Polymer Testing 15 (1996) 45-52

0 1995 Elsevier Science Limited

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ELSEVIER

MATERIAL PROPERTIES

Some Properties of Polymer Blends Based on EPDM/PP

Ana Lticia Nazareth da Silva & Fernanda M. B. Coutinho*

Instituto de Macromokulas, LJFRJ, PO Box 68525, 21945-970, Rio de Janeiro, RJ, Brazil

(Received 6 February 1995; accepted 14 March 1995)

ABSTRACT

This work describes the effect of the addition of EPDM to polypropylene on the
mechanical performance of EPDMjPP blends prepared in different composition
ranges and mixing conditions, and evaluates the eflect on the mechanical properties
when controlled degraded polypropylene is added to these blends as a third
component. It was found that as the EPDM content increased, the impact strength
of EPDMjPP blends increased; the tensile strength and Young’s modulus decreased
and the elongation increased but showed a slight decrease at 50/50 composition.

INTRODUCTION

Polymer blends comprise one of the most interesting and useful class of
materials, characterized by the intimate combination of two distinct
phases.’
Since 1980, new developments of polymer blends and alloys of thermo-
plastic species have been sharply increasing and the main reason for this
is economy. If a material can be generated at a lower cost with properties
meeting specifications, the manufacturer must use it to remain competi-
tive.2
The most difficult task is development of materials with a full set of
desired properties. This has been achieved by selecting blends components
in such a way that the principal advantages of the first polymer will
compensate for deficiencies of the second one and vice versa.2
In recent years, elastomeric rubber-plastic blends have become techno-
logically interesting for use as thermoplastic elastomers.3 These materials
*To whom correspondence should be addressed.
45
46 A. L. N. da Silva, F. M. B. Coutinho

exhibit some of the physical properties of elastomers at lower temperatures

and are processable at elevated temperatures.4
Polypropylene (PP) because of its poor impact strength is often modi-
fied by elastomers.5
Among the various elastomers used as impact modifiers, ethylene-
propylene-diene terpolymers (EPDM) have proved to be the most effective
ones. Thus considerable work has been reported on the blends of poly-
propylene (PP) and ethylene-propylene-diene terpolymer (EPDM) due to
their commercial interest.6,7
Thus, the objective of this work was to investigate the effect of EPDM
on the mechanical properties of polypropylene for EPDM/PP blends and
to evaluate the influence of the addition of controlled degraded polypropy-
lene to the EPDM/PP blends.

EXPERIMENTAL

1 Materials

The polymers used in this work are listed in Table 1. Polypropylene (PP)
and ethylene-propylene-diene terpolymer (EPDM) with ethylidene nor-
bonene (ENB) as a termonomer were all commercially available grades.
The peroxide employed in the PP degradation was CI,cr’-di-(tert-butyl-
peroxy)-1,4-di-isopropylbenzene (DIPP) from Atochem-Penwalt (99% of
purity) and o-dichlorobenzene distilled before use was the solvent used.

2 Polypropylene degradation

The degradation reaction was carried out at 150°C (controlled by a thermo-

stated silicon oil bath) in o-dichlorobenzene solution in 1.0 L glass reactor
equipped with a mechanical stirrer, a condenser, and a nitrogen input.

TABLE 1
Characteristics and Sources of PP and EPDM

Material Characteristics Sources

PP MFI (g/10 mm) 3.5 POLIBRASIL S. A.

wt % of PP 25.7
EPDM wt % of ENB 5.0 NITRIFLEX S. A.
MWD 2.9
 Some properties of polymer blends based on EPDMjPP 41

Commercial PP (40 g) and 400 ml of solvent were added to the reactor.

The polymer solubilization was carried out at 150°C under nitrogen atmos-
phere with constant stirring (150 rpm). Under a continuous flow of nitrogen,
the peroxide solution (0*30% wt of PP) was finally added to the reactor. After
two hours, the reaction was interrupted. The mixture was cooled and the
polypropylene filtered off in a Buchner type filter, washed thoroughly with
toluene and acetone and finally dried in an oven at 60°C for 12 h.8

3 Blends preparation

The polypropylene and EPDM were blended in a Brabender mixer (GNF

106/2) in the proportions of 25, 30, 50 and 75 wt% EPDM in the molten
state at 220 and 250°C for 10 min. During the experimental runs, the shear
intensity was controlled by adjusting the rotating speed of the mixer at 20,
40, 60 and 100 rpm.
The degraded polypropylene (PP-deg) was only added to 25/75 and
50/50 EPDMjPP blends.

4 Preparation of the samples

Samples for mechanical properties measurements were cut from pressed

material (198”C/5 min. in a hydraulic press).

5 Measurements

Melt flow index (MFI) of PP, PP-deg, EPDM/PP and EPDM/PP/PP-deg

according to ASTM D1238 were determined on an EMIC TFT 315
instrument at 23O”C/2.16 kg.
The tensile properties were obtained by tensile testing analysis on an
Instron Tester (Model 4204) at a strain rate of 10 cm/min. at room
temperature.
The impact strength analysis was carried out according to ASTM D256
on an Impact Tester (TM1 NO 43-l).

RESULTS AND DISCUSSION

The mechanical and flow properties of EPDM/PP blends are shown in

Figs l-6. Tables 2-4 show the PP and PP-deg properties, and the effect of
the mixing temperature and the addition of PP-deg on the EPDM/PP
properties.
48 A. L. N. da Silva, F. M. B. Coutinho

0 50 100

Mixer rotrtlng speed (rpm)

Fig. 1. Elongation at break as a function of EPDM content (220”C/20rpm).

0 25 50 75 100
WEPW
Fig. 2. Stress at maximum load of EPDM/PP blends as a function of EPDM content
(22O”C/20 x-pm).

0 25 50 75 100

SC EPDM

Fig. 3. Young’s modulus of EPDM/PP blends plotted against EPDM content (22O”C/20rpm).

Effect of EPDM on the mechanical propertiesof EPDM/PP blends

In Fig. 1 the elongation at break of the blends is plotted as a lunction of

elastomer content. The elongation increased with the increase cf the elastomer
content, but showed a slight decrease at 50/50 composition.g This behavior
was also related by Pukanszky and Tiidiis.”
 Some properties of polymer blends based on EPDMjPP 49

0 25 !a 75 100
SCEPDM
Fig. 4. Impact strength (IZOD) of EPDM/PP blends versus EPDM content (22O”C/20rpm).

800 -.
f
3
- mo--
fi 4
[ 400--

t; 200-- l
l
% (Jq

0 25 50 75 loo
% EPDM
Fig. 5. Toughness as a function of EPDM content (22o”C/20 rpm).

Fig. 6. Effect of shear intensity on the flow index behavior for EPDM//PP blends (22O”C),
where (A) PP; (B) 25175; (C) 30/70; (D) SO/50 and (E) 75/25.
50 A. L. N. da Siiva, F. M. B. Coutinho

TABLE 2
PP and PP-deg properties

Material Stress at Elongation Modulus Toughness MFI

maximum at break (MPa) (MPa) (g/l 0 min)
IOld WI
WW

PP 32 880 900 180 3

PP-deg 22 3 965 0.2 10

TABLE 3
Mechanical properties of EPDM/PP blends (220 and 25o”C/20 rpm)

EPDMIPP Modulus (MPa) Elongation at Toughness (MPa)

break (%)

220°C 250°C 220°C 250°C 220°C 250°C

25175 400 490 685 660 110 100

so/so 230 190 670 160 50 10

TABLE 4
Effect of PP-deg on the mechanical properties of EPDMjPP blends (22O”C/20 rpm)

EPDM/PP/PP-deg (phr) Toughness MFI Impact Strength (IZOD)

(MPA) (g/IO min) (J/m)

25/75/O 110 1.6 150

2517515 15 1.8 140
25175125 10 2.2 120

50/50/0 50 0.6 540

50/50/5 45 1.0 460
50/50/25 40 1.2 220

Figures 2 and 3 show that as EPDM content increased, as expected, the

stress at maximum load and Young’s modulus decreased, i.e., the rigidity of
the blends decreased.”
Figure 4 shows that as EPDM content increased, the impact strength of
EPDM/PP blends, as expected, increased, as it was also shown by Choudhary
and Varma. ’ ’
Figure 5 shows that as EPDM content increased, the material toughness
increased up to 30/70 composition and then a decrease of this property was
observed, because of the significant loss of rigidity of the blends.
 Some properties of polymer blends based on EPDMjPP 51

E&et of the mixer rotating rate on tbe melt flow characteristicsof EPDM/PP
blends

Figure 6 shows that, as expected, the stronger shear forces with higher mixer
rotating speed provoked a more intense mechanical degradation in the
polypropylene chain, The decrease of molecular weight provoked by mechan-
ical degradation was confirmed by the increase of melt flow index as the shear
intensity increased.
Table 2 shows that in spite of the higher melt flow index (higher flow rate in
the molten state) presented by PP-deg, its toughness was smaller in compari-
son to the virgin polypropylene (PP). These results are in agreement with the
work of Tzoganakis who has related that controlled degraded polypropylene
has a higher melt flow index (MFI) and a reduced elasticity.5
Table 3 shows that when the mixing temperature increased the mechanical
properties of the EPDMjPP blends decreased. That can be attributed to an
increase on the material degradation.
Table 4 shows that the addition of PP-deg to EPDM/PP blends provoked
a decrease in the toughness and an improvement in the flow characteristics of
the mixtures analysed.

CONCLUSIONS

(1) It was verified that when the elastomer content increased, the rigidity of
EPDM/PP blends decreased: Young’s modulus and stress at maximum
load decreased and elongation at break increased.
(2) When the proportion of EPDM increased (regions of energy absorp-
tion), the impact strength increased.
(3) Up to 30/70 EPDM/PP composition, the rigidity of the blends
decreased significantly, and a decrease in the material toughness was
observed.
(4) At a rotation rate higher than 40 rpm, an intensification on the
mechanical degradation of the polypropylene occurred. This fact was
confirmed by the increase on the polymer melt flow index.
(5) When polypropylene was degraded, a reduction in the number of
longer chains occurred. It provoked a decrease in the elongation of the
material and consequently a decrease in the toughness of the poly-
propylene.
(6) An increase on the mixing temperature provoked a decrease in the
mechanical properties of the blends, indicating that elevated tempera-
tures combined with shear forces must have provoked an increase in
the material degradation.
52 A. L. N. da Silva, F. M. B. Coutinho

(7) The addition of PP-deg to EPDM/PP blends resulted in decrease of

the material toughness and an increase in the melt flow index of the
EPDM/PP compositions analysed, indicating an increase in the rigidity
and an improvement in the flow characteristics of the blends.

ACKNOWLEDGMENT

Financial supports by CAPES, CNPq and CEPG/IJFRJ are gratefully ac-

knowledged. We are also grateful to POLIBRASIL S. A., NITRIFLEX S. A.
and CENPES/PETROBRAS.

REFERENCES

1. Paul, D. R., Background and perspective. In Polymer Blends, eds D. R. Paul & S.
Newman, Academic Press, New York; Vol. 1, 1978, pp. l-2.
2. Utracki, L. A., Polymer Alloys and Blends: Thermodynamics and Rheology,
Hanser Publishers, New York, 1989, pp. 13-33.
3. Rader, C. P., Introduction to TPES. In Modern Plastic, ed. R., Greene, New
York, 1992, pp. 99-100.
4. Thomas, D. A. & Sperling, L. H., Interpenetrating Polymer Networks. In
Polymer Blends, eds. S. Newman & D. R. Paul, New York, Academic Press, Vol.
2., 1978, pp. l-5.
5. Tzoganakis, C., Tang, Y., Vlachopoulos, J. & Hamielec, A., Controlled degrada-
tion of polypropylene: a comprehensive experimental and theoretical investiga-
tion, Polym. Plast. Technol. Eng., 28(3) 319(1989).
6. Chang, S. H., Dong, J. I. & Sung, C. K., Structure and properties of dynamically
cured EPDM/PP blends, Journal of Applied Polymer Science, 32 (1986) 6282.
7. Pukanszky, B., Tiidos, F.,, Kallo, A. & Bodor, G., Multiple morphology in
polypropylene/ethylene-propylene-diene terpolymer blends, Polymer, 30 (1989)
1399.
8. Coutinho, Fernanda M. B. & Costa, Thais H. S., Controlled degradation of
polypropylene in solution by organic peroxides, Polymer Testing, 9 (1994) 2.
9. Sabet, A. & Patel, R., Morphology of elastomeric alloys, Rubber Chemistry and
Technology, 64(5) (1991) 769.
10. Pukanszky, B., Tiidiis, F., Kallo, A. & Bodor, G., Effect of multiple morphology
on the properties of polypropylene/ethylene-propylene-diene terpolymer blends,
Polymer, 30 (1989) 1407.
11. Choudhary, V., Varma, H. S. & Varma, I. K., Polyolefin blends: effect of EPDM
rubber on crystalization, morphology and mechanical properties of polypropy-
lene/EPDM blends. 1, Polymer, 32(14) (1991) 2534.