Conference Record of the 1994 IEEE International Symposium on Electrical Insulation, Pittsburgh, PA USA, June 5-8, 1994

THE EFFECTS OF AGING ON THE INTERFACIAL BOND

IN PAPER-POLYPROPYLENE-PAPER LAMINATES
Paul J. Somodi and R. K. Eby
Department and Institute of Polymer Science
The University of Akron
Akron, OH 44325-3909

EXPERIMENTAL PROCEDURE

Abstract - This study is focused on understanding the

behavior of paper-polypropylene-paper (PPP) laminate aging
in hot oil in the absence of voltage stress. Peel strength
measurements on two laminates aged in polybutene oil at
90C for up to 950 hours showed an initial rapid loss of
strength followed by a much slower loss as a function of
long times. Weibull analysis of the data obtained on unaged
samples ahd those aged for 120 hours showed that the
strength loss is consistent with one failure mechanism and
the failure rate increases with applied stress. For the aged
sample, Weibull analysis results are consistent with the prior
loss of peel strength due to hot oil aging. Experiments on
the solubility of the polybutene oil show that lamination
reduces the amount of absorption in comparison to that for
the unlaminated composite. Swelling measurements on both
the polypropylene and paper components alone in the
machine and transverse directions show that the
polypropylene swells and the paper shrinks in both
directions. Slight differences (less than 1%) between the
amount of polypropylene swelling or paper shrinkage in the
two directions is due to orientation in the machine direction
for both components. Swelling measurements on the
laminate show that both paper and polypropylene shrink,
indicating that the paper govems the laminate swelling
process. It is suggested that during the aging time, the
differential swelling between the paper and polypropylene
imposes a stress on the interface and is responsible for the
loss of strength.

Materials
Two different PPP laminate samples were used. The sum of
the component thicknesses given in Table 1 is greater than
the laminate thickness possibly due to surface alterations of
the components resulting from the peeling process [31. Both
were produced by melt extrusion of Phillips Marlex@HGX330 polypropylene between two sheets of Tervakoski
capacitor grade-kraft paper. The polypropylenz has high
melt flow with M, equal to 42.5 kg/mol and MJM, equal to
3.8 [4]. Samples were stored at room temperature and about
50% RH.
When the laminates were immersed in hot oil to simulate the
service environment, Cosden OSH polybutene oil was used.
This type of oir is typical of those used as a pipe filling oil
with PPP insulated cables. It has a lower viscosity than the
cable impregnating oil and should hasten swelling effects.

Peel Strength Measurements

A 180" peel test geometry was used according to ASTM D
903-49, save for an extension rate of 10 cm/min.
Measurements were made on both sides of the two laminates
before aging in the polybutene oil and after 6, 12, 20, 48,
120, 300, 550, and 950 hours of oil aging at 90C. All
samples had dimensions of approximately 11 cm in the
transverse direction by 2.54 cm in the machine direction.
Samples were tested in air at room temperature and about
50% RH. At least five tests were performed for each
measurement. After all immersion agings, the samples were

INTRODUCTION
The PPP laminate system has been shown to be an
acceptable insulation for the high pressure oil-frlled high
voltage power cable based not only on outstanding dielectric
properties but also on economic feasibility. These cable
system types are rated to 345 kV and are being used for
commercial application in the United States [ll. An
important aspect of the PPP tapes is the paper-polypropylene
interfacial bond strength. Delamination can cause problems.
For example, failure of the bond can increase the dielectric
loss and reduce the mechanical performance [21.

Table 1. Samples investigated

Thickness (um)
Laminate
130
141

563

Poly~ro~ylenepaDer
90
85

43
54

paned dry with a paper towel to remove excess oil on the

surface.

microscopy results suggest the presence of mechanical

interlocking and, due to the close proximity of the
interaction, the existence of relatively weak secondary
forces. In addition, optical microscopy revealed no evidence
of transcrystallie growth at the interface.

X-ray Difiaction Measurements

Measurements were made on the polypropylene film from
peeled PPP with a Rigaku CN 2155R6 diffractometer
operated in both the transmission and reflection modes. The
scanning rate was lo/minute and the radiation was copper
filtered by nickel. The samples were single layers of the
film cut to dimensions of 2 cm by 1.7 cm. Measurements
were made with the long dimensions of the slits both parallel
to and perpendicular to the machine direction. Transmission
diffraction patterns of 43 pn kmft paper which had not been
bonded were also obtained with the same radiation, pinhole
collimation, an area detector, and the beam perpendicular to
the paper surface. The paper was cut to 2 cm x 2 cm and
slacked to make a sample with a 0.5 mm thickness.

Peel Strength Measurements

Depending on the laminate thickness and side tested, typical
unaged bond strengths range from 30 to 50 N/m. Since the
different thicknesses and sides exhibited different initial
unaged peel strengths, it was necessary to normalize the
strength obtained at a given aging time with this unaged
strength for each laminate thickness and side tested. The
scatter of 64 individual peel strength measurements obtained
from both sides of the 130 pm and 141 pm laminates after
aging in the oil at 90C for 120 hours gives a Weibull
distribution which appears to have the form characteristic of
a single failure process [51.

Oil Solubility at 90C

Weibull Analysis
The 130 pm laminate, the peeled polypropylene, and the 43
pm paper which had not been bonded were immersed in
polybutene oil at 90C. At specifk time intervals, samples
were removed, patted dry with a paper towel to remove
excess oil on the surface, and weighed to determine oil
uptake.

Swelling at 90C
The 130 pm laminate, the peeled polypropylene, and the 43
pn paper which had not been bonded were immersed in
polybutene oil at 90C. At specific time intervals, samples,
having initial dimensions of approximately 5.1 cm x 5.1 cm,
were removed from the bath, placed in a flat-bottomed dish
containing a small amount of oil from the bath, and covered
with a glass microscope slide to maintain flatness. The dish
was placed on an optical microscope stage, and the sample
dimensions, in the machine and transverse directions, were
measured with a traveling stage under reflected light. Three
measurements were made on each sample over a time period
of approximately six minutes in air at room temperature.

RESULTS AND DISCUSSION

Adhesion Mechanisms
Scanning electron micrographs [51 of the unaged, peeled
polypropylene surface showed the imprint of the surface
paper fibers. The majority of these are oriented parallel to
the polypropylene and penetrate only partially through the
surface. The presence of holes indicated that a few of the
fibers, which were normal to or at a steep angle to the
polymer surface, did penetrate the polypropylene. The

564

The functional form of the Weibull distribution [6] is given

by:

= 1- exp

[- (x/Xo-

XJX,)"

where x is the normalized strength, P the cumulative

probability of peel, m the shape parameter, x, the location
parameter, and x,the scale parameter. The three parameters
m, xu, and x, each have physical significance. The shape
parameter m is a measure of the dispersion of the
normalized strengths. The location parameter xu is the
normalized strength at which the first failure occurs [7].
The scale parameter x, is related to the normalized strength
at a probability of failure equal to 63.2% [8]. For certain
applications, it is sufficient to express the distribution as a
two parameter model with x,, = 0. However, the S test [9]
showed that at the 90th percentile, the 64 peel strength data
obtained after 120 hours of hot oil aging should be described
by a three parameter model. Therefore, Weibull analysis
[6,81 on aged and unaged data yields plots such as those
found in Figure 1. The data yield values of m, xu, and x,
equal to 8.75, -0.19, and 0.58 for the aged sample and 2.95,
0.82, and 0.20 for the unaged sample, respectively. A value
of m greater than one indicates that the failure rate increases
with stress, and a negative value of xu indicates that there
has been some loss of strength (the effect of the aging) prior
to the peel strength measurement. In addition, the straight
line nature of the plots provides further evidence that only
one failure mechanism exists.
Because of the existence of a single failure mechanism

Polypropylene and Paper

-2.5

-2.0

-1.5

-1.0

-0.5

0.25

0.0

0 100 200 300 400 500 600 700 800 900 1000
Time (hours)
Figure 3. Oil absorption by components and laminate

W - X J

Figure 1. Weibull analysis

Contrary to the swelling of the polypropylene, the kraft

paper in hot oil shrinks rapidly by 0.27% and 0.74% in the
machine and transverse directions, respectively. The
magnitude of the shrinkage in the transverse direction
increases an additional 0.25% over the aging time. The
difference in the shrinkage behavior between the two
directions of the paper is also due to orientation in the
machine direction. A two dimensional wide angle x-ray
diffraction pattem shows the equatorial arcs which are
characteristicof oriented cellulose materials [l l-121. Figure
4 illustrates the differential swelling which occurs in the
transverse direction between the paper and polypropylene.
This imposes a stress on the interface of the laminate.

acting in all of the samples, the normalized strengths

obtained at a given aging time for all sample thicknesses and
sides investigated could be averaged to obtain the composite
curve of Figure 2 [5]. It shows that there is an initial rapid
loss of strength followed by a slower loss at longer aging
times.

Oil Absorption at 90C

Results show that oil absorption by the laminate is much
slower than by either the paper or polypropylene components
alone. In addition, for samples of equal dimension, the sum
of the weights of the components is greater than the weight
of the laminate at any aging time as is illustrated in Figure
3. This result indicates that the paper of the laminate does
inhibit oil uptake at 90C.

Measurements on the laminate in hot oil indicate that both

the paper and the polypropylene shrink. This is consistent
for both the machine and transverse directions with the paper
shrinkage being slightly greater than that of the
polypropylene. As is illustrated in Figure 5. the magnitude
of the shrinkage of both paper and polypropylene in the
transverse direction increases over the aging time. This
phenomenon is consistent with the paper goveming the
laminate swelling process and is parallel to the rapid
decrease in bond strength followed by the slow decrease in
Figure 2.

Swelling at 90C
The swelling of the polypropylene at 90C is also rapid.
The swelling in the machine and transverse directions is
7.5% and 6.8%, respectively, in agreement with ref. 10.
This difference is attributed to the slight crystal orientation
detected by x-ray diffraction in the machine direction [5].

0.6
0.4

bF

The greater swelling and oil uptake for the unlaminated over
the laminated polypropylene probably accounts for the
increased dielectric loss and reduced mechanical properties
of the unlaminated compared to the laminated PPP [2].
Absorbed small molecules not only increase the mobility of
the polypropylene and impurities [13] present before the
uptake but can also contribute directly to a change of
dielectric properties [ 141.

,o 0.2
&

0.0
&
CONCLUSION

0 100 200 300 400 500 600 700 800 9001000

Time (hours)

The bond strength of PPP laminates is reduced by aging in

hot oil. Weibull analysis of peel strength data indicates that

Figure 2. Average of normalized strength vs. time (ref. 5 )

565

.s 4 t

!iG

.Ei

.E

2t

Polypropylene
PaDer

-7'; - ;.' =8 I
8 ot"l-=l~=-~

I2

-2

&-21

0 100 200 300 400 500 600 700 800 9001000

Time (hours)

0 100 200 300 400 500 600 700 800 900 1000
Time (hours)

Figure 4. Differential swelling in transverse direction

Figure 5. Laminate shtinkage in transverse direction

only one failure mechanism is responsible for this decrease.

Bemstein, "Characterization of the Interfacial Bond in

Paper-Polypropylene-Paper Laminates," Polym. Engr.
Sci., in press, 1994.
[6] W. Weibull, "A Statistical Distribution Function of Wide
Applicability," J. Appl. Mech., vol. 18, pp. 293-297,
September 195 1.
[7] C. F. Joyce, "A Weibull Model to Characterize Lifetimes
of Aluminum Alloy Electrical Wire Connections," in
IEEE Transactions on Components, Hybrids, and
Manufacturing Technology, vol. 14, pp. 124-133,March
1991.
[8] C. Lipson and N. J. Sheth, Statistical Design and
AnaZysis of Engineering Experiments. New York:
McGraw-Hill, 1973, ch. 2, pp. 4 2 4 .
[9] N. R. Mann and K. W. Fenig, "A Goodness-of-Fit for
the Two Parameter vs. Three Parameter Weibull;
Confidence Bounds for Threshold," Technometrics, vol.
17, pp. 237-245, May 1975.
[lo] D. R. Edwards, J. A. H. Counsell, J. A. M. Gibbons,
and R. M. Scarisbrick, "Polymer and PolymerRaper
Laminated Tapes for EHV Oil-Filled Cables," in
Proceedings of the Internatioml Conference on Large
High Volfage Electric Systems, CIGRE, 1972, 15-05,
pp. 1-8.
[l I] W.A. Sisson, "X-ray Studies of Crystallite Orientation
in Cellulose Fibers. 11," J. Phys. Chem., vol. 40,pp.
343-359, 1936.
[121 R. E. Mark,in Handbook of Physical and Mechanical
Testing of Paper and Paperboard vol. 2. New York:
Marcel Dekker, 1984, ch. 24, pp. 306-307.
[13] M. Fox, K. W. Plessner, and T. E. Shen, "The Effect of
Impregnants on the Dielectric Loss in some Polymer
Films," in Conference Publication, Dielectric Materials,
Measurements and Applications, IEE, 1970, pp. 22-25.
[14] J. le G. Gilchrist and J. K. Vij, "Dielectric Absorption
in Hydrocarbon Polymers with Non-polar Additives,"
Chem. Phys., vol. 115, pp. 319-323, July 1987.

This analysis also indicates that the failure rate increases

with applied stress, and that for the aged sample there is
some loss of strength prior to peel test measurement.
During aging in hot oil, the polypropylene swells and the
paper shrinks. It is suggested that the differential swelling
which occm between the paper and polypropylene creates
internal stress in the laminate and that it increases over long
aging times. This would lower the strength by allowing for
a smaller applied force to separate the two components. The
differential swelling in the transverse direction parallels the
decrease of bond saength with aging.
ACKNOWLEDGMENT

The authors acknowledge valuable discussions with Bruce

Bemstein and Ralph Sa", as well as support by the
Electric Power Research Institute under conmct RP7880-12.
REFERENCES

[l] E. M. Allam, A. L. McKean, and F. A. Teti,

"Development and Commercialization of PPP-Insulated
Pipe-Type Cable Systems," in Conference Record of the
IEEE International Symposium on Electrical Insulation,
1992, pp. 203-208.
[2] V. A. A. Banks and A. C. G. Secret4 "Plastic-Paper
Laminate for Oil-Filled Cables," in Conference
Publication, Dielectric Materials, Measurements and
Applications, IEE, 1975, pp. 205-208.
[3] R. K. Eby, S . A. Johnston, and A. Barbari, "An
Investigation of the Interfacial Bond Strength of
Polymeric Laminates," EPRI Report EL-7404, pp. 2-1,
August 1991.
[4] Phillips' Specification Sheet and personal communication
from Dr. E. T. Hsieh, Phillips Petroleum Co.
[5] S. A. Johnston, P. J. Somodi, R. K. Eby, and B. S .

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