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Sandwich Injection Moulding of Thermosetting Materials.

Part I: Initial Experiments

Sandwich Injection Moulding of Thermosetting


Materials. Part I: Initial Experiments
S. Kiatmanaroj, V. Goodship and G.F. Smith

Advanced Technology Centre, Warwick Manufacturing Group, University of Warwick,


Coventry, CV4 7JL, UK

Received: 16 September 2003 Accepted: 28 November 2003

ABSTRACT
Thermoset co-injection moulding is a novel technology that might be an
alternative for thermoset recycling. This paper describes some experiments on
the sandwich moulding of two polyesters, a powder coating and a BMC using
a new special design thermoset co-injection machine and manifold system. The
first thermoset sandwich moulding has been made and a number of initial
moulding problems are presented and discussed.

1. INTRODUCTION
Sandwich injection moulding technology is one of the multi-material injection
moulding processes. The machine is capable of producing two-material plastic
components by injecting the polymer melts from two separated barrels in a
suitable order. Generally, skin material is injected first and then followed by
core. Once the skin melt touches the mould wall, a frozen layer is formed,
which allows the core melt to flow through. Some more skin is injected again
to seal the moulding. By doing this, the skin will encapsulate the core
completely at the end of the process cycle. Hence, the moulding will appear
as if it is made of only one material. This technology is very successful in the
plastic market since a lower cost component can be made of a cheaper or
recycled material covered with a virgin one. A soft feel surface moulding
injected with a stronger core material or a smooth surface part with foam core
are also possible(1). Another interesting application is in-mould coating
plastic. By using a thermoplastic paint as skin, colour coated mouldings can
be produced without being sent to the paint line(2).

Since the technology was invented, many research papers have been published.
Most of them focussed on how to control the skin and core distribution and how
to get adequate interfacial adhesion between the skin and core layers by
looking at the effect of processing parameters such as viscosity ratio, injection
time and speed and the amount of compatibilisers(1,3-11). The simulation works

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used that information to predict the formation and shape of the sandwich
mouldings. It was successful for some simple geometry moulds, but not for the
more complicated ones(7,12-14).

As mentioned previously, the technology is very successful today, but is limited


to thermoplastics. However, the idea of sandwich injection moulding is also
possible for thermosets, even though it might be more difficult since controlling
temperature and cross-linking may be a problem. The use of recycled materials
as the sandwich’s core is very interesting in terms of thermoset recycling. Apart
from the two recycling methods that have already been used, which are (i)
mixing some regrind material with the pure polymer(15-17) and (ii) reusing the
glass fibre obtained by combustion of the polymer in a fluidised bed(18), we
now have the sandwich technique as a third choice. The technique has the
advantage that a greater percentage of recyclate can be used in the core without
leading to a strength problem, since there is almost no effect on impact strength
if the core content varies(19).

Another useful application of the sandwich technology is to coat a glass-filled


thermoset with a smooth material or paint. As with the thermoplastic case, a
coloured component can be made in one cycle without the need for a paint line.

At present, no research work has been done on injecting two thermoset


materials together. Hunold(20) presented the first conference paper on the
sandwich injection moulding of different types of material, thermoset and
thermoplastic, and thermoset and rubber. The first sandwich moulding was a
combination of a phenolic skin and a polyethylene core. Nevertheless, there
were some heat-related problems, which require more development using
improved compounds, mould and machine technology.

To co-injection mould thermosets, their temperature, curing rate and flow


properties are very important. This study presents a new manifold system
designed for the co-injection of thermoset materials and for overcoming the
problems experienced in making a thermoset sandwich moulding. The result
is analysed by considering the system and the materials properties.

2. EXPERIMENTAL

2.1 Machine and tooling


A Battenfeld thermoset co-injection moulding machine, BA2000/630+630BK
equipped with the UNILOG 9000C control system has been especially

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Sandwich Injection Moulding of Thermosetting Materials. Part I: Initial Experiments

designed and built for this project. It consists of a horizontal stuffer-feed


injection unit suitable for bulk moulding compounds and a vertical hopper-
feed injection unit for granular materials. Between the machine injection unit
and mould, a new manifold system (shown in Figure 1) has been installed to
work as a gate channel where the two injected polymers meet at the mould
sprue. PDE cartridge heaters and type-J thermocouples in both halves of the
manifold are used to control the operating temperature.

A central sprue, tray shape mould of dimensions 312 x 242 x 2.5 mm was used
in this experiment. It provides a good flat surface with bending curves at its
four sides. As with the manifold, heaters were also placed inside both mould
halves in order to heat the materials during the curing process, which causes
the plastics to cross-link. Insulation plates are placed between the mould and
the machine to prevent heat transfer from the mould, thus keeping the mould
temperature in the desired range. Around the sprue area are water jackets,
which help reduce the heat transfer from the material in the mould cavity to the
manifold part.

2.2 Materials
The materials used in this experiment were a general grade bulk moulding
compound, BMC G7B 5580 from BIP Ltd as a core material and a black
powder coating, Interpon PM-300011-F from Akzo Nobel as a skin material.

Figure 1. a) The manifold for 2K thermoset injection moulding machine. Both


halves have been placed between the injection unit and the heated mould. b) The
cross-section of the manifold nozzle

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S. Kiatmanaroj, V. Goodship and G.F. Smith

The resin used in the BMC was a glass filled unsaturated polyester with a
density of 1.73 g/cm3. This material is normally injection or compression
moulded to produce engineering and electrical components. Interpon is an
unsaturated polyester in-mould coating, normally used with BMC in
compression moulding technology. Its density is 1.25 g/cm3.

2.3 Gel time and melt flow index measurement


The gel time and flow ability of Interpon had been examined prior to the
injection moulding experiment with BMC, to establish its processing window.
5 g of powder coating was put onto a hot plate and levelled to around 1 mm
thickness. With variable temperature from 60–200 °C, the gel time was
measured from the time that the material started to melt until it turned to gel,
which was determined by a metal stick. Uncured material would show plastic
behaviour and could be picked up without breakage. Figure 2 shows the effects
of temperature on the material gel time.

The gel time of Interpon decreases dramatically as the temperature increases.


At a very high temperature, more than 120 °C, the melt takes only few seconds
to turn into gel. The three temperatures, 80, 85 and 90 °C were selected from
the gel time curve since the material could be in liquid state for what was
considered a reasonable processing window of 875-1375 seconds. The material

Figure 2. The effect of temperature to the powder coating gel time

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Sandwich Injection Moulding of Thermosetting Materials. Part I: Initial Experiments

was then put into a Ray-Ran 4MPCA melt flow indexer to examine the
material’s flow characteristics. By selecting a multi-slicing mode, the MFI
value was measured ten times at ten different points, giving an average MFI
value and the standard deviation. Table 1 shows the effect of temperature on
the material MFI value.

Table 1. The powder coating melt flow index


(g/10 min) and standard deviation at three
temperatures

Temp (°C) MFI STD


80 11.767 0.170
85 19.316 0.363
90 25.099 1.573

At the higher temperatures the material tends to flow more easily, as is shown
by the higher MFI numbers, but the time the material can stay in a liquid state
is shorter. The material tends to cure more easily at the higher temperatures
too, as shown by an increase in the standard deviation value. A melt temperature
of around 80-85 °C was selected as the temperature window of the skin
material.

2.4 Injection moulding of BMC and Interpon


To start, it was decided to mould BMC alone to set up a suitable manifold
temperature and sprue temperature. The molten BMC would be injected from
the horizontal barrel through the manifold runner and then flow into the mould,
while the top runner was blocked to prevent the melt escaping from the system
during injection. The manifold system was initially designed to operate at a
sufficiently high temperature to cure the whole runner after the mould had
completely filled, and then the part would be removed at the same time as
ejecting the component from the mould. Several tests showed that the
plasticised polymer tended to cure in the runner and sprue before it could flow
into the mould, since the sections there are too small in comparison with the
component (Figure 3). The problem would be worse when the top runner was
in use, because of a smaller runner diameter.

Consequently, the material in the manifold part was preserved in its molten
state during the moulding cycle by setting the manifold temperature to 80 °C.

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Moulding

Manifold runner

Figure 3. A side view of the tray moulding and manifold runner

To separate the manifold from the high temperature mould, water jackets were
placed around the mould sprue and the temperature was varied from 90 down
to 70 °C (this temperature is the outlet temperature of the cooling water),
where a full moulding could be made without gate freeze-off. The machine
was set as shown in Table 2 for the BMC according to the supplier’s
recommendation. Figure 4 shows the complete moulding made of BMC. The
best temperature for moulding this material was around 74 °C.

Using the settings shown in Table 2 both BMC and Interpon were injected into
the mould to make the first thermoset sandwich moulding. The skin and core
metering strokes were set at 80 and 50 mm respectively, and the switch-over
point was at 30 mm.

The sandwich moulding of the two thermosets is shown in Figure 5. Only half
of the mould could be filled and core material broke through at the centre. With
the two materials moulded together, the melts were cured, hardening and
blocking the flow before the entire mould could be filled. It was uncertain
where the melt started to cure and whether the powder coating affected the
flow properties of the BMC.

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Sandwich Injection Moulding of Thermosetting Materials. Part I: Initial Experiments

Figure 4. The component made of BMC

a) b)

Figure 5. a) The 2K thermoset moulding. b) The sandwich moulding and the


complete tray

Table 2. Settings for sandwich injection moulding of BMC and Interpon

Settings/Material BMC G7B 5580(21) Interpon*


Mould Temperature (°C) 160 160
Barrel temperature (°C) 35/ 35 (front/rear) 80/ 60 (front/rear)
Screw rotational speed (rpm) 50 50
Back pressure (bar) <3 0
Injection speed (mm/sec) 80 80
*The material melt temperature is around 80-85 °C under this setting condition

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Interpon was single-injected from the top barrel using the same condition
applied to the above dual injection moulding, in order to study its flow in the
mould. The result is shown in Figure 6.

The amount of Interpon material that could flow into the mould was even lower
than for the BMC and the sandwich mouldings. Compared with the result in
Figure 5, it was the BMC melt that helped push more Interpon into the mould
before the gate was frozen off. In other words, Interpon retarded the flow of
BMC in the sandwich moulding.

The difficulty of injecting the Interpon might be caused by the material


properties themselves or by the design of the machine system. The next two
sections focus on how these factors might affect the moulding.

2.5 Effect of material properties


Gel times of the two materials were compared and the results are shown in
Figure 7. This shows how fast those materials reacted to the temperature
changing. At a temperature above 90 °C the BMC tended to cure faster than
the Interpon, while the opposite happened at lower temperatures.

All temperature settings of the manifold and mould tools were set at around
80 °C or higher, which means there was a greater chance that the BMC could
turn solid, rather than Interpon. In reality, the Interpon was cured first and
caused the short shot problem already described in the previous section. So,

Figure 6. The moulding made of Interpon

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Sandwich Injection Moulding of Thermosetting Materials. Part I: Initial Experiments

Figure 7. Gel time curves of BMC and Interpon

other factors apart from the temperature must have affected the cross-linking
reaction during the moulding.

In Figure 8 the viscosities of both materials were compared. The relationship


between the viscosity and shear rate of Interpon at 85 °C was measured using
a Rosand rheometer RH7, while the viscosity of BMC was determined by an
in-line viscosity measurement, provided by the supplier(22). The viscosity of
Interpon was higher than that of the BMC at any shear rate, i.e. Interpon was
more viscous and so more difficult to inject at the same settings as those used
for BMC. At the same injection speed and the same volume, more shear
friction can be generated at the tool wall and produce excess heat. This heat
might be a factor in activating the curing reaction.

2.6 Effect of the manifold system


The manifold was designed to be a gate for the two materials to flow through
and form a sandwich layer prior to entering the mould sprue. The complete
plastic part, including the manifold, is shown in Figure 9.

The skin runner was designed to be quite long, as there was a design limitation

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S. Kiatmanaroj, V. Goodship and G.F. Smith

Figure 8 The relationship of viscosity and shear rate of BMC and Interpon

Skin runner (Interpon)


Mould

Core runner (BMC)

Manifold

Figure 9. The complete moulding part including the component and the manifold
runners

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Sandwich Injection Moulding of Thermosetting Materials. Part I: Initial Experiments

in moving the top barrel down to the sprue position. Its diameter was 6 mm (to
reduce the plastic scrap from the injection moulding) while the core runner was
6.5 mm diameter to match the nozzle of the horizontal injection unit, which
was easily reached from the back.

Consider the manifold geometry. The skin has to flow to a longer and smaller
runner than the core. At the same injection rate, this generates more shear
friction. Especially when a viscous material like Interpon is injected through
the system, more frictional heat is likely to be produced. The effect this has on
the curing of the material in the mould can be seen from Figure 6. During the
single injection moulding, the Interpon was cured almost as soon as it touched
the mould wall, even though the system temperature was kept as low at around
80 °C, which should have provided enough time for the material to be able to
flow in and fill the mould. In contrast, the BMC could fully fill the mould under
the same settings.

More Interpon could be injected in the sandwich moulding, as shown in


Figure 5. The improvement was achieved because the BMC was injected
within one second of the Interpon injection. This retarded the Interpon melt
cure, and together with the very low inlet temperature of the BMC, helped
reduce the Interpon temperature so that the skin was still able to flow in.

To increase the amount of Interpon in the mould it is necessary to decrease the


melt temperature, or more precisely, to counter any effects that cause the melt
temperature to rise. The two solutions that might be considered are (a) reducing
internal shear friction by reducing the injection speed and (b) modifying the
manifold runner and cooling the melt down by reducing the manifold temperature.
The latter needs to be carefully adjusted as too low a temperature causes the
material viscosity to increase.

2.7 Breaking through at the moulding’s centre


In Figure 5, looking at the middle front of the component where it is opposite
the mould sprue, there was a breakthrough of the core material. At the back of
the moulding, the core was fully encapsulated. The same moulding was
sectioned and checked to see whether the core material could penetrate to the
skin or whether it had accumulated only at the centre. The cross section is
shown in Figure 10.

The moulding shows a sandwich structure at the far end of the disk, with the
skin layer getting thicker away from the centre, and it is thicker at the back than
the front. When injection moulding with a tool such as this, the direction of

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Sandwich area Core breakthrough Sandwich area

Figure 10. The cross-section of the 2K thermoset moulding

flow changes suddenly from horizontal to vertical. This results in very high
pressure and shear at the moving half surface, especially opposite the gate. In
order to fill the mould, the new material melt from the barrel pushes the
previous material outwards and replaces it. Generally the previous material
melt will leave a thin film, called a frozen layer, on the mould surface. This film
is thicker in the case of thermoplastics, as the material can form the layer as
soon as it touches the cold wall, while with thermosets it is molten. This results
in a lower viscosity when it enters the hot mould, and then it becomes solid
because of the cross-linking reaction. If the speed of injection is too high, there
will be no time for the material to form that layer.

When two thermosets are injected, the molecular flow is more complex, since
the melt properties are a function of both materials. The core breakthrough at
the centre shows that the skin (Interpon) did not have enough time to form a
solid layer. At the time when the new melt was injected into the mould, the
BMC melt swept out the skin. The moulding shows that the skin was pushed
outward because of fibre abrasion and the higher density of the BMC melt. It
was not until the cross-linking took effect that the skin could form the solid
layer, when it had covered around half of the flow path. In order to provide
more time for the skin to form the layer, the act of starting the core injection
should be delayed. This can be done by increasing the delay time or reducing
the switch-over distance. However, the core speed may have to be increased
to force the core to penetrate into the skin as far as the edge of the moulding.

Another possible way to increase the sandwich area on the moulding’s surface
might be to move the gate position to one of the edges of the moulding, as
shown in Figure 11. The molecular flow is similar to that in the bottom half of
the central gate moulding, but more uniform. However, more shear stress and
cavity pressure may occur and the melt might be cured before the mould could
be fully filled. These factors need to be carefully considered.

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Sandwich Injection Moulding of Thermosetting Materials. Part I: Initial Experiments

Orientation at skin

2.000

1.000

8
174
Scale (120 mm)
-47

Figure 11. The molecule orientation of a polymer at skin in a side gate mould(23)

3. CONCLUSION
This paper describes some initial experiments on the sandwich injection
moulding of two thermoset polyesters, and the problems are presented. Prior
to the test run on the machine, the powder coating was investigated in terms
of gel time and flow behaviour in order to optimise the temperature settings for
the co-injection machine.

The BMC was injected solely to set up the manifold system. The manifold
temperature was chosen on the principle that the plasticised polymer was still
in its molten state during all injection cycles. All information gained from
those tests was used in determining the machine’s initial settings for the
moulding.

The first thermoset sandwich component was produced. Two problems found
from the experiment were (a) short shot resulted from pre-curing of the skin
and (b) breakthrough of the core component at the position opposite the mould
sprue.

It was shown that the short shot problem was caused by the powder coating
being pre-cured during injection. The excess heat generated in the system
especially in manifold runner was the main cause.

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The core breakthrough was the result of incorrect injection time and high
pressure at the position opposite the gate. A longer core injection delay time
or a shorter switch over distance will allow enough time for the skin to form
a solid layer and cover the core. The simulation from Moldflow® showed that
changing the sprue position might help to achieve a more uniform flow.
However, more experiments are needed to investigate this aspect further.

A number of potential problems with co-injection moulding of thermosets


have been highlighted by this work. It has been shown that balancing the shear
rate, cure time and change in viscosity during co-injection are vital for
successful thermoset sandwich moulding to be achieved.

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