Akita University

75

Received December 30, 2005

Accepted for Publication February 24, 2006
C2006 Soc. Mater. Eng. Resour. Japan

Mechanical and Dielectric Breakdown Properties of

Eco-Friendl y Dielectric Materials

Katsuyoshi SHINYAMA and Shigetaka FUJITA

Department of Electronic Intelligence and Systems. Hachinohe Institute of Technology

88 - 1, Myo Ohbiraki, Hachinohe, 031 - 8501 JAPAN
E-mail .' shinyama@hi-tech.acjp

The mechanical and dielectric breakdown properties ofpolylactic acid (PLA) and PET copolymer, which
are biodegradable plastics, were examined, and physicochemical analysis were performed. At room
temperature, the Young's modulus of PLA and PET copolymer were about 3 .6GPa and about 3.9GPa,
respectively. Moreover, the temperature to which Young's modulus of PLA and PET copolymer begins to
decrease was about 60'C and about 55'C, respectively. The dielectric breakdown strength (E*) ofPLA and
PET copolymer at room temperature were about 6.2 MV/cm and about 4.8 MV/cm, respectively. The E* of
PLA increased with an increase in temperature, and was about 6.9MV/cm at 60'C (aE*/6 T :O). The E.
of PET copolymer was hardly dependent on temperature in the domain of 70'C or less (6E*/a T 0) . In
contrast with it, when it became a high temperature region, E* of PLA and PET copolymer decreased with
the rise of temperature (6E /a T< O) .

Key Words : biodegradable plastics, mechanical properties, dielectric breakdown properties

the method used to produce them. Synthetic polymer is currently

1 INTRODUCTION in use.
The production of synthetic plastics including cross-linked Synthetic polymers can be ftirther classified into "plant based
polyethylene and epoxy resin has gathered pace rapidly as a result polymers" and "mmeral oil based polymers "
of developments in the petrochemical industry. These products We selected polylactic acid (PLA) that was "Plant base" and
now dominate all areas of daily life and industry. Synthetic polyethylene terephthalate copolymer (PET copolymer) that was
plastics are light-weight, easily processed, and have features of "Mineral oil base", which are considered as eco-friendly dielectric
viscoelastic materials such as mechanical properties, electric materials. In our research, we examined the mechanical and
insulation, insulation characteristics, and corrosion resistance, and dielectric breakdown properties of PLA, and conducted a physico-
are therefore widely used as electric insulation materials. In chemical analysis.
addition, with consumer electronics and digital assistants having
quickly become widely available, and the development of modern
2 EXPERIMENTAL METHODS
electrical, electronic and network industries, synthetic plastics will 2.1 Samples
be increasingly used as electric insulation material. However, most The sample used was biaxially oriented PLA and PET copoly-
of these instruments are disposed of after use and damage the mer films (trade name: Palgreen LC and BO, 25 and 20 /Im thick)
environment, causing a large problem for society. from Tochello Co, Ltd [1 1 1 . Figure I shows the chemical struc-
Biodegradable plastics are plastics that are decomposed via ture of PLA and PET copolymer. Low-density polyethylene
bacteria and decomposition enzymes in nature to produce water (LDPE) and polypropylene (PP) films were used as samples for
and carbon dioxide. They can therefore be treated as waste by comparison. The thickness of the samples for comparison was 25
being buried in the ground. These plastics generate only a small fl m.
amount of heat during combustion and do not release poisonous
2.2 Thermal analysis
nlaterials such as dioxins. This means that using biodegradable
A differential scanning calorimetry (DSC) instrument
plastics instead of synthetic plastics protects the environment
(Shimadzu, DSC-60) was used for thermal analysis. a -Alumina
[ I -5]. However, there are very few research reports into or
was used as a reference material, and the DSC spectra for PLA
authors working on the electrical characteristics of biodegradable
were observed over a rise in temperature from 30'C to 230'C at a
plastics, and for this reason, these plastics are not yet actually used
rate of I O'C/min. in a nitrogen atmosphere.
as electrical insulation materials [6-lO] .
There are three types of biodegradable plastics: biopolymers, 2.3 Mechanical properties
synthetic polymers, and modified natural polymers, which differ in A tensile test was performed based on the Japanese Indusinal

Int. J. Soc. Mater. Eng. Resour. Vol. 13, N0.2, (Mar. 2006)
Akita University

76 Katsuyoshi SHINYAMA et al

Standards (JIS K7 127*,,,) . In order to eliminate stress concentra- breakdown strength. The samples were cut into 50><50mm
tion, the sample was cut so that cracks would not develop. Figure squares. The side at high voltage was made into a ball electrode
2 shows the dimensions of the sample used in the tensile test. The with c 10 mm, and the earthed side was made into a disk electrode
sample was cut into strips of 150XIOmm like paper, with the with c25 mm, and rounded edges. To prevent creeping discharge,
distance between zippers (L) set to 100 mm. The distance between guard insulation was put in place on the contacts surrounding the
benchmarks (L ) was 50mm, and the samples were studied to high voltage electrode and the sample using epoxy resin. The
ensure that they would fracture within the distance L*. For LDPE, sample and the electrode system were soaked in silicone oil, and
L was set to 50mm. This is because the displacement at the time a positive high voltage direct current was applied at a rate of
of breakage is very large, and exceeds the capacity for displace- increase of I kV/sec. The temperature of the sample changed from
ment of the examination apparatus. The tensile speed was set to the room temperature to 120'C , and the specific conditions were
l OOmm/min, and the tensile strength was measured while the measured at least ten times.
sample was heated from room temperature to 1 20"C , and the
specific conditions were measured at least five times.
3 RESULTS AND DISCUSSION
3.1 Thermal analysis
2.4 Dielectric breakdown properties
Figure 4 shows DSC spectra ofPLA and PET copolymer. In the
Figure 3 shows the experimental system for measuring dielectric
glass transition temperature (Tg) values derived from the DSC
spectra, the value for PLA was about 66"C , and PET copolymer
was about 54'C . Thus. T= of PLA was a little higher temperature

H TO-CHHIC TOH than PET copolymer. A Iarge absorption peak also appears at
temperatures above 1 50'C . The peak was attributed to melt transi-
IlO

tion, the temperature of which corresponds to the melting point

(T*) . In the T* values derived from DSC spectrum, the value for
PLA was about 168'C, and PET copolymer was about 203'C .
(a) pLA
Therefore, it was seen that PET copolymer with the aromatic ring
is more excellent thermal stability than PLA.

3.2 Mechanical properties

Cll UrCll OCH,CH M Figure 5 shows the relationship between tensile strength and
O
O

temperature at breakage. The tensile strength of PLA and PET

copolymer at room temperature were about I OOMPa, almost the
(b) PET copolymer same as the value for PP. This value was about four times the
tensile strength of LDPE. In all the samples, tensile strength
Figure I Chemical structure of PLA and PET copolymer. decreased with a rise of temperature, and at I OO "C the tensile
strength of PLA was almost the same as LDPE. The decreasing
rate of tensile strength of PET copolymer became a tendency to
150 mn 100k like PP, and was more gradual than the decreasing rate of
PLA.
Figure 6 shows curves of tensile strength against displacement

15 mm
0.2
l Tr66 C
Figure 2 Dimensions of the sample used in the tensile test.
f

' nu
aD jt f ' '
' s'/
/

. ,,..,
..
I

DC High voltage
(1 kV/sec)
j

e: -0.2 Tg=54C
i'
Weight e' Tm=203'C
:

High voltage electrode

(-500 g) // (EPoxy(Brass,
resin)c20 mm) o
i

- 0,4
Guard Insulation
11 PIA
f

Fi ------ ET copolymer
Sample (50x50 mm) ' -0.6

lisul tbn Qil Earth electrode

(silicone) (Brass, c25 mm) T =168C - 10'C/inim
*o . 8

50 IOO 150 200

Temperature ('C)
Figure 3 Experimental system for measuring dielectric breakdown
strength. Figure 4 DSC spectra of PLA and PET copolymer.

Int. J. Soc. Mater. Eng. Resour. Vol.13, N0.2, (Mar. 2006)

Akita University

Mechanical and Dielectric Breakdown Properties of 77

Eco-Friendly Dielectric Materials

at 40"C . The tensile strength and displacement curves of PLA were

PIA

e!,e5
similar to PP, and the tensile yield strength of PLA became higher
eo il !le eee ,, .. .e ..

16
e
than the value for PP. On the other hand, the tensile strength and

l;;'
displacement of PET copolymer became higher than the value for 60 '

D,
PLA. l rA AAAAA AAAAAA
Figure 7 shows curves of tensile strength against displacement
of PLA and PET copolymer. The tensile yield strength of PLA be-
came lower as the sample temperature rose, and the slope of the
g40
(,D
start of the curves tended to be straight. The tensile yield strength

J
of PET copolymer became lower as the sample temperature rose " I20
!"'(all l""I' I Il 11 l"I'

"
't)
like PLA, but the tensile yield strength didn't appear at 60 'C .

"
Moreover, the slope of the tensile strength and displacement

5
o

2
curves of PET copolymer became looser than that of PLA. That is,

1
4
the PET copolymer became soft by the rise of temperature than
Displacement (mm)
PLA .
(a) PIA
The Young's modulus was evaluated from the inclination of the
straight line portion of the beginning of these curves L 12] . The
Young's modulus of the other samples was also evaluated. The
_80 r lA ::: I ed'eee ,bN
PET coplymer /

e
results are shown in Figure 8. This figure shows the relationship

f
'5

b
e e
60 Ll ] .()

,
)

/
,:

.
l

120 o pLA
40

'rl
A PEr *'p'lym"
a u)PE CQ A AdLAA
-,, 100
e pp
_'1' ' "AIAAA'AA
Yf
x! }!
)
l.1

e " l20
'C"'

IJ f
f

80 "f"'_
o

Idl'lii'lii 'I I' id l'

'
O

D
o

5
2
1

e , 60
S

Displacement (mm)
1' (b) PET copolymer
.- 40
El

'a

E
,,
20 e c o o Figure 7 Tensile strength-displacement curves of PLA and PET
co polymer.
o

20 60
40 80 1 OO (oC) 1 20
8

Temperature
S

Figure 5 The temperature dependence of tensile strength at break.

7
>
150
6
'I

I
2

D
ee
:5
*o

IOO
i

PET copolymer

l4
I15:l

.:
g'

t'
eJD
3
l
t)

-O- PLA
,__o 50
PIA 2 F pET copolymer
Q F

PP :- LDPE
1
Iio

n)pE 20 4060Temperature
80 100 (oC) 120
O

Figure 8 Relationship between Young's modulus and temperature.

Displacement (mm)
Figure 6 Tensue strength-displacement curves at 40'C .

Int. J. Soc. Mater. Eng. Resour. Vol.13, N0.2, (Mar. 2006)

Akita University

78 Katsuyoshi SHINYAMA et. al.

Table I Feature of dielectric breakdown properties of PLA and PET rise in temperature above 60 'C in the high temperature region
co polymer. (6E*16T< O) . This indicates that the temperature can be divided
into two regions bordering on the neighborhood of 60'C . On the
other hand, the E* of PET copolymer at room temperature was
about 4.8 MV/cm, and is lower than PLA. The E* of PET copoly-
mer increased with a rise in temperature.
The E* of PET copolymer was hardly dependent on temperature
in the domain to the neighborhood 70"C from room temperature
(aE*/a T O) . However, E* of PET copolymer decreased with a
20ec (_ ' 120'C rise in temperature above 70'C in the high temperature region.
Glass-1ike Rubber-like This indicates that the temperature can be divided into two regions
bordering on the neighborhood of 60'C ( 6E*/6 T<0). Here, the
E*: dielectric breakdown strength, T: temperature
Tg: glass transition temperature, T=: softening point results in Figures 4 and 8 shows that the T* and T, of PLA is near
the temperature of this boundary, and the T= and T, of PET copoly-
mer is about 1 5 degrees lower than the temperature of boundary.
between Young's modulus and temperature. The Young's modulus This feature of the dielectric breakdown properties above was
of PLA at room temperature was about 3.6 GPa, about I .7 times as summarized in Table I . Below, the dielectric breakdown mecha-
large as the value for PP, and about I I times as large as the value nism in each domain is examined based on this fact.
for LDPE. On the other hand, the Young's modulus of PET
Dielectric breakdown mechanism in Region I
copolymer at room temperature was about 3 .9 GPa, and became a
value a little higher than PLA. The Young's modulus of PLA and Although the E* of PLA increased with the rise of temperature,
PET copolymer decreased gradually with a rise in temperature, the E* of PET copolymer hardly changed with variation of sample
and decreased rapidly for high temperatures, 50'C and above. temperature. An electron avalanche breakdown can be considered
From these results, it was found that the softening point (T,) of to be the mechanism acting in this region [14, 1 5] .
PLA and PET copolymer were at a high temperature just over
Dielectric breakdown mechanism in Region II
60"C and 50'C , respectively, and it is thought to be near T*. At
80'C and above, the Young's modulus of PLA and PET copolymer In this domain, as shown in Table I , the state become
became similar to PP. This result shows that PLA and PET copoly- aE*/a T< O, and so thermal breakdown can be considered to be a
mer are harder than PP and LDPE at temperatures lower than 80'C. primary candidate for the dielectric breakdown mechanism [14,
15].
3.3 Dielectric breakdown properties
The results of the investigation by the authors into the depend-
Figure 9 shows the relationship between dielectric breakdown
ence of temperature on the current conducted by PLA and PET
strength (E*) and temperature. The E* of PLA at room tempera-
copolymer, shows that the current increases rapidly at a level
ture was about 6.2 MV/cm, about I .4 times as large as the value for
above T=, and it is thought that ion conduction occurs easily due to
LDPE. It has been reported that the impulse breakdown strength of
the micro Brownian motion of molecule chains [7, 9, I O] . In other
PLA at room temperature is 1.3times that of XLPE [13]. The
words, since the Joule heat due to ion conduction increases when
E* of PLA increased with a rise in temperature, and was about 6.9
the temperature of the sample is raised, it is thought that E* falls.
MV/cm at 60'C (aE*/6T 0). The E* of PLA decreased with a
In the next state, PLA and PET copolymer are thermoplastic
polymers, since this temperature domain is higher than the T= and
T, of PLA and PET copolymer, shown in Table I , and so Maxwell
8

stress occurs with the inter-electrode pressure accompanying the

S

applied voltage, and it is expected that electromechanical break-

down will take place easily here. According to the electromechani-
_C' 7
> cal breakdown theory [14, 15], the relationship between the
6 dielectric strength and the Young's modulus is
1*

eJD E =rexp f[_ 1j """""""' (1)

.

:i5
i

where E is the electromechanical breakdown strength, :* , is

, 4 the dielectric permittivity, and Y is the Young's modulus. The
3,92

relationship between temperature and E calculated using the

relative permittivity (e,) of PLA and PET copolymer which the
- - plA authors have reported [ I O] , and the Young's modulus of PLA and
Q2 - pEr copolymer
PET copolymer shown in Figure 8, is shown in Figure I O with the
-a- LDPE
result of this experiment. The measured value of the dielectric
1

breakdown strength (E*) shown in Figure 9 is also shown in the

20 60
40 80 1 oo 1 20
Temperature ('O figure. As can be seen from this figure, the calculated value (E )
was higher than the measured value (E*). This tendency is also
Figure 9 Relationship between dielectric breakdown strength and reported for other polymer films [16, 17] . Y. Inuishi and M. Ieda
tem perature. [18] consider that the above tendencies are shown in local

Int. J. Soc. Mater. Eng. Resour. Vol. 13, N0.2, (Mar. 2006)
Akita University

Mechanical and Dielectric Breakdown Properties of 79

Eco-Friendly Dielectric Materials

mechanical weak points. That is, where E Q<:E* even if E > E*, it
is likely that electromechanical breakdown may have occurred. 4 CONCULUSIONS
Here, if Equation (1) is simplified, the relationship between E* The mechanical and dielectric breakdown properties of
and Young's modulus can be given as follows. polylactic acid (PLA) and polyethylene terephthalate copolymer
(PET copolymer) , which are biodegradable plastics and are
EFo(:fY (2) considered as eco-friendly dielectric materials, were examined,
and a physicochemical analysis was performed. The results of
The relationship between EB and Young's modulus of PLA and these were as follows:
PET copolymer are shown in Figure 1 1 . The dotted line in the ( I ) The tensile strength of PLA and PET copolymer at room
figure shows the curve of Equation (2) . This Figure shows that the temperature were about I OO MPa, almost the same as the value for
relationship in Equation (2) is found in the temperature domain PP. At I OO C, the tensile strength of PLA was almost the same as
ftom 80 to 120'C in PLA. Moreover, this Figure shows that the LDPE. The decreasing rate of tensile strength of PET copolymer
relationship in Equation (2) is found in the temperature domain is similar to that of PP.
from 70 to 1 20"C in PET copolymer. That is, it is shown that a (2) The Young's modulus of PLA in room temperature was
local mechanical weak point occurs about here. In this domain, it about 3.6GPa, about 1.7times as large as the value for PP, and
thought that electromechanical breakdown occurs in addition to about 1 1 times as large as the value for LDPE. The Young's
thermal breakdown, and the temperature of PLA is above 80'C , modulus of PET copolymer at room temperature was about 3 .9
and the temperature of PET copolymer is above 70'C . GPa, and became a value a little higher than PLA. The temperature
to which Young's modulus of PLA and PET copolymer begins to
decrease was about 60'C and about 55"C, respectively.
(3) The dielectric breakdown strength (E*) of PLA and PET
102
copolymer in room temperature was about 6.2 MV/cm and about
EM 4.8MV/cm, respectively. The E* of PLA increase with a rise in
,. >

temperature, and was about 6.9MV/cm at 60'C (6E*/aT 0).

The E* of PET copolymer was hardly dependent on temperature in
the domain to the neighborhood 70'C from room temperature
-o- } PIA
( 6 E*/6 T :O) . In this domain, it is thought that an electron
.: -1-
-h } copolymer
PET avalanche breakdown occurred. In contrast with it, when it became
I

e9
. -
S

a high temperature region, E* of PLA and PET copolymer

,

lOl
decreased with the rise of temperature (6E*/a T< O). In this
domain, it was thought that electromechanical breakdown occurs
! :1!

in addition to thermal breakdown, and the temperature of PLA is

above 80'C, and the temperature of PET copolymer is above 70"C .
:
e: l ,

EB Acknowledgments
This work was supported by a targeted research subsidy from
100 the Hachinohe Institute of Technology. The authors would like to
20 40 Temperature
60 80 100 (oC)
1 20 thanks Tochello Co., Ltd, for supplying the test samples.

Refere n ces
Figure 10 Comparison between measured value of dielectric breakdown
strength EB and theoretical value of electromechanical break-
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O PIA
>7 A PET copolymer 7crc
.." o
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9 C "'
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5

l 10'C/6 / O'C evc

"

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Int. J. Soc. Mater. Eng. Resour. Vol.13, N0.2, (Mar. 2006)