electrical properties of pure PC and its composites are shown in Table 2. Pure PC and
composites added with 40 wt% GF are insulators, meaning that PC and GF are not
electrically conductive. For composites containing CF, both surface resistivity and
volume resistivity decrease dramatically when the CF loading is increased in the compo-
sites. This shows that CF is able to provide electrical conductivity to the composites and
the conductivity increased with its loading. Volume resistivity was found to be higher than
surface resistivity. This means that the current flows better through the body of the mate-
rial, rather than along the surface of the material. CF can form a continuous network,
which allows the current to pass through.

Table 2. Resistivity of PC and its composites.

Fiber content (wt%)

Surface Volume
GF CF resistivity (X/m2) resistivity (X cm)

— — 1012 1011
40 — 1012 1011
— 40 1.280  104 4.39  103
20 20 4.004  105 3.53  104
25 15 4.443  105 9.00  104
30 10 1.3  106 2.89  106
2596 Y.J. PHUA ET AL.

Critical concentration of CF to convert from an insulator to a conductor is known as

‘percolation threshold’ [2]. This is often determined from the surface resistivity of the
material. From the results shown in Table 1, the percolation threshold can be determined
at 15% CF. Below the percolation threshold, the amount of CF is insufficient to provide
conductivity to the material. To obtain a more accurate percolation threshold, reduction
of the gap of CF content between each formulation is advisable [6]. This will be the subject
of our future work.

Mechanical Properties

The dependence of tensile strength and tensile modulus on fiber content for composites
is shown in Figure 1. It can be seen that tensile strength of PC increased dramatically with
the incorporation of GF and/or CF. This provides a clear indication of the reinforcing
effect imparted by GF and CF to the composites.
For a single-fiber system, the tensile strength of PC reinforced with 40 wt% GF was found
to be slightly higher than 40 wt% CF composite. A similar trend was also observed from
hybrid composites, i.e., tensile strength is increased by increasing GF content. In general,
CF should be able to provide a better reinforcing effect to the composites as compared to
GF [2]. This rather unexpected trend may be attributed to relatively poor fiber—matrix
interfacial adhesion between CF and PC as revealed by the SEM micrographs shown in
Figures 2 and 3. It can be seen that CF has a poor interaction with the PC matrix as
compared to GF. A low interfacial shear strength value of about 10 MPa has been reported
for PC/CF system [7]. This was attributed to a weak physical interaction and mechanical
interlocking at the fiber—matrix interface. Carneiro and Maia [8] reported that the poor
adhesion between CF and PC had caused slipping between fibers and matrix and conse-
quently diminished the reinforcing ability of the fibers. In the present study, it can be seen
that the surfaces of the pulled-out CF are smooth and not covered with any matrix (e.g.,
Figure 3). In addition, holes observed on the fracture plane indicate the occurrence of
interior fiber pull-out. Contrarily, the pulled-out GF are well coated and wetted by PC
matrix. The good interfacial bonding will facilitate the stress transfer from polymer
matrix to fibers [8,9]. Generally, fibers will be pulled out when the fiber length is shorter
than the critical fiber length, lc, which is determined through the following equation [9]:
rf fu
lc ¼ ð1Þ

where rf is the fiber radius, rfu is the fiber strength, and  is the interfacial shear stress.

120 8.0
Tensile modulus (GPa)
Tensile strength (MPa)

100
6.0
80
60 4.0
40
2.0
20
0 0.0
Pure 0:40 20:20 25:15 30:10 40:0
PC
GF:CF ratio (wt%)

Figure 1. Tensile strength and tensile modulus of pure PC and PC reinforced fiber composites.
Injection Molded GF and CF Reinforced PC Composites 2597

Figure 2. SEM micrograph of fracture surface of PC reinforced 40 wt% GF. (Arrowed: the pulled-out GF are
well coated with matrix).

Figure 3. SEM micrograph of fracture surface of PC reinforced 40 wt% CF. (Arrowed: the pulled-out CF have
smooth surface).

Moreover, as observed, the surface of PC matrix in PC/GF composites is relatively

rougher compared to PC/CF composite.
Figure 4 shows the SEM micrographs of PC reinforced 20 wt% CF and 20 wt% GF. GF
and CF could not be differentiated easily since both of them are of the same diameter.
However, based on the observation from single-fiber system (Figures 2 and 3), it can be
ascertained that the pulled-out fibers, which were well coated with matrix, are of GF,
whilst the pulled-out fibers, which had smooth surface, are of CF.
2598 Y.J. PHUA ET AL.

Figure 4. SEM micrograph of fracture surface of PC reinforced 20 wt% CF and 20 wt% GF.

Table 3. Mean fiber length of fibers in composites.

Fiber length (mm) Fiber aspect ratio

Composite GF CF GF CF

PC + 40 wt% GF 0.36 — 27.7 —

PC + 40 wt% CF — 0.21 — 16.2
PC + 20 wt% GF + 20 wt% CF 0.23 0.22 17.7 16.9
PC + 25 wt% GF + 15 wt% CF 0.26 0.22 20.0 16.9
PC + 30 wt% GF + 10 wt% CF 0.29 0.26 22.3 20.0

Apart from fiber—matrix interfacial bonding, another possible factor that may influence
the tensile strength of PC composites is the fiber aspect ratio. Both GF and CF used in this
research are of the same diameter, so that the aspect ratio of fibers is directly dependent on
the fiber length. The effects of glass and carbon fiber loading on mean CF and GF lengths
are presented in Table 3. It can be seen that the mean fiber length of both GF and CF
decreased with the increase of CF content in the composites. Prior to extrusion compound-
ing, the initial length of CF is longer than GF. After processing, the mean fiber length of CF
became shorter than that of GF. This may be due to the fact that CF are more brittle and
thus fracture much easily than GF during processing [9,10]. Besides that, it is noted that the
mean CF and GF lengths increased with the increment of GF content, whilst they decreased
with the increment of CF content in the hybrid composites. This indicates that the interac-
tion between GF and CF (GF—CF interaction) leads to more damage to GF than the
GF—GF interaction; whilst the GF—CF interaction bring about less damage to the CF
than CF—CF interaction [9,11]. Shorter fiber lengths will create more fiber ends, which
eventually act as stress concentration points where failure often occurs at these sites. This
possibly explains the reduction of tensile strength with increasing CF content in the hybrid
PC composites. The extent of damage of both GF and CF could be reduced by using a
single-screw extruder instead of a twin-screw extruder used in the present study. This will be
the subject of our future research.
Injection Molded GF and CF Reinforced PC Composites 2599

Figure 1 reveals the effect of fiber loading on the tensile modulus of PC. Upon incor-
poration of fibers, tensile modulus increased significantly. As expected, for the single-fiber
composite system, CF gives higher modulus compared to GF. In the case of the hybrid
composites, a gradual drop in the tensile modulus was observed as the CF was replaced by
GF [9,11,12].
Figure 5 shows the effect of fiber loading on the flexural strength and modulus of PC
and its composites. With the incorporation of fibers, flexural strength increased, showing a
similar trend as observed in tensile strength (Figure 1). The flexural strength increased
gradually as more amounts of CF were replaced by the GF. As mentioned earlier, this may
be attributed to the better fiber—matrix interactions between GF and PC as compared to
CF and PC. The relatively better interfacial bonding in the former allows a more efficient
stress transfer at the interfacial region, which consequently leads to higher strength of the
resulting composites [2]. As expected, flexural modulus of PC increased dramatically upon
the incorporation of fibers [11—13].
Charpy impact strengths of notched and unnotched specimens are presented in Figure 6.
Charpy impact strengths of unnotched and notched pure PC are 85.37 kJ/m2
and 102.51 kJ/m2, respectively. Impact strength of pure PC is much higher than that

200 20

Flexural modulus (GPa)

Flexural strength (MPa)

150 15

100 10

50 5

0 0
Pure 0:40 20:20 25:15 40:10 40:0
PC
GF:CF ratio (wt%)

Figure 5. Flexural strength and modulus of pure PC and PC reinforced fiber composites.
Charpy impact strength (KJ/m2)

35
30
25
20
15
10
5
0
0:40 20:20 25:15 30:10 40:0
GF:CF ratio (wt%)
Notched Unnotched

Figure 6. Charpy impact strength of PC reinforced GF and CF.

2600 Y.J. PHUA ET AL.

of its composites. High impact properties of PC are contributed by the carbonate groups
that exist in its structure, by giving high flexibility to the material [5].
From Figure 6 it can be seen that the incorporation of GF and/or CF has resulted in a
dramatic reduction in the impact strength of PC. The presence of stiff GF and CF in PC
had increased the stiffness of the composites, which consequently brought about lowering
of toughness, and thus reduced the impact strengths.
It can be seen that impact strength increases with increasing GF content in the PC/GF/
CF hybrid composites. This can be attributed to the nature of GF, which is relatively
ductile compared to CF [11]. As expected, the introduction of notches into the specimens
leads to a further drop in the impact strength values. Notched impact strength revealed the
energy required to propagate an existing crack in a sample, whilst unnotched impact
strength represented the energy required to initiate and propagate a crack [10].
Examination of fracture surfaces using SEM has revealed that the main energy dissipative
processes in both single-fiber and hybrid PC composites are the fiber pull-out. Similar
features of failure mechanism have been observed by other workers for other short fiber
reinforced thermoplastic composites [13].

Heat Deflection Temperature

Table 4 shows the effect of fiber incorporation on the HDT of PC. The presence of stiff
GF and CF in composites plays a vital role as a physical cross-link network, which could
limit the thermal movement of the polymer chain and prevent the elastic and plastic
deformation of the polymeric matrices [14]. It is interesting to note that in the case of a
single-fiber system, GF is more effective in increasing the thermal stability of PC.
Increasing the content of GF has also enhanced the HDT of PC/GF/CF hybrid compo-
sites. The inferior performance of CF could be related to its poor interfacial bonding with
the PC matrix [11].

Dynamic Mechanical Thermal Analysis

Figure 7 shows the temperature dependences of storage modulus (E0 ) of PC with different
composition of CF and GF. It can be seen that E0 of PC increased with the incorporation of
both GF and CF below the glass transition temperature (Tg) of PC, i.e., at around 160 C.
This is in agreement with the trend observed in the flexural test as discussed earlier. As
expected, PC is an amorphous glassy polymer, above the Tg, E0 values of each sample
decrease drastically. The results also show that E0 value of CF is higher than that of GF.

Table 4. HDT and coefficient of linear thermal expansion (CLTE)

of PC and its composites.

Composite HDT ( C) CLTE (105  C1)

Pure PC 127.7 7.03

PC + 40 wt% GF 141.6 6.40
PC + 40 wt% CF 128.6 9.03
PC + 20 wt% GF + 20 wt% CF 132.2 6.71
PC + 25 wt% GF + 15 wt% CF 133.6 6.64
PC + 30 wt% GF + 10 wt% CF 136.3 6.02
Injection Molded GF and CF Reinforced PC Composites 2601

15,000

Storage modulus (MPa)

10,000

5000

0
20 40 60 80 100 120 140 160 180 200
Temperature (°C)

Pure PC PC+40 wt% GF

PC+40 wt% CF PC+30 wt% GF+10 wt%CF

Figure 7. Storage modulus of PC and its composites as a function of temperature.

1.5
Shifted tan δ

0.5

0
20 40 60 80 100 120 140 160 180 200
Temperature (°C)

Pure PC PC+40 wt% GF

PC+40 wt% CF PC+30 wt% GF+10 wt%CF

Figure 8. Tan  of PC and its composites as a function of temperature.

In Figure 8, the tan  peak temperature, which represents the Tg of the polymer, does
not show a distinct change after incorporation with fibers. However, the peak height of
fiber reinforced composites decreased due to the reduction of polymer matrix in the system
[15]. The results showed that the Tg is only influenced by the polymer matrix in a com-
posite system and will not be influenced by the incorporation of fibers. The tan  peak
becomes broader by incorporation of fibers into PC, which may be considered as a result
of reduction in the mobility of the polymer chain, which is restricted by fiber [16]. Table 5
reported the area of tan  peak for PC and its composites with different fiber loadings. The
tan  peak area is affected by the restriction of polymer chain movement that causes
immobilization of molecules [16]. The area sums the amount of such activity retained
by the resin after incorporation of fibers. The area of tan  peak decreases after PC
incorporation with GF and CF. The reduction of area is more significant for PC/
40 wt% CF composite as compared to PC/40 wt% GF composite, which suggests the
2602 Y.J. PHUA ET AL.

Table 5. Area of the tan d peak for PC and its composites.

Composite Area

Pure PC 13.89
PC + 40 wt% GF 10.07
PC + 40 wt% CF 6.63
PC + 20 wt% GF + 20 wt% CF 8.03

greater restriction of molecular chains by CF. The result of hybrid composites is the
intermediate between single-fiber composites.

CONCLUSIONS

In fiber reinforced composites, fiber—matrix interaction is important in determining the

properties of the particular composite. SEM micrographs of both 40 wt% GF composite
and 40 wt% CF composite displayed that GF bonded well with PC matrix, whilst CF had
poor interaction with the polymer matrix. Thus, CF does not function as expected in this
research by giving low tensile strength and flexural strength than GF. Strengths have been
reduced when CF content in the composite was increased. Moreover, mean fiber length
was found to be a possible reason affecting the mechanical properties of composites. Mean
fiber length was reduced with the increase of CF loading in composites. CF provides good
electrical conductivity to composites, and the conductivity increases with CF concentra-
tion in the composites. GF had provided higher HDT to the composites than CF. From
the DMTA study it was found that the incorporation of CF and/or GF significantly
increased the E0 below the Tg of the composites while Tg of the composites remain
unchanged. The reduction in the area of tan  peak with the addition of fibers is believed
to be the reason for immobilization of polymer chains.

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