Polymer Degradation and Stability 24 (1989) 327 333

Some Property Changes in Injection Moulded

Polypropylene Structural Foam
N. T o u l e s h k o v , S. D j o u m a l i i s k y & G. K o t z e v

Institute for Metal Science and Technology, Bulgarian Academy of Sciences,

U1. Chapaev 53, 1574 Sofia, Bulgaria

(Received 22 August 1988; accepted 1 September 1988)

ABSTRACT

In the injection moulding of structural foam, the polymer is subjected not only
to heat and mechanical stress, but also to the action of the decomposition
products of the blowing agent. Some property changes which occur in isotactic
polypropylene during processing by injection moulding have been studied
when a chemical blowing agent ( azodicarbonamide ) was used. The structural
foam samples were produced on an in-line injection moulding machine,
KuASY 800/250, and on a two-stage machine, SIEMAG 'Structomat'
2000/70, the melt temperature being varied in the range 200 to 260°C. The
properties studied were density distribution, flow index and mechanical
properties. It was established that injection moulding caused specific
structural changes in the polypropylene including strong cross-linking, which
affects the properties of the structural foam components.

INTRODUCTION

During processing, polymer melts are subjected to various effects, which

cause changes in their structure. In almost all cases these effects are due to a
combination of thermal and mechanical action in the presence of oxygen.
Because of the diversity of factors involved, it is very difficult to obtain data
which will allow the effects to be predicted. 1 M o s t frequently, the
thermomechanical action results in degradation, which is associated with
the increase in the flowability of the polymeric material, which has been
observed for polypropylene at various temperatures 2 and on multiple
extrusion. 3 A synergetic effect has been demonstrated on simultaneous
327
Polymer Degradation and Stability 0141-3910/89/$03-50 © 1989 Elsevier Science Publishers
Ltd, England. Printed in Great Britain
328 N. Touleshkov, S. Djoumafiisky, G. Kotzev

thermal and mechanical action on a melt of polypropylene and high-density

polyethylene.4
The situation is even more complicated in the case of processing foamable
polymer melts in which a blowing agent is added to the base polymer. The
most frequently used blowing agents are of the chemical type. 5 The presence
of a chemical blowing agent causes changes in the polymeric material for
three basic reasons, namely, the action of the products of thermal
decomposition, local overheating due to the thermal effect of the
decomposition reaction and changes in the rheological properties of the
polymer melt.
Isotactic polypropylene and azodicarbonamide are basic materials used
for the production of structural foam components. An investigation of the
changes which occur during injection moulding of this base compound is
therefore of special interest.

EXPERIMENTAL

Materials

Three types of test specimen were used of the following shape and sizes:
A cylinder of 182mm diameter, 10mm height and overall density
p = 730kg/m3; A prism with dimensions of 74 x 20 x 10mm; A double
paddle-type specimen with overall size of 167 x 28 x 14 mm.
The test specimens were produced by injection moulding from isotactic
polypropylene BUPLEN 7523 with a melt flow index of 3"5 g/10 min, and
into which was added 1% by wt of azodicarbonamide blowing agent
'Genitron EPA'.

Methods of moulding test specimens

The various conditions of moulding and thermomechanical treatment of the

melt were achieved by varying the melt temperature in the injection cylinder
between 200 and 260°C and by using three moulding processes designated A,
B and C, under a gas counter-pressure of 1"5 MPa.
The specimens of series A were produced on a two-stage injection
moulding machine, Siemag 'Structomat' 2000/70 (diameter of the plas-
ticising cylinder, 45 mm; diameter of the injection cylinder, 85 mm). The
injection nozzle channel (D = 16mm, L = 60mro) was connected to the
injection cylinder via a conduit with a diameter of 20 mm and 250 mm in
length.
The specimens of series B and C were produced using an in-line machine,
 Property changes in injection moulded polypropylene 329

KuASY 800/250, with a cylinder diameter of 70 mm. The injection nozzle

channel was directly connected to the cylinder which was 30 m m in length.
For specimens of series C the resistance was increased.
In all three methods the foaming of the material in the mould cavity was
effected by egression of part of the melt from the core of the moulded body
towards the injection cylinder. In some of the investigations, tests were also
made on unfoamed test specimens produced by conventional injection
moulding on the in-line machine without the use of any blowing agent
(Series S). The processing variables of injection moulding provide the
following conditions in the production of the test specimens:
Series A: An intricate Z-shaped path of the flow of the material from the
plasticising channel to the mould. Prolonged thermal action on part of the
material and the lowest mechanical action during injection, 7 = 150 to
200 s- 1.
Series B: A linear flow path, short thermal action time and an average
mechanical action, 7 = 1300 to 1600s 1.
Series C: As in series B, but with maximum mechanical action, ~:= 26 000
to 32 000 s- 1

Methods of investigation

Four general types of property changes were investigated.

(a) A determination was made of the insoluble residue (gel-fraction) after
dissolution of 1 g of the cylindrical test specimen in xylol at 125°C for
150 min.
(b) A plot was made of the density profile across the section of the
cylindrical test specimen by measuring, with a Carl Zeiss G-3 photometer,
the amount of light transmitted through an X-ray photograph of a prism,
182 x 16 x 10mm, cut-out from it.
(c) The Sharpy impact strength of test specimens, 74 x 20 x 10 mm, was
determined. Distance between the supports was 40 mm.
(d) Measurements were made of the tensile strength and the residual
deformation of the paddle-type test specimens (size of the working sector,
70 x 23 x 14) at a deformation rate of 10mm/min.
The impact strength o-i and the tensile strength ~r, are represented by
reduced values:
F P
ar - 6 and ~ -
So 6~ S°~oo

where F is the load, P is the work, So is the initial cross-sectional area, 6 is the
330 N. Touleshkov, S. Djoumaliisky, G. Kotzev

overall density of the test specimen and 6o (= 0.90 g/cm 3) is the density of the
polypropylene.
The melt flow index was determined in accordance with the Soviet
standard GOST 11645-73.
The cylindrical test specimens (6 =0"73g/cm 3) were used for the
determination of all characteristics; only the mechanical tests were
conducted with the other specimens (prism, 5 = 0.80g/cm3; paddle-type,
6 = 0.76 g/cm3).

RESULTS A N D DISCUSSION

Although all test specimens were produced from the same compound with
the same preset processing parameters, considerable differences were
observed in their structures. This result, which is a consequence of the
different combinations of thermooxidative and mechanical effects, which are
specific for each of the methods used, is a characteristic of all morpho-
logical levels, from the molecular structure of the polypropylene to the
macrostructure of the test specimens. The most obvious effect is the
occurrence in the tubular samples of series A, of considerable compaction of
part of the melt, which has been subjected to prolonged thermal action; this
material gets into a well defined zone of the test specimen, forming a visually
observable section of increased density.
Figure 1 shows density profiles across cylindrical test specimens obtained
by measuring the amount of light transmitted through X-ray photographs
(Fig. 2). Curve A' corresponds to the section with increased density. It is

O,6

0,~'31
I 0 B mm
Fig. 1. Density profile across structural foam samples.
 Property changes in injection moulded polypropylene 331

A
B
C

R r2 0 5 R:9
Fig. 2. X-ray photographs of the cross-section of structural foam samples.

obvious that distribution of the overall density in test specimen A results in

the establishment of two zones with specific density profiles across the
section. The specimens of the other two series, and particularly of series C,
are characterised by a distinct solid skin and a narrow, but highly foamed,
core zone. In this case, the skin thickness grows with increase in the
moulding temperature (Fig. 3); this can be explained by more intensive
degassing of the melt. This effect is less well defined in series C, at larger skin
thicknesses, because of the additional heating of the melt within the nozzle
channel.
Since the formation of the section with increased density is also a result of
prolonged thermal action on the melt, the material from this zone of the test
specimen is used to represent series A in the determination of the gel-fraction
and the melt flow index. Figure 4 shows that increase in moulding
temperature results in an increase in the content of insoluble residue.
Although this increase is greater for material not containing a blowing

2,5
8
ram!
2,0

1.5

1.0
220 240 260 Tm?C
Fig. 3. Dependence of the solid skin thickness, 6, on the melt temperature, Tin, in injection
moulding.
332 N. Touleshkov, S. Djoumafiisky, G. Kotzev

6
6,%

4
..-At

i... -~ B
& -A I

0 22.0 2/~0 2to0 Tm°,C

Fig. 4. Dependence of the gel-fraction, G, on the melt temperature, Tm, in injection
moulding.

agent, the absolute values are higher in the case of material containing a
blowing agent, particularly for series A. This means that both factors, the
content of blowing agent and the increase in temperature, cause cross-
linking of the polypropylene. The data for the melt flow index (Fig. 5) show
that the processes of degradation and spatial cross-linking of polypropylene
in the presence of azodicarbonamide occur simultaneously, the total effect
depending on the actual combination of temperature and mechanical
loading.

~in
DA
15

12

3
200 220 240 260 Tm,°C
Fig. 5. Dependence of the melt flow index, MFI, on the melt temperature, Tin, in injection
moulding.
 Property changes in injection moulded polypropylene 333

50
£
Oi 2 240"C 5t %
kJ/m 4Pc

30 30 12 220"C
2 20"C 240"C

Eljl
20 v J
20
v J

v ~

10 v f
IfJ
10
v /
v i

0 |f J

Fig. 6. Influence of the melt temperature, Tm, in injection moulding on some mechanical
properties of the test specimens:A, reduced impact strength ~ri;B, reduced tensile strength a,;
C, residual deformation ~..

The structural changes caused by thermomechanical action also influence

the mechanical properties of the test specimens. This is illustrated in Fig. 6 by
values of the impact strength (A), the tensile strength (B) and the residual
deformation (C). The considerably higher values of impact strength for the
specimens of series B and C correspond to the greater thickness of the solid
skin of the test specimen. The lower deformability of the specimens of series
A confirms that the processes of degradation and crosslinking are more
active in them.

CONCLUSIONS

This study shows that the mechanical load, the intensity and duration of
heating and the presence of a blowing agent cause remarkable differences in
the structural organization of the test specimens.
The processes of degradation and spatial cross-linking reach a greater
depth when the processed polypropylene contains azodicarbonamide.

REFERENCES

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3. Zamorsky, Z. & Muras, J., Poly. Deg. and Stab., 14 (1986) 41.
4. La Mantia, F. P., Valenza, A. & Acierno, D., Poly. Deg. and Stab., 13 (1985) 1.
5. La Clair, R. C., Plast. Techn., 22 (1976) 31.