Understanding the Thermoforming Issues of Carbon Fibre

Reinforced Polyphenylene Sulphide [PPS] Composite

Meng Hou 1* and Lm. Y e2

ICooperative Research Centre for Advanced Composite Structures Ltd
361 Milperra Road, Bankstown, NSW, 2200, Australia

2 School of Aerospace, Mechanical & Mechatronic Engineering

University of Sydney, NSW, 2006, Australia

ABSTRACT

This paper presents the recent research results in understanding the processing
parameters of rubber stamp forming of CFIPPS. Processing conditions such as mould
temperature, consolidation pressure and forming time were investigated to determine
their effect on the forming ofCP/PPS composites. The effect of forming conditions on
the spring-in phenomena, deconsolidation of CF/PPS and the morphological property
of PPS matrix were studied. CFIPPS composite quality was assessed using
micrographs of sectioned specimens and mechanical characterisation. The
temperature profile of CF/PPS during stamp forming was monitored and simulated
using finite element analysis.

INTRODUCTION

FIGURE 1: Thermoplastic component made of CFIPPS

Thermoplastic composites have a number of advantages over traditional

thermosetting composites in aeronautical application which could lead to cost
reduction. Rapid transformation of advanced thermoplastic composites into finished
parts is vital to the acceptance of these materials by industry. Thermoforming is one
such fabrication method. In order to develop an Australian capability for design and
production of cost-effective advanced thermoplastic composite aircraft structures, a
project of design and manufacturing of a demonstrator thermoplastic composite

• Correspondence author, Fax: +61 29772 8482, Email: m.hou@crc-acs.com.au

806 Carbon Fibre Reinforced Polyphenylene Sulphide Composite

component (Figure 1) was undertaken in a research program within the Cooperative

Research Centre for Advanced Composite Structures (CRC-ACS), which included
researchers from the University of Sydney and Hawker de Havilland. Rubber stamp
forming and thermal welding techniques were used to manufacturing the
demonstrator. This paper presents the recent research results in understanding the
effect of processing parameters of rubber stamp forming on the mechanical and
morphological properties of CF/PPS composite.

EXPERIMENTAL

Material

Cetex Carbon fabric [plain weave and 5H satin] reinforced PPS pre-consolidated
laminates and CF Fabric/PPS semipreg supplied by Ten Cate Advanced Composite,
The Netherlands, were used in the study. The pre-consolidated laminates had a
stacking sequence of [±45, 0/90, ±45, 0/90], and had a resin content of about 50% by
volume. The semipreg was made of 5H satin fabric sandwiched between two PPS
films. The fibres were not impregnated but only slightly fused to the PPS film, which
was quenched to an amorphous state to provide an improved drapability. Laminates
[0/90]8 with embedded thermocouples were made in-house using the semipreg. The
semipregs were placed between two aluminium platens and UPLEX films were
introduced between the composites and aluminium platens for easy de-moulding. The
materials were then consolidated in hot press and the moulding conditions were
adopted from Ref [1] .

Forming Facility

Rubber

Heated Metal Tool

Hot-plate
Preheating
Equipm ent

FIGURE 2: Forming facility

The experimental set up used in this study is shown in Figure 2. The hydraulic
press (TYSCY 5092) has two working strokes, i.e. opening/closing and compression
stroke and can build up a maximum load of 10 kN in opening/closing stroke and 500
kN in compression stroke, respectively; further, it allows opening and closing
velocities of 70 mmls and a compression stroke rate between 1 and 3 mmls,
respectively. The characteristic of the press is that it allows the mould to be rapidly
closed on the preheated laminate panel in the opening/closing stroke to a specific
pressure and then close more slowly in the compression stroke to build up high
pressure during forming and dwell to promote consolidation of material in the mould.
A specially designed die-set was installed in the press. Metal and rubber [rubber block
or rubber cavity] were fixed onto the die-set as the forming tools. The metal tool was
equipped with electric heating elements and could be heated up to 200°C. A hot plate
Carbon Fibre Reinforced Polyphenylene Sulphide Composite 807

was used to pre-heat the CFIPPS laminate. The typical forming procedure involves:
(a) heating the pre-consolidated laminate panel to a temperature above the melting
temperature of PPS matrix between two hot plates without any external pressure; (b)
quickly transferring the hot laminate panel into the forming system (transfer times are
of the order of a few seconds to prevent significant cooling); and (c) forming the hot
laminate panel into the final part, in which the press is so adjusted that a high closing
speed is used to close the mould in the opening/closing stroke, and when a specified
pressure was reached, the press was changed to its compression stroke, in which the
mould was closed slowly but a high pressure could be built up.

Characterisation

Characterisations of mechanical properties as a function of the processing

conditions were carried out using flexure (three-point bending) tests. The span was 48
mm; the width and length of the specimen were 25 mm and 60 mm, respectively. The
crosshead speed was set to 1.2 mmfmin. The flexure elastic modulus and flexure
strength were determined according to ASTM D-790. At least five specimens for each
processing condition were tested at ambient temperature. DSC and DMA were used to
investigate the morphological property and deconsolidation behaviour of PPS matrix,
respectively. In addition, reconsolidation and crystallite structure were examined
using light microscopy and polarized light microscopy.

RESULTS & DISCUSSION

Deconsolidation

The major problem encountered was the de-consolidation of the laminate

during heat-up. It was found that the degree of de-consolidation was dependent on the
structure of the reinforcement (Figure 3) and the optimum processing conditions had
to be adjusted accordingly. It was found that higher pressures; higher speed and
higher pre-heating temperature were needed to form 5H satin CFIPPS than plain
weave CFIPPS. As an example, Figure 4 shows the voids formed on the metal tool
surface (due to a quick cooling) could be eliminated by an applying high stamping
pressure.

100 200

Plain Fabric

FIGURE 3: Deconsolidation of CF fabriclPPS laminate

Spring-in

Due to high processing temperatures, the residual stresses in thermoplastic

composites are inevitable. The most common residual stress effect encountered in
manufacturing composites is a reduction in the enclosed angle in channel or angle
808 Carbon Fibre Reinforced Polyphenylene Sulphide Composite

components [2]. This reduction in enclosed angle is referred to as spring-in. The

spring-in phenomenon was investigated at an early stage of the project in order to
provide necessary information for tool design. Based on the experimental results an
allowance angle was set up in tooling system to compensate for part spring-in. Figure
5 shows the effect of different holding time on spring-in angle of 5 H satin CF/PPS. It
can be seen that the spring-in angle was a function of forming time and was
minimised to 0.5 degree when the holding time was 30s or more.

FIGURE 4: Re-consolidation of 5H satin CF/PPS

1.2
5H Satin CF/PPS

1.0

~ 0.8
il'
0

t
c
0.6

:[ 0.4

U) 0.2

10 20 30 40 50

Holding Time [s 1

FIGURE 5: Spring-in angle of 5H satin CFIPPS

Temperature Profile during Stamp Forming

The temperature profile of CF/PPS during forming was monitored using in-house
made laminates with embedded thermocouples, which were placed in different
locations as well as through the thickness of the laminate. Different temperatures have
been used for the metal tool, while the rubber side was kept at room temperature. It
was found that the metal tool had a predominate influence on the cooling of CFIPPS.
Because of the good insulation properties of rubber, the contact between the rubber
mould and the hot laminate does not lead to excessive cooling of the laminate. A 2D-
FEM heat transfer model was also generated to simulate the cooling-down
temperature profile (Figure 6). The temperature profiles provided valuable
information on the thermal history, degree of crystallinity and the morphological
property ofPPS matrix.
Carbon Fibre Reinforced Polyphenylene Sulphide Composite 809

350[ ........................................................•.................................................. I
11
r=~~~~~~.

300i\">!, I R"bbee025'C

I \.;J\~.: -~_~~_.~E. ~.'-p~e ;m~.~"'

2501-
1
~~~LI. .!: : r;dI~~i[~LI~~~-.L~il.
Metal Tool - 170 oc

'- / ' FEM I

200 ~~.,,¥.: I
150

100L-_ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _---l
o 20 40 60 80 100 120
Time [s]

FIGURE 6: Cooling-down temperature profile of CFIPPS laminates

Morphological Property of PPS

Experimental results showed that different tool temperatures result in different

cooling histories of PPS matrix and hence generated various degrees of crystallinity
[Figure 7]. The amount of crystals formed depended on the energy absorbed during
cooling. By cooling slowly (higher tool temperature) maximum crystallinisation
occurred.
Cooling rate:
IlHeK".6.Hen
ii.BOC/s 8.?OC/s
150.4 [J/g)

~ 25~-----+---r~~
j 20 1--------,---'--,----1

~
Hex.
5'
AsreceivedPPSFilm
15 e - - - - - - - . j 20.1 24.6

V;,"ngT.mp".tu,,, 1300C '0 f-------1

V
~ 10
~
ToolingT.mp.ratu,.: 170'C iii' 5 ,--,--'---- 1
o 6.3

As Received ToolT ToolT

Film 130°C 170°C

Temperature [OC 1

FIGURE 7: Different tool temperatures resulted in different degree of crystallinity of PPS matrix

The image of PPS crystal spherulite was investigated using polarised light
microscopy. Amorphous PPS film (obtained from the CFIPP semipreg) was stamp
formed under the same processing conditions as the CFIPPS laminates. Figure 8
shows the spherulitic structures formed by different tool temperatures. In general,
high tool temperatures resulted in slow cooling rates and large sizes of crystal
spherulite. To ensure optimal performance of PPS composites after processing,
maximum crystallinity is usually desired. However, larger crystals will cause
extensive resin volume shrinkage and can generate micro-cracks in the PPS
composite. For this reason, processing conditions need to be carefully controlled in
such a way that a high degree of crystallinity as well as small crystals can be obtained.

1901 'c I
- - - - - Tool Temperature --~ Size of Spherulite --------+~

Cooling Rate

FIGURE 8: PPS Crystal structures formed by different tool temperatures

810 Carbon Fibre Reinforced Polyphenylene Sulphide Composite

Mechanical Performance of Stamp Formed CF/PPS

Different from matched metal die forming, in rubber forming one of the rigid
metal dies was replaced with a flexible rubber block. The rigid metal die determined
the final shape of the component and gave a good surface quality on the contacting
side of the product, while the rubber produced a homogeneous pressure distribution.
Figure 9 shows the effect of forming pressure on the flexural properties of CFIPPS
laminates. It was found good quality of CF/PPS composites could be obtained in the
pressure range from 2 to 5 MPa and the rubber tool needed to be constrained within a
solid metal frame to prevent extensive deformation of the rubber. Large deformation
of the rubber would delay the time needed to build up the maximum pressure and
generate voids in the composite.

am
'"
a.
::2
800

7m
<f)
J:: :>
0, "S
c: "0
~
(J) 700
0
::2
1:':> 1:':>
6fJJ
u:" u:"
(l) (l)

800
2 4
Fanirg AtssLre [ M>a J

FIGURE 9: Flexural properties of formed CFIPPS laminate

CONCLUSIONS

The project has focused upon providing deep understanding of processing

conditions of rubber stamp forming of the CF/PPS composites. Processing conditions
such as mould temperature, consolidation pressure and forming time were
investigated to determine their effect on the forming, morphological, consolidation
and mechanical performance of carbon fibre reinforced PPS composites. Generic
aircraft rib components were manufactured to investigate the forming behaviour of the
material and to demonstrate the rubber stamp forming concept. A sound scientific
basis for understanding what happens during the processing and how that stage affects
the service performance of the structure has been established. The outcome of this
project will benefit the ongoing technology development program ofCRC-ACS.

REFERENCE

1. CETEX®- PPS Guide Lines, Ten Cate Advanced Composites, Nijverdal, The Netherlands. 2000
[ITD440 1. 0 1]
2. Jain, L. K., Hou, M., Ye, L. and Mai, Y. W., "Spring-in study of the aileron rib manufactured from
advanced thermoplastic composite", Composites Part A: Applied Science and Manufacturing, Vol.
29, issue 8, 1998, p. 973-979