New Epoxy Composite Insulating Material with Nano

Fillers and Micro Fillers of Silica with Higher

Thermal Conductivity

T. Tomkov*1, L. Harvnek1, P. Trnka1, V. Mentlk1 Milan Sebok2, Miroslav Gutten2

Faculty of Electrical Engineering1 Faculty of Electrical Engineering2
University of West Bohemia in Pilsen1 University of Zilina2
Pilsen, Czech Republic1 Zilina, Slovakia2
*Email: <tomaskot@ket.zcu.cz>

Abstract This article describes the influence of thermal electrical rotating machine (e. g. thinner electrical insulation
properties of materials to properties of electrical insulating layer) and thus change the price of electric rotating machines.
systems (EIS) in electrical rotating machines. Multi-component
composite materials combine the advantage of the individual
materials, and allow generate new materials with better
properties than those of individual components (the synergistic
effect). The objective of this experiment is to improve the thermal
and electrical properties of epoxy composites using nano fillers
and micro fillers of silica 1% (SiO2 supplementing fillers of silica
with better thermal conductivity (1,5 (Wm1K1)) to the
electrical insulating systems with typical values of thermal
conductivity = 0,2 (Wm1K1) can be modified (to increase) of
its thermal conductivity [1], [7]. The electrical insulating systems
consists of glass cloth ( = 0,6 1,2 (Wm1K1)), an epoxy resin
(binder) ( = 0,2 (Wm1K1)) and a standard mica paper ( = 0,3
Fig. 1. Part of stator with indirectly-cooled bars turbo generator
0,6 (Wm1K1)) [1], [18]. Fillers with low thermal conductivity
form a barrier to the flow path of heat from the beginning (from
winding) in the electrical device to the cooling medium. Thermal flow Q (W) is connected to a temperature gradient
Furthermore, this article describes the electrical properties of T1 T2 (K) through similar law as the Ohms law.
nanocomposites based on epoxy resin filled of nano particles of T1 T2
hydrophobic and hydrophilic silica (1%). Q= (1)
RT
Keywords electrical insulation system; composite; epoxy resin;
where: RT is the thermal resistance (K/W).
hydrophilic nanosilica; hydrophobic nanosilica; dielectric
properties; thermal conductivity; dielectric properties. l l
RT = (2)
I. INTRODUCTION S
Electrical insulation systems (EIS) turbogenerators are where: is the thermal conductivity (Wm1K1), S is the
based on mica-glass fabric tapes with epoxy resin impregnation surface (m2), l is the length (m).
by vacuum pressure impregnation, or pre-impregnated resin-
rich mica glass fabric tapes, for example the part of stator with Q (3)
=
indirectly-cooled bars turbo generator, see Figure 1. Multi- S t (T1 T2 )
component composite materials combine the benefits of the
individual components, and allow generate materials with where: S is the surface (m2), t is the time (s), T is the
better properties than those of individual components. Epoxy temperature (K).
resin is a polymer in general used in EIS, but epoxy resin has a The heat losses generated in the winding of turbo
low thermal conductivity. generators with indirect cooling (the steel sheets of the stator
In the event that it found electrical insulating materials with are cooled by, such as air or hydrogen gas) is transferred pass
higher value of thermal conductivity, thermal resistance (2) through the main electroinsulation systems to the cooling
will decrease and thus it would be possible to increase medium. The electrical insulation system as a thermal barrier
utilization of machine, alternatively encumber of rotating (for example the material Relanex 45,033A with catalog values
machine of higher values of current, reduce the size of the of = 0,2 (Wm1K1)) restricting the efficiency of the cooling
system and thus limiting the utilization of machine, the power

978-1-5090-1249-7/16/$31.002016 IEEE 89
and capacity of the turbo generators with indirect cooling as the main insulation generators, an example may be the
systems. In turbo generators with direct cooling systems the material Relanex 45,033A. The basic concept of the model was
situation compared with turbo generators with indirect cooling that epoxy resin was considered as a solid surface in which
systems is different. The heat losses generated in the winding particles of silica were introduced. The particle of silica was
(stator bars - hollow tube chilled) of turbo generators with distribution assumed random. The thermal conductivity of the
direct cooling is transferred directly to the cooling medium for fillers silica is = 1,5 (Wm1K1) [7]. The heat flux was
example water or hydrogen gas. Accordingly in turbo considered only along one direction, i.e. x-direction. One edge
generators with direct cooling the thermal conductivity of the was set at T1 (155 C = 428,15 K) and the other at T2 (40 C =
main electroinsulation systems has not substantial effect on the 313,15 K). Heat transfer by conduction takes place through the
efficiency of the cooling system. surface and it is a steady-state problem. The models are
presented in Fig. 2.
Nowadays development of new electroinsulation materials
that are used in the manufacture of electrical machine and
development of new construction methods made possible the
production of air-cooled turbo generators of up to 250 MW
compared with the past when turbo generators by 80 MW
produced with hydrogen, turbo generators from 230 MW
combined water and hydrogen. Indirectly cooled turbo
generators are increasingly used because they construction is
simpler and less expensive [1 - 6], [17], [18].
The objective of this experiment is study the thermal and
electrical properties of epoxy composites using nano fillers and
micro fillers of silica (SiO2). Fillers with low thermal
conductivity form a barrier to the flow path of heat from the
beginning (from winding) in the electrical device to the cooling
medium.
Furthermore, this paper studies the electrical insulation
properties and thermal properties of nanocomposites based on
epoxy resin filled of nanoparticles of hydrophobic and T1 T2
hydrophilic silica. Electrical insulating materials are sensitive x
to moisture, which can cause serious and sometimes
irreversible changes as deterioration of the dielectric properties. Fig. 2. Heat flux perpendicular to the x-direction
Therefore, was performed the experiment where we tried
improve and influence electrical, thermal and mechanical Additions of filler of silica, with good thermal conductivity
properties to add nanoparticles into an existing epoxy resin. to the epoxy resin increase its thermal conductivity. Electrical
But even nano filler provides the complications associated with insulation materials with low thermal conductivity form a
absorb moisture from the surroundings. The focus of the thermal barrier on the path of the heat flow (such as the stator
experiment was investigated primarily by measurement bars) from its beginning in the electrical equipment to the
dielectric properties (resistivity, dissipation factor, dielectric cooling medium.
strength, resorption curve, polarization indexes) and thermal
properties (thermal conductivity) on samples of epoxy resin B. Components
filled with two types of nanoparticles, according to the For manufacture of samples was used epoxy resin as the
humidity, it is a hydrophobic and hydrophilic silica. matrix DGEBA - Poly (Bisphenol A-co-epichlorohydrin).
Epoxy resin is used very often for manufacture of electrical
II. EXPERIMENT insulation systems for its dielectric properties, weather, thermal
and chemical resistance, high strength and excellent adhesion
The aim of thermal calculations is to define the medium
to various surfaces.
and maximum temperature rise in individual parts of electrical
machine which are in direct contact with the main electrical Furthermore, for manufacture of samples was used as
insulation of the electrical machine. With increased load in the hardener Laromin C260 - diamine crosslinker - cycloaliphatic
temperature of active parts (such as the winding), this may lead diamine - 3,3-dimethyl-4,4'diaminocyklohexyl-metan.
to increased stress of electric insulation systems, or their
destruction. The hydrophobic silica used was the product with the
manufacturing designation AEROSIL R 974, prepared by the
modification of the silica with a specific surface of 200 m2/g.
A. Simulation of the temperature field
Two dimensional models were developed with the use of The hydrophilic silica used was the product that provides
the finite element software Agros 2D in order to model the by the company Sigma - Aldrich in the form of a white powder
thermal conductivity of polymeric composites based on epoxy with a specific surface area of 175 m2/g - 225 m2/g.
resin = 0,2 (Wm1K1). Parameters of the insulating
material correspond to the typical values of the materials used

90
 The large area of fillers of silica (SiO2) can improves the
compaction of the material, as well as the transparency of the
complete system during production of samples.
Two set of samples with addition of hydrophobic nano and
hydrophobic micro filler of silica were produced. These
samples were compared with a set of sample without silicon
dioxide. Nanoparticles of hydrophobic silica (SiO2) have size
approx. 10 nm. Micro particles of hydrophobic silica (SiO2)
have size approx. 40 m 60 m.
Furthermore, were produced two set of sample
nanocomposite based on epoxy resin filled with hydrophobic
and hydrophilic silica (size approx. 10 nm).
Many research teams in many publications, improvement in
the electrical, thermal and mechanical properties of polymers in
which nano or micro particles (such as diamond, boron nitride,
aluminium nitride, aluminium oxide, silicon oxide) were
embedded, has been reported [2 - 16]. Motion of molecules
nanocomposites is limited by a specific strong link between
nanoparticles and matrix. The nanocomposites can have certain
properties which are different from microcomposite materials.
C. Thermal conductivity measurement
Fourier's laws are used for the description of heat transfer
by conduction. The first Fourier's law is used for the stationary
transfer of heat by conduction. The second Fourier's law is
used to describe the spread of heat dissipation. Heat transfer by
radiation in the large electrical equipment (such as turbo
generator) is not extensive, as conduction and convection.
Therefore with regard to accuracy of the thermal calculations it
can be neglected.
Two types of methods exist for measuring the thermal
conductivity of the sample: the steady-state and non-steady
state method. In this paper it was used the steady-state method
and were carried out according to ISO 22007-2:2015 (Plastics
Determination of thermal conductivity and thermal
diffusivity Part 2: Transient plane heat source (hot disc)
method).
The values of the thermal conductivity of produced samples
with addition of hydrophobic nano 1%, hydrophilic nano 1%
and hydrophobic micro 1% filler of silica, see in Table I
TABLE I. THE VALUES OF THE THERMAL CONDUCTIVITY
The sample tan
(Wm1K1) (-)
Pure epoxy resin 0,01
0,19
EP + 1% Microparticles hydrophobic SiO2 0,23 0,006
EP + 1% Nanoparticles hydrophobic SiO2 0,22 0,004
EP + 1% Nanoparticles hydrophilic SiO2 0,005
0,20
The values of thermal conductivity of the samples with
nanofillers of hydrophobic silica are lower compared with the
samples with the addition microparticles of hydrophobic silica
but the values of thermal conductivity of the samples with
nanofiller of hydrophobic silica are larger compared with the
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samples with the pure epoxy resin. The coefficient of thermal
conductivity of the sample with hydrophilic silica is lower
compared to the sample manufactured with hydrophobic silica
Molecular motion in nanomaterials is limited by a strong link
between nanoparticles and matrix. The nanomaterials can have
certain properties which are different from micro composite
materials. The form, amount and size of nano- or micro-
particles can affect thermal properties of the resulting material,
see Table I.
The values of tan , see in Table I, measurements values of
tan were carried out at a voltage of 500 V, frequency 50 Hz
and temperature 20 C.
D. Dielectric strength measurement
The term dielectric strength in electrical rotating machines
means that, an electrical insulating material, the maximum
electric field that a material can withstand under specific
conditions without breaking down. For a specific configuration
of dielectric material and electrodes with a diameter 6 mm
applied electric field that results in breakdown. The electrode
system with the sample was immersed in the test oil bath
because of the high values of breakdown voltage.
Dielectric strength was measured using HIGHVOLT
testing device. Dielectric strength tests were carried out
according to IEC 60243-1 (Electric strength of insulating
materials - Part 1: Tests at power frequencies).
The values of the dielectric strength of produced samples
with addition of hydrophobic nano 1%, hydrophilic nano 1%
and hydrophobic micro 1% filler of silica, see Fig. 3. The best
value of dielectric strength is shown in Fig. 3, Ep = 49,2
(kVmm1), achieves resin with microfiller.
Fig. 3. Dielectric strength on samples filled by micro fillers hydrophobic
SiO2, nano fillers hydrophobic SiO2 and nano fillers hydrophilic SiO2
At breakdown, the electric field frees bound electrons, free
electrons accelerated to velocities that can liberate additional
electrons during collisions with neutral atoms or molecules in a
process called avalanche breakdown. Breakdown occurs quite
abruptly, resulting in the formation of an electrically
conductive path and a disruptive discharge through the pure
material. The situation is more complex when heterogenic are
involved. In these cases, the values of the electrical strength
can be influenced by the size of the particles silica, see Fig. 3.
E. Volume resistivity measurement
Volume resistivity is a basic parameter of electrical
insulating systems. The measurement of volume resistivity was
carried out using cylindrical electrodes a three electrode
system. The value of the volume resistivity is evaluated based
on the measured resistance value and dimensions of the
electrodes and sample.
Measurement was implemented on DC voltage of 500 V,
power frequency 50 Hz, temperature 20 C and values were
recorded using High Voltage Supply 240 A - Keithley 610 C
Solid State Electrometer.
The measurement of volume resistivity was carried out
according to IEC 60093:1980 (Methods of Test for Volume
Resistivity and Surface Resistivity of Solid Electrical
Insulating Materials).
The values of the volume resistivity of produced samples
with addition of hydrophobic nano 1%, hydrophilic nano 1% Fig. 5 Dissipation factor on samples filled by micro fillers hydrophobic
and hydrophobic micro 1% filler of silica, see Fig. 4. Best SiO2, nano fillers hydrophobic SiO2 and nano fillers hydrophilic SiO2
value reaches epoxy resin with hydrophobic nanofillers v =
2,03 E+16 (m) in comparison with another samples, see Fig. 5 shows the dissipation factor versus temperature from
Fig. 4. 30 C to 130 C it is noticeable that epoxy resin with nano
fillers hydrophobic SiO2 has the lowest value at temperature 30
C. When increasing the temperature in samples are specific
chemical processes between nanoparticles and matrix but
samples with nano fillers hydrophobic silica have the lowest
value of the loss factor. The values of the loss factor of another
samples increase with temperature.
The highest values have a dissipation factor at 130 C (Fig.
5), which may correspond to the glass transition temperature
(Tg) of used epoxy resin [17 - 19], [23].

G. Measurement of absorption current

Fig. 4. Volume resistivity on samples filled by micro fillers hydrophobic
SiO2, nano fillers hydrophobic SiO2 and nano fillers hydrophilic SiO2
In Fig. 6 are the waveforms of the absorbent current which
leads to the conclusion that the curve of the epoxy resin
containing hydrophobic silica falls faster. This fact determines
that the resin with a hydrophobic silica is much drier than the
epoxy resin with the hydrophilic silica.

The greater the value of resistivity, the smaller conductivity

of the substance and the greater the local electrical resistance
has material. Motion of molecules nanocomposites is limited
by a specific strong link between nanoparticles and matrix
which can lead to greater value of resistivity, see Fig. 4.

F. Dissipation factor measurement

The measurement of dissipation factor was carried out on
an automatic bridge (LDV - 5 Dissipation factor and
capacitance measuring system LDIC) at voltage 500 V and
power frequency 50 Hz.
The measurement of dissipation factor was carried out
according to IEC 60250 (Recommended methods for the
determination of the permittivity and dielectric dissipation
factor of electrical insulating materials at power, audio and Fig. 6 Measurement of absorption current
radio frequency including metre wavelengths). The filler has a higher permittivity than the non-filled
The values of the dissipation factor of produced samples epoxy which may lead to increase the proportion of
with addition of hydrophobic nano 1%, hydrophilic nano 1% polarization. On what course of polarization currents decides
and hydrophobic micro 1% filler of silica, see Fig. 5. structure of dielectric, the accumulation of free charge carriers
for example interfaces inhomogeneities. At the higher
polarization material is growing dielectric losses.

92
 III. CONCLUSION
This papier describes the study of possibilities of increasing
of epoxy resin thermal conductivity, see Table I. Described is
access using micro particles of silica and nanoparticles of
silica. The samples filled micro particles of silica improve
thermal conductivity in comparison with the nanoparticles of
silica. Other features include improved dielectric strength but
the difference between micro and nano is not so noticeable. In
contrast, samples filled with nanoparticles improving volume
resistivity and dissipation factor versus temperature.
Hydrophilic particles of silica absorb water in the epoxy
resin and this has resulted in the deterioration of the active
property of the whole composite system (the sample with
hydrophilic silica). The sample with hydrophobic particles of
silica have better value of absorption current, the volume
resistivity, dielectric strength and thermal conductivity than the
sample with hydrophilic particles of silica.
On the contrary, expensiveness of nanoparticles and
tendency to agglomeration (technically difficult to avoid) still
belong to their disadvantages.
ACKNOWLEDGMENT
This work was supported by the Student Grant Agency of
the West Bohemia University in Pilsen, grant No. SGS-2015-
020 "Technological and Material Systems in Electrical
Engineering.
This research has been supported by the European Regional
Development Fund and the Ministry of Education, Youth and
Sports of the Czech Republic under the Regional Innovation
Centre for Electrical Engineering (RICE), project No.
CZ.1.05/2.1.00/03.0094
The authors would like to acknowledge Jaroslav Barto, for
his experimental support during measurement. Furthermore,
the authors would like to acknowledge Ing. Tom Dugan
Ph.D. for his help in usage of the microscope and Doc. Ing.
Pavel Karban, Ph.D. for his help with the use of the finite
element software Agros 2D.
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