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IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS, VOL. 40, NO. 4, JULY/AUGUST 2004

Electrical Properties of Biodegradable

Polylactic Acid Film
Takashi Nakagawa, Takuo Nakiri, Ryuichi Hosoya, and Yoshiro Tajitsu, Member, IEEE

AbstractWe measured the basic electrical insulation characteristic of biodegradable polylactic acid (PLA), and the following
results were obtained. The volume resistivity, dielectric constant,
and dielectric loss tangent measured at room temperature were almost the same as those of crosslinked polyethylene (XLPE) currently used as insulating material for cables and electric wires. The
mean impulse breakdown strength of PLA was about 1.3 times that
of XLPE. Also, space charge accumulation in PLA and XLPE was
measured. The amount of space charge accumulation in PLA was
one-half that in XLPE when dc voltage was applied for a short time.
Index TermsBiodegradable polymer, electrical insulation
characteristics, film, polylactic acid (PLA).

I. INTRODUCTION

VERY YEAR, the amount of industrial waste increases,

and as a result, environmental pollution is now becoming
serious. Certain types of polymers can be decomposed into
their component elements by the action of microorganisms,
even in a local environment [1], [2]. Such polymers are called
biodegradable polymers [1], [2]. As materials that are expected
to provide a solution to environmental pollution, biodegradable
polymers have attracted much attention [1], [2]. Polylactic
acid (PLA) is an aliphatic polyester with the most advanced
biodegradability research [1], [2]. For this reason, PLA is
attracting much attention in industrial fields. PLA is manufactured in three steps. First, starch is produced from corn,
for example. Second, microorganisms are used to decompose
starch into lactic acid. Third, PLA is produced from lactic acid
through chemical synthesis. The structural formula of PLA
is shown in Fig. 1 [1], [2]. PLA is a chiral polymer in which
molecules containing asymmetric carbon atoms have a helical
orientation [1], [2]. Two optical isomers exist in PLA: PLLA
and PDLA [1], [2]. The crystal structure of PLLA is based on
Paper MSDAD-A-04-04, presented at the 2003 Joint Meeting of the Electrostatics Society of America and the IEEE Industry Applications Society Electrostatic Processes Committee, Little Rock, AR, June 24-27, and approved for publication in the IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS by the Electrostatic Processes Committee of the IEEE Industry Applications Society. Manuscript submitted for review June 27, 2003 and released for publication March
29, 2004. This work was supported in part by the Ministry of Education, Culture, Sports, Science and Technology, Japan, under Grant-in-Aid for Scientific
Research 15550100.
T. Nakagawa is with Kansai Electric Power Company, Inc., Amagasaki 6610974, Japan (e-mail: K439570@kepco.co.jp).
T. Nakiri is with Kansai Tech Company, Inc., Osaka 552-0013, Japan (e-mail:
nakiri@aioros.ocn.ne.jp).
R. Hosoya was with the Department of Polymer Science and Engineering,
Yamagata University, Yamagata 992-8510, Japan. He is now with The Ministry
of Justice, Japan.
Y. Tajitsu is with the Graduate School of Engineering, Kansai University,
Osaka 564-8680, Japan (e-mail: tajitsu@ipcku.kansai-u.ac.jp).
Digital Object Identifier 10.1109/TIA.2004.830751

Fig. 1. Structural formula of PLA. Two optical isomers exist in PLA: one is
PLLA and the other is PDLA.

an orthorhombic-base-centered unit cell that contains two 10/3

helical chains arranged along the axis, as shown in Fig. 1
[3]. The point group of the PLLA crystal is
[3]. We have
investigated the optical properties of PLLA due to its chiral
structure for the application of this material in optical devices
[4][6]. In this study, in order to apply PLLA as an insulating

0093-9994/04$20.00 2004 IEEE

NAKAGAWA et al.: ELECTRICAL PROPERTIES OF BIODEGRADABLE POLYLACTIC ACID FILM

1021

material, for example, in electric wires and cables, we studied

its basic electrical insulation characteristics, such as volume
resistivity, dielectric constant, dielectric loss tangent, impulse
breakdown strength, and storage of space charge at room
temperature. Crosslinked polyethylene (XLPE) is used as the
reference sample.
II. SAMPLE (BIODEGRADABILITY)
PLLA is a crystalline polymer. Generally, PLLA is an extremely large molecular aggregate of chains whose individual
units are covalently bound to each other. It has a complex
higher ordered structure with intermingled crystalline and
amorphous regions. However, it is possible to control the
degree of crystallinity of PLLA as a result of progress in
research on the crystal growth of PLLA. On the other hand,
PLLA biodegradability is strongly dependent on its fixed and
surface structures [1], [2]. At present, research on the structure
and function of degrading enzymes is widely advancing. We
have prepared several types of PLLA film samples, such as
those with degrees of crystallinity higher than 50% (c-PLLA)
and lower than 10% (a-PLLA). The degradation characteristic
of PLLA strongly depends on its higher order structure [1], [2].
Also, in the local environment, the biodegradation process of
PLLA, as well as that of other biodegradable polyester, occurs
in two stages [1], [2]. In the first step, the depolymerization
of PLLA occurs. With this depolymerization, biopolyester-degrading microorganisms can proceed with their metabolic
processes using their enzyme activity. In the second step, the
depolymerized PLLA is resolved into carbon dioxide and water
by an enzyme produced by microorganisms in soil. Following
this, depolymerization progresses by nonenzymatic hydrolysis
or photolysis. However, the abiotic decomposition in the second
step is not by nonenzymatic hydrolysis or photolysis. It is clear
that the decomposition in the second step progresses with the
involvement of microorganisms. In this study, the biodegradability of the PLLA samples used in the insulation examined
was tested using fertile soil from a field in Yamagata City,
Japan, in which microorganisms grow well. The biodegradation
process of the film was influenced by the sample thickness.
We use a PLLA film with a thickness of 20 m. Every five
days, the biodegradation process of the PLLA film sample
was observed using a polarizing microscope (POM). During
this experimental period, we maintained at a temperature of
30 C and humidity of 50%. The POM image of the c-PLLA
film sample used here, in which the spherulite structure had
developed, is shown in Fig. 2. The decomposition of c-PLLA
was induced. We were able to confirm that the decomposition
of this sample occurred after 80 days. However, the sample
was still not completely decomposed after 120 days. The
POM photograph of the PLLA sample after 80 days is shown
in Fig. 3. In the central and concentric circular parts of the
spherulite, it is evident that decomposition had been initiated.
The spherulite structure of the polymer has been investigated in
detail [7]. It was found that the boundary of the lamellar crystal
which forms spherulite is amorphous, and increases in extent
in the central part of the spherulite [7]. That is, it is evident in
Fig. 3 that decomposition is promoted in the amorphous region.

Fig. 2.

Polarizing microscope image of spherulites grown in PLLA (c-PLLA).

Fig. 3. Polarizing microscope image of PLLA with spherulite structure

(c-PLLA) under the biodegradation conditions for 80 days.

These results coincide with those in previous reports where

decomposition begins between the crystalline and amorphous
regions [1], [2].
III. ELECTRICAL PROPERTIES
To investigate the insulation characteristics of PLLA, we
measured its electrical tree degradation, volume resistivity,
dielectric constant, dielectric loss tangent, and impulse breakdown strength at room temperature.
A. Electrical Tree Degradation
The sample for electrical tree degradation experiments is a
rectangular prism with a base of 20 mm
4 mm and a length
of 25 mm [8], as shown in Fig. 4. The rectangular prism sample
was fabricated by the injection molding method. Namely, the
PLLA resins were extruded in the die, at 160 C, in which the
needle was put in the fixed position, about 20 mm from the base
of the rectangular prism sample, as shown in Fig. 4. The radius
of curvature of the needle point was 3 m. The base of the rectangular prism of the PLLA sample is earthed. The dc voltage
was applied to the sample during 10 min in dry Ar atmosphere
at 20 C. If the tree is not observed by CCD camera, the applied dc voltage was increased. In the PLLA sample, an elec-

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TABLE I
ELECTRICAL PROPERTIES

Fig. 4. Schematic diagram of sample cell used for electrical treeing

measurements. (Sample dimensions: 4 20 25 mm ).

2 2

Fig. 6. Schematic diagram of sample cell used for dielectric breakdown

measurements.

Fig. 5.

Enlargement of front region of electrical tree in c-PLLA.

trical tree was generated when a voltage of 6.5 kV was applied

to the needle. The branch curls like a thread chip without extending linearly. The electrical tree was about 80 m long. This
phenomenon is shown in Fig. 5. The branch does not elongate
from 6.5 to 10 kV. In comparison with these PLLA experimental
results, under the same experimental conditions, the branch of
the electrical tree in XLPE was generated at 4 kV and greatly
elongates in the needle at 6 kV. The electrical tree in XLPE is
needlelike or ramiform. The electrical tree grew to a length of
about 200 m when a voltage of 8 kV was applied. However,
the electrical tree experiment was greatly influenced by experimental conditions [8]. Therefore, it is not possible to compare
the experimental results obtained here. In the future, many experiments will be necessary to draw a conclusion.
B. Volume Resistivity, Dielectric Constant, and Dielectric
Loss Tangent
We measured the complex permittivity and conductivity of
the PLLA and XLPE film samples in the frequency range from
10 mHz to 10 MHz, using a nonlinear conductivity measurement system developed by us [9]. The measurements are carried
out in dry Ar atmosphere at 20 C. The complex permittivity
of PLLA is almost independent of frequency in the range from

10 mHz to 10 MHZ. Therefore, in this study, we pick up the

data of dielectric constant and dielectric loss tangent at 50 Hz.
The volume resistivity, dielectric constant, and dielectric loss
tangent obtained from the results are shown in Table I. The results of the XLPE measured as reference are also summarized
in Table I. The volume resistivity and dielectric loss tangent of
PLLA are almost equal to those of XLPE. The dielectric constant of PLLA is larger than that of XLPE. One of the reasons for
this may be that the polymer chain of PLLA contains a carbonyl
group. The dielectric constant of polyvinyl chloride (PVC) currently used for insulating electric wires is 3.4 [7], [10], and the
dielectric constant of oil-immersed insulating paper used for insulating high-electrical-field cables is about 3.5 [7], [10]. The
dielectric constant of a-PLLA is smaller than those values.
C. Impulse Breakdown Strength
The thickness of the film sample used for the impulse breakdown strength experiments [8] is 250 m. Using the film samples, we produced a tube element system using a spherical electrode. We ensured that the electrode contact with the film sample
was complete, as shown in Fig. 6. The experimental system must
be isolated from the external environment. Therefore, we enclosed the spherical electrode and film sample with epoxy resin
in an acrylic pipe. Then, to prevent creeping discharge, the tube
element system was placed in an oil bath, as shown in Fig. 7.
The outline of the measurement method is as follows [8]. The
impulse voltage with a rising time of 1 s and an attenuation
time up to one-half of 40 s is applied to the sample. Equal
impulse voltages were applied three times. Simultaneously, the
current waveform is observed using an oscilloscope. It is determined that the sample was destroyed when current flowed in the
sample. The applied impulse voltage increased when current did

NAKAGAWA et al.: ELECTRICAL PROPERTIES OF BIODEGRADABLE POLYLACTIC ACID FILM

1023

Fig. 9. Setup for space charge measurement.

Fig. 7.

Fig. 10.

Space charge profile of XLPE.

Fig. 11.

Space charge profile of a-PLLA.

Experimental system for measuring impulse breakdown strength.

Fig. 8. Impulse breakdown strengths of PLLA and XLPE.

not flow in the sample. The result is shown in Fig. 8. The impulse breakdown strength of PLLA is 1.3 times that of XLPE.
D. Storage of Space Charge
We measured the storage of space charge in XLPE and PLLA
using the pulsed electroacoustic method [11], with dc electric
field applied to the sample. The samples used here are 250 m
thick. Au was deposited on the sample as electrode. Fig. 9 shows
the schematic diagram of the measurement system for space
charge in the polymer film. The applied dc voltage is 5 kV for
10 min. The pulse voltage is 750 V. The space charge measurement was carried out in dry Ar atmosphere at 20 C. The
results are shown in Figs. 10 and 11. In XLPE, as shown in
Fig. 10, it was found that homocharge mainly accumulates in the

neighborhood of the anode after electric charging. Although homocharge accumulates similarly in PLLA, as shown in Fig. 11,
in the neighborhood of the anode, the amount of accumulation is
less than that in XLPE. The electric charge induced in the anode
of PLLA is compared with that induced in the anode of XLPE,
with the electrode grounded after the applied field is switched
off. At this time, the electric charge of PLLA is about 60% that
of XLPE. The pioneering work on the storage of space charge
in XLPE was performed by Takada et al. [12]. On the basis of
their results [12], it seems evident that a large homocharge accumulates in XLPE because the nonreactive residue in it is eliminated [12]. However, because such promising research on PLLA
has only recently begun, the nature of its future direction is unknown. Thorough and careful consideration should be given to
these phenomena.

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IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS, VOL. 40, NO. 4, JULY/AUGUST 2004

IV. SUMMARY

Takashi Nakagawa was born in Kyoto, Japan, in

1971.
In 1991, he joined Kansai Electric Power Company, Inc., Amagasaki, Japan, where he has been
engaged in the design of underground transmission
lines and research on space charge characteristics
of high-voltage power cables. Currently, he is an
Engineer in the Electric Power Service Engineering
Office.
Mr. Nakagawa is a Member of the Institute of Electrical Engineers of Japan.

The basic electrical insulation characteristics of PLLA

were investigated. In this study, XLPE was used as the reference sample, and the following results were obtained. The
biodegradability of the PLLA sample as an environmentally
friendly material was observed. The volume resistivity, dielectric constant, and dielectric loss tangent of PLLA were found
to be almost the same as those of XLPE. However, the impulse
breakdown strength of PLLA was 1.3 times that of XLPE. The
amount of space charge accumulation in PLLA was one-half
that in XLPE, when dc voltage was applied for a short time.
We know that it will still take a while before practical applications of PLLA to electrical cables and wires can be realized.
We must examine many characteristics, for example, chemical
and thermal properties, to determine the influence of those on
the environment. In the next step, we plan to examine the mechanical properties of PLLA. In the future, we desire to obtain
excellent results for the PLLA sample and hope to realize the
practical applications of PLLA.
ACKNOWLEDGMENT

Takou Nakiri was born in Ube, Japan, in 1946. He

is currently working toward the D.Sc. degree in the
Graduate School of Engineering, Kansai University,
Osaka, Japan.
In 1967, he joined Kansai Electric Power Company, Inc., where he has been engaged in the design
of underground transmission lines and development
of power cables. Since 2000, he has been a Senior Research Engineer with the Engineering Center, Kansai
Tech Company, Inc., Osaka, Japan.
Mr. Nakiri is a Member of the Institute of Electrical
Engineers of Japan.

The authors are grateful to Prof. E. Fukada of the Kobayashi

Institute of Physical Research and Prof. Y. Sekii of the Chiba
Institute of Technology for useful comments.
REFERENCES
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optical properties of polylactic acids, J. Appl. Phys., vol. 77, pp.
29572973, 1995.
[4] Y. Tajitsu, Y. Shikinami, M. Date, and E. Fukada, Huge optical rotatory
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Lett., vol. 18, pp. 17851788, 1999.
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by biode-gradatic poly-L-lactic acid film, J. Mater. Sci. Lett., vol. 19,
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[6] Y. Tajitsu, Optical rotatory power and light modulation by polylactic
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Applied Science, 1998, pp. 195238.
[8] IEEE Trans. Dielect. Elect. Insulation (Special Issue on Progress in Understanding Treeing Phenomena), vol. 5, Oct. 1998.
[9] Y. Tajitsu, Nonlinear ionic-conductivity spectra of antistatic polymer
films, J. Electrostat., vol. 55, pp. 299310, 2002.
[10] A. Chelkowski, Dielectric Physics. New York: Elsevier, 1980.
[11] T. Maeno, T. Funai, H. Kushibe, T. Takada, and E. Cookie, Measurement of spatial charge distribution in thick dielectrics using the pulsed
electroacoustic method, IEEE Trans. Dielec. Elect. Insulation, vol. 23,
pp. 433439, June 1988.
[12] Y. Li, M. Yasuda, and T. Takada, Influence of crosslinking agent
residues on space charge distribution in XLPE, IEEJ Trans. Fundam.
Mater., vol. 112-A, pp. 209214, 1992.

Ryuichi Hosoya was born in Yamagata, Japan, in

1974. He received the B.Eng. and M.Eng. degrees
from the Department of Materials Science and Engineering, Yamagata University, Yamagata, Japan, in
1998 and 2000, respectively.
In 2004, he joined The Ministry of Justice, Japan.

Yoshiro Tajitsu (M03) was born in Tokyo, Japan, in

1955. He received the B.Eng. and D.Sc. degrees from
the Department of Applied Physics, Waseda University, Tokyo, Japan, in 1978 and 1988, respectively.
He was a Research Member in the Central Laboratory of Asahi-Dow Company Ltd, a Visiting Researcher in the Biopolymer Physics Laboratory, Institute of Physical and Chemical Research (RIKEN),
Saitama, Japan, from 1983 to 1995, and an Associate
Professor at Yamagata University, Yamagata, Japan,
from 1995 to 2004. Since 2004, he has been a Professor at Kansai University, Osaka, Japan. His current interests are piezoelectricity and ferroelectricity in polymers and their applications.
Prof. Tajitsu is a Member of the Materials Research Society, USA, Society
of Polymer Science, Japan, Japanese Society of Applied Physics, and Institute
of Electrical Engineers of Japan. He has received Scientific Awards from the
Institute of Electrostatics, Japan.