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510 J. Liu et al.

: Dielectric Frequency Response of Oil-paper Composite Insulation Modified by Nanoparticles


1070-9878/12/$25.00 2012 IEEE
Dielectric Frequency Response of Oil-paper Composite
Insulation Modified by Nanoparticles
Jun Liu, Lijun Zhou, Guangning Wu, Yingfeng Zhao

College of Electrical Engineering, Southwest Jiaotong University
No.111. Sec.1, North Erhuan Road
Chengdu, Sichuan, 610031, China
Ping Liu and Qian Peng
Electrical Test and Research Institute of Sichuan Province
No.24, Qinghua Road
Chengdu, Sichuan, 610072, China
ABSTRACT
The research on dielectric frequency response of oil-paper composite insulation modified
by nanoparticles has been carried out in order to seek possible way to improve insulation
properties thereof. Before and after nanoparticles being added, the dielectric frequency
responses of oil-paper composite insulation with different moisture contents at different
temperatures have been measured within the frequency from 0.1 mHz to 1 MHz. The
Cole-Cole relaxation model has been used to analyzing the measured data. The results
show that the variation rules of insulation condition can be indicated by the parameters of
relaxation model. By adding nanoparticles, a new low frequency relaxation appeared.
Index Terms Dielectric frequency response, oil-paper composite insulation,
Cole-Cole model, nanoparticles modification, complex dielectric coefficient.

1 INTRODUCTION
OIL filled transformers are widely used in extra high voltage
and ultra high voltage power transmission systems. Thus the
oil-paper composite insulation condition will seriously affect the
electrical life of transformer insulation [1-2]. With increasing
transmission voltage level, it is more difficult for the traditional
oil-paper composite insulation to meet the demands of small
size, high tolerance to field strength, and high reliability. The
emergence of nanotechnology leads to the development of
composite materials into a new era. Much research has been
carried out recently incorporating various nanoparticles into
existing solid dielectric systems [3-4]. It showed that their
breakdown characteristics, interfacial properties, space charge,
partial discharge, etc. have been improved [5-6]. The early
research of nanofluids focused on their excellent cooling
features, for example, nanoparticles were added into the
transformer oil to form colloid for enhancing the cooling effect
of the transformer windings [7]. The research on breakdown
characteristics of transformer oil modified by nanoparticles
under ac, dc and lighting voltages has shown that the addition of
nanoparticles plays an important role in improving its aging and
damage performance [8-9]. Nanoparticles modifying
technology provides a new effective way to improve the
performance of oil-paper insulation system. However, the
dielectric response of nanoparticles modified oil-paper
composite insulation has not been reported yet.
Dielectric response method as a new technique of
insulation diagnosis was presented at the commencement of
the 1980s. Time-domain dielectric response methods such as
return voltage measurements (RVM), polarization and
depolarization current (PDC) measurements emerged
successively [10-11]. Frequency domain spectroscopy (FDS)
measurements were introduced for diagnosis of transformer
insulations in the late 1990s [12-16]. The relationship
between the transformer insulation condition and dielectric
response was researched by Saha using return voltage
measurement [13]. Gubanski applied the frequency response
method to diagnose moisture in transformer insulation
[17-20]. In this paper, the dielectric frequency responses of
oil-paper composite insulation with different moisture
contents at different temperatures have been measured before
and after nanoparticles being added within the frequency
range from 0.1 mHz to 1 MHz. The Cole-Cole relaxation
model has been used to analyze the measured results.
Parameters of the Cole-Cole relaxation model were obtained
by a least squares fitting. The influence of nanoparticles
addition on the relaxation parameters is discussed.
2 EXPERIMENTAL SETUP
The TiO
2
-oil nanofluids were prepared by solvothermal
[21]. The oil used in experimental was new pure DB-#25
transformer oil produced in Kelamayi (moisture content is
8 ppm), which is applied in the ultra high voltage Manuscript received on 28 July 2011, in final form 12 December 2011.
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 19, No. 2; April 2012 511
transformer about 1000 kV. The steps of the nanoparticles
synthesis are as follows:
1) The analytical reagent oleic acid (12.5 ml), triethylamine
(10 ml) and cyclohexane (50 ml) were filtered and dried. They
were mixed and stirred 10 min by constant temperature
heating magnetic stirrer (DF-101S, made by the Shanxi
Taikang Biological Technology Co., Ltd. in China) at 25 C.
2) 2.5 ml tetrabutyl titanate was added dropwise into the
mixture by burette. The rate was about 0.5 ml/s. After being
stirred for 30 min at 25 C, they were moved into the pressure
vessel. The reaction was kept at 150 C for 48 h.
3) When the solution cooled to room temperature, the
transparent TiO
2
cyclohexane sol was formed, which
precipitated after adding excess ethanol. The precipitate was
centrifuge washed three times by 300 ml ethanol to neutral (PH
7). The semi-dried cake was obtained after filtration.
4) The precipitates obtained from the above procedure were
centrifuged four times (at 5000 rpm for 3-min intervals). Then
it was ground to pale yellow powder by mortar manually.
5) The powder was calcined in muffle furnace for 2 h at 700
K. The white TiO
2
nanoparticles were formatted. Average
particle size is about 25 nm. The crystal structure and type is
the rutile. The SEM micrographs of the TiO
2
powders were
shown in Figure 1.



Figure 1. SEM micrographs of TiO
2
for 210
5
times zoom in. The scale
is 50 nm.

6) Appropriate amount of TiO
2
powder was added to
the transformer oil. The concentration of nanoparticles in
the oil was controlled about 0.3 g/l. The bulk density of
TiO
2
is 0.48 g/cm
3
, the estimate of the volume fraction
would be about 0.06%. In order to avoid agglomerate, the
ultrasonic dispersion instrument (FS-450, made by
Shanghai Sonxi ultrasonic equipment company in China)
was used to disperse the nanoparticles evenly throughout
the oil. The TiO
2
-oil nanofluids were transparent. The
dispersed phase particles cannot be observed with the
unaided eye. For observed the dispersion of nanoparticles
in the oil, the test paper was immersed horizontally in the
nanofluids and then taken out for TEM analysis. The
result was shown in Figure 2. Although the nanoparticles
had a little agglomeration, they were also in the
nanometer level.



Figure 2. TEM photo of oil with TiO
2
nanoparticles for 210
5
times
zoom in. The scale is 50 nm.

The pressboard samples used for the measurements were
discs with thickness of 1 mm and diameter of 55 mm. The
weight of the dried paper was 2.36 g. The diameter of the
electrodes was 50 mm. The oil used for impregnation was
1970 ml. The preparation of oil impregnated papers
included the following steps: paper drying, paper
moisturizing, impregnating with transformer oil. First, the
papers were dried at 80 C in a thermal-vacuum chamber
for 2-3 days. During this process, their weights were
monitored using the precision scale EP114C, made by
OHAUS in America, for identifying whether they became
dried out. After drying, the papers were kept in an open
atmosphere for absorbing moisture from the air. Weights of
the papers were again monitored to obtain predefined levels
of moisture intakes. The papers were put into containers
filled with virgin and nanoparticles modified transformer
oil for impregnation. Five groups of samples were prepared
with moisture concentrations of 0.5, 1, 2, 3 and 4%.
The first group of samples was used to measure frequency
response of oil-paper composite insulation with different
moisture contents. The papers with 0.5, 1, 2, 3 and 4%
moisture contents were immersed in pure virgin transformer
oil and TiO
2
nanoparticles modified transformer oil. They
were sealed and placed in the oven at 50 C for two weeks, so
that the moisture diffusion in oil-paper composite insulation
achieved steady state. Moisture contents in oil and paper
before measurement are shown in Table 1. Take the paper with
3% moisture contents as an example. Before equilibrium, the
moisture from that in the paper is about 0.07299g
(0.07299/(2.36+0.07299)=3%). The moisture from that in the
oil is about 810
-6
1970 ml0.87 g/ml=0.01371 g. The all
moisture is about 0.0867 g. After equilibrium, the moisture
from that in the paper is about 0.050623 g
(0.050623/(2.36+0.050623)=2.1%). The moisture from that in
the oil is about 21.510
-6
1970 ml0.87 g/ml= 0.036848
g. The all moisture is about 0.0874 g. Considering the test
error, the moisture gets balances before and after equilibrium.
512 J. Liu et al.: Dielectric Frequency Response of Oil-paper Composite Insulation Modified by Nanoparticles
Table 1. Moisture contents of oil-paper composite insulation before
dielectric frequency response measurement at 50 C.
Moisture contents
before equilibrium
Moisture contents
after equilibrium
In paper (%) In oil (ppm) Sum (g) In paper (%) In oil (ppm) Sum (g)
0.5 8 0.026 0.7 5.3 0.026
1 8 0.037 1.0 8.0 0.037
2 8 0.062 1.5 14.6 0.061
3 8 0.087 2.1 21.5 0.087
4 8 0.112 2.3 32.1 0.110

The second group of samples was used for measuring
frequency response of oil-paper composite insulation at
different temperatures. The 2% moisture intakes samples were
immersed in pure new transformer oil and TiO
2
nanoparticles
modified transformer oil. Then they were placed in sealed
oven set the temperature about 10, 30, 50 and 70 C for two
weeks. After the moisture diffusion reached steady state, the
moisture contents in oil and paper were shown in Table 2.

Table 2. Moisture contents of oil-paper composite insulation before
dielectric frequency response measurement at different temperature
Moisture contents
before equilibrium
In paper (%) In oil (ppm) Sum (g)
2 8 0.062
Moisture contents
after equilibrium
In paper (%) In oil (ppm) Sum (g)
10 C 2.4 2.3 0.062
30 C 2.2 5.0 0.062
50 C 1.5 14.6 0.061
70 C 1.0 22.3 0.062


(a) Principle of test system


(b) Setup used for experiment

Figure 3. Setup of the test system.
The following text used the moisture contents of about 0.5, 1,
2, 3 and 4% which refer to the samples based on their nominal
moisture concentration before equilibration. The measurement
setup was designed as Figure 3. The tested papers were placed
between the voltage electrode and measuring electrode. The
oven was used to control the temperature. In order to eliminate
edge effects, a guard electrode was employed. The dielectric
frequency response of oil-paper from 10
-4
Hz to 10
4
Hz were
tested by the frequency domain insulation diagnostic analyzer
IDAX300 manufactured by Megger Group Limited. The
applied effective voltage was 140 V. The dielectric responses in
higher frequency range about 10
4
to 10
6
Hz was performed by
the LCR testers HIOKI 3532-50. The applied effective voltage
was 5 V.
3 MEASUREMENT RESULTS
3.1 DIELECTRIC FREQUENCY RESPONSES OF
OIL-PAPER COMPOSITE INSULATION WITH
DIFFERENT MOISTURE CONCENTRATIONS
The dielectric frequency response of the oil-paper
composite insulation with the moisture contents about 0.5,
1, 2, 3 and 4% have been measured at 50 C. The results
are shown in Figure 4.

10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3
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i
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Frequency (Hz)


'
0.7% moisture content
1% moisture content
1.5% moisture content
2.1% moisture content
2.3% moisture content

(a) Real part of permittivity

10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
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Frequency (Hz)


"
0.7% moisture content
1% moisture content
1.5% moisture content
2.1% moisture content
2.3% moisture content

(b) Imaginary part of permittivity

Figure 4. Dielectric frequency response of oil-paper with different
moisture contents.
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 19, No. 2; April 2012 513
At 50 C, with the moisture content increasing, complex
permittivity of oil-paper composite insulation increases
significantly at low frequency. However, they tend to be
constant at high frequency. Above 10 kHz, the imaginary parts
are rising with increasing frequency, which indicates a presence
of another loss peak at high frequencies. That is different from
the typical dielectric relaxation model equation (e.g., Debye
equation, Cole-Cole arc equation, Davidsion-Cole asymmetric
arc equation). Consequently, the Cole-Cole expression with two
relaxation times was used to fit them. The corresponding real
part of permittivity could be written as [20, 22-23]:
1 2
'
1 2
(1 ) (1 )
1 2
Re
1 ( ) 1 ( )
n
A
j j
o o
c c e
c c
et et


= + +
( A A
+
(
+ +

(1)
The imaginary part of complex permittivity is equal to
the Kramers-Kronig(K-K) transformation of formula (1)
plus the dc loss [19, 20].
1 2
" dc
0
1 2
(1 ) (1 )
1 2
cot (1 )
2
Im
1 ( ) 1 ( )
n
A n
j j
o o
o t
c e
c e
c c
et et


(
= + +
(

( A A
+
(
+ +

(2)
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2


Measured
Fitted
Frequency (Hz)
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l

P
a
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t

o
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P
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v
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c

'

(a) Measured and fitted real part of permittivity

10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
Frequency (Hz)
Measured
Fitted
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P
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o
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c

"

(b) Measured and fitted imaginary part of permittivity

Figure 5. Measured and fitted complex permittivity of oil-paper with
2% moisture content at 50 C
The parameters A, n,
1
,
2
,
1
,
2
,
1
,
2
,
dc
were used to
describe the different contributions to dielectric response. Figure
5 is the measured and fitted complex permittivity of oil-paper
composite insulation with 2% moisture content at 50 C. There
are two relaxations at high frequency and low frequency,
respectively. The
dc
give much contribution at the low
frequency range. The decrease part of permittivity with the
increasing frequency at low frequency range was modeled by an
inverse power dependence on frequency, A
-n
, whereas the
remaining part was modeled by Cole-Cole expression [20] with
two relaxation times. The 1/2
1
,
1
, 1-
1
represent the
relaxation center frequency, the relaxation amplitude and the
slope of the first Cole-Cole relaxation in the low frequency
range, respectively. Its center frequency is about 10
-2
-10
2
Hz. So
do the
2
,
2
,
2
to the second Cole-Cole relaxation in the high
frequency range, which is mainly contribute to the increase part
of permittivity after the minimum. Its center frequency is upper
than 10
9
Hz. The parameters consequently estimated by means
of the least square technique to obtain the best fit of the
measured permittivity. A good agreement between the
measured data and fitted response based on Cole-Cole
expression with two relaxation times can be observed. Fitting
the dielectric responses of oil-paper with different moisture
contents at 50 C, the results are shown in Figure 6. The
estimated parameters by the least squares for the dielectric
responses of the oil-paper samples are listed in Table 3.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3
0.7% measured
0.7% fitted
1% measured
1% fitted
1.5% measured
1.5% fitted
2.1% measured
2.1% fitted
2.3% measured
2.3% fitted
R
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P
a
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o
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i
v
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c

'

(a) Measured and fitted real part of permittivity
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
0.7% measured
0.7% fitted
1% measured
1% fitted
1.5% measured
1.5% fitted
2.1% measured
2.1% fitted
2.3% measured
2.3% fitted
I
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P
a
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Frequency (Hz)
c

"

(b) Measured and fitted imaginary part of permittivity
Figure 6. Measured and fitted complex permittivity of oil-paper with
different moisture contents at 50 C.
Frequency (Hz)
514 J. Liu et al.: Dielectric Frequency Response of Oil-paper Composite Insulation Modified by Nanoparticles
Table 3. Estimated Cole-Cole model parameters of oil-paper with
different moisture content at 50 C.
Parameters
Oil-paper with different moisture content at 50 C
0.5% 1% 2% 3% 4%
A 0.24 0.068 0.8 1.88 0.628
n 0.55 0.68 0.48 0.62 0.785

1
0.6 1.8 0.11 0.1 14.9

1
24 28 18 0.00318 0.8

1
0.96 0.42 0.735 0.8 0.5

2
3.6 3.5 4.2 4.4 4.6

2
2.510
-12
2.610
-12
3.310
-12
7.110
-12
1.910
-11

2
0.68 0.75 0.757 0.77 0.73

dc
8.510
-14
3.210
-13
3.310
-12
7.110
-12
1.210
-11

Similarly, dielectric frequency response of oil-paper
composite insulation modified by nanoparticles with
different moisture contents about 0.5, 1, 2%, 3 and 4% have
been measured at 50 C. The results are shown in Figure 7.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3
10
4
R
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a
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o
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0.7% moisture content
1% moisture content
1.5% moisture content
2.1% moisture content
2.3% moisture content
Frequency (Hz)
c

'

(a) Real part of permittivity

10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
I
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0.7% moisture content
1% moisture content
1.5% moisture content
2.1% moisture content
2.3% moisture content
Frequency (Hz)

c

"

(b) Imaginary part of permittivity

Figure 7. Measured complex permittivity of oil-paper modified by
nanoparticles with different moisture contents at 50 C.
Comparing Figures 7 and 4, the dielectric frequency
responses of oil-paper composite insulation shows that some
changes after adding nanoparticles, especially in the low
frequency. The measured data was fitted by Cole-Cole
expression with two relaxation times. The result is shown in
Figure 8.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3


Measured
Fitted
Frequency (Hz)
R
e
a
l

P
a
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t

o
f

P
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i
t
t
i
v
i
t
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c

'

(a) Measured and fitted real part of permittivity
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4


Measured
Fitted
c

Frequency (Hz)
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(b) Measured and fitted imaginary part of permittivity
Figure 8. Measured and fitted complex permittivity of oil-paper
modified by nanoparticles with 2% moisture content at 50 C based on
Cole-Cole expression with two relaxation times.

There is a clear deviation when the Cole-Cole expression
with two relaxation times was used to fit the dielectric
frequency response of oil-paper composite insulation
modified by nanoparticles, especially at the low frequency.
Considering a new relaxation peak appeared below 0.01 Hz,
a low frequency relaxation was added to fit the result. The
real part of complex permittivity based on Cole-Cole
expression with three relaxation times can be obtained:
1 2
3
'
1 2
(1 ) (1 )
1 2
3
(1 )
3
1 ( ) 1 ( )
Re
1 ( )
n
A
j j
j
o o
o
c c e
c c
et et
c
et

= + +
A A (
+ +
(
+ +
(
( A
(
+

(3)
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 19, No. 2; April 2012 515
The corresponding imaginary part of complex
permittivity is equal to the Kramers-Kronig (K-K)
transformation of formula (3) plus the dc loss.
1 2
3
" dc
0
1 2
(1 ) (1 )
1 2
3
(1 )
3
cot (1 )
2
1 ( ) 1 ( )
Im
1 ( )
n
A n
j j
j
o o
o
o t
c e
c e
c c
et et
c
et

(
= + +
(

A A (
+ +
(
+ +
(
( A
(
+

(4)
The parameters A, n,
1
,
2
,
3
,
1
,
2
,
3
,
1
,
2
,
3
,

dc
were consequently estimated by means of the least square
technique to obtain the best fit of the measured permittivity.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3
10
4

Measured
Fitted
Frequency (Hz)
R
e
a
l

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y

c

'

(a) Measured and fitted real part of permittivity
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4

c

Measured
Fitted
Frequency (Hz)

I
m
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a
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(b) Measured and fitted imaginary part of permittivity

Figure 9. Measured and fitted complex permittivity of oil-paper
modified by nanoparticles with 2% moisture content at 50 C based on
Cole-Cole expression with three relaxation times.

Figure 9 is the measured and fitted complex permittivity
of oil-paper modified by nanoparticles with 2% moisture
content at 50 C based on Cole-Cole expression with three
relaxation times. After nanoparticles adding, a new
relaxations modeled by the Cole-Cole expression was
contributing to the dielectric response. Its center frequency is
lower than 10
-4
Hz. Compared to Figure 8, the established
new relaxation model can reflect the relaxation peak
produced by nanoparticles at the low frequency band. Fitting
the dielectric responses of nanoparticles modified oil-paper
with different moisture contents at 50 C, the results are
shown in Figure 10. The estimated model parameters by the
least squares for the dielectric responses are listed in Table 4.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3
10
4
0.7% measured
0.7% fitted
1% measured
1% fitted
1.5% measured
1.5% fitted
2.1% measured
2.1% fitted
2.3% measured
2.3% fitted
Frequency (Hz)
R
e
a
l

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y


c

'

(a) Measured and fitted real part of permittivity

10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
0.7% measured
0.7% fitted
1% measured
1% fitted
1.5% measured
1.5% fitted
2.1% measured
2.1% fitted
2.3% measured
2.3% fitted
c

"
Frequency (Hz)
I
m
a
g
i
n
a
r
y

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y


(b) Measured and fitted imaginary part of permittivity

Figure 10. Measured and fitted complex permittivity of oil-paper
modified by nanoparticles with different moisture contents at 50 C.

Table 4. Estimated model parameters of oil-paper modified by
nanoparticles with different moisture contents at 50 C.
parameters
Oil-paper modified by nanoparticles with different moisture
contents at 50 C.
0.5% 1% 2% 3% 4%
A 0.038 0.09 0.122 0.1 0.19
n 0.73 0.71 0.68 0.65 0.59

1
3.45 4.52 7.13 9.12 10.9

1
935 420 200 110 92

1
0.42 0.56 0.5 0.45 0.43

2
1.8 5.9 6.2 8.1 8.8

2
2.210
-12
6.510
-12
8.710
-12
9.810
-12
1.110
-11

2
0.76 0.72 0.68 0.66 0.65

3
56 98 2023 2902 5256

3
1953 1617 978 406 218

3
0.14 0.16 0.2 0.25 0.28

dc
7.210
-14
1.210
-13
4.510
-12
8.910
-12
1.610
-11

516 J. Liu et al.: Dielectric Frequency Response of Oil-paper Composite Insulation Modified by Nanoparticles
3.2 DIELECTRIC FREQUENCY RESPONSES OF
OIL-PAPER COMPOSITE INSULATION AT
DIFFERENT TEMPERATURE
In order to study the influences of temperature on the
dielectric frequency response, the complex permittivity of
oil-paper composite insulation with 2% moisture content
has been measured at 10, 30, 50 and 70 C. According to
the Cole-Cole expression with two relaxation times, the
results were fitted. The measured data and fitting curves are
shown in Figure 11. The parameters are listed in Table 5.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10C measured
10C fitted
30C measured
30C fitted
50C measured
50C fitted
70C measured
70C fitted
R
e
a
l

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y

Frequency (Hz)


'

(a) Measured and fitted real part of permittivity
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
I
m
a
g
i
n
a
r
y

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y

10C measured
10C fitted
30C measured
30C fitted
50C measured
50C fitted
70C measured
70C fitted
Frequency (Hz)


"

(b) Measured and fitted imaginary part of permittivity
Figure 11. Measured and fitted complex permittivity of oil-paper
with 2% moisture content at different temperature

Table 5. Estimated model parameters of oil-paper with 2% moisture
content at different temperature
Parameters
Oil-paper with 2% moisture content at different temperature
10 C 30 C 50 C 70 C
A 0.073 0.11 0.8 2.5
n 0.44 0.55 0.4 0.45

1
3.9 8 0.11 1.28

1
4600 200 18 0.24

1
0.37 0.12 0.735 0.32

2
3.8 4.4 4.2 3.6

2
310
-10
4.3810
-11
3.3310
-12
1.3810
-12

2
0.75 0.74 0.757 0.7

dc
7.810
-14
4.910
-13
3.2510
-12
2.810
-11

Also, the complex permittivity of oil-paper modified by
nanoparticles with 2% moisture content has been measured
and fitted at different temperature levels of 10, 30, 50 and
70 C. The Cole-Cole expressions with three relaxation
times were established to analyzing the results. The
measured data and fitting curves are shown in Figure 12.
The parameters are listed in Table 6.
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
0
10
1
10
2
10
3
10
4
R
e
a
l

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y

10C measured
10C fitted
30C measured
30C fitted
50C measured
50C fitted
70C measured
70C fitted
Frequency (Hz)

'

(a) Measured and fitted real part of permittivity
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10C measured
10C fitted
30C measured
30C fitted
50C measured
50C fitted
70C measured
70C fitted
I
m
a
g
i
n
a
r
y

P
a
r
t

o
f

P
e
r
m
i
t
t
i
v
i
t
y

Frequency (Hz)


(b) Measured and fitted imaginary part of permittivity
Figure 12. Measured and fitted complex permittivity of oil-paper
modified by nanoparticles with 2% moisture content at different
temperature.

Table 6. Estimated model parameters of oil-paper modified by
nanoparticles with 2% moisture content at different temperature.
parameters
Oil-paper modified by nanoparticles with 2% moisture
content at different temperature
10 C 30 C 50 C 70 C
A 0.143 0.192 0.122 0.173
n 0.78 0.74 0.68 0.62

1
5.41 7.62 7.13 5.42

1
162 178 200 268

1
0.16 0.32 0.5 0.362

2
7.25 7.6 6.2 6.8

2
310
-10
1.110
-11
8.7410
-12
7.210
-12

2
0.723 0.72 0.68 0.652

3
23 243 2023 2902

3
345 425 978 4675

3
0.11 0.13 0.2 0.18

dc
1.2510
-13
8.510
-13
4.510
-12
9.710
-12

IEEE Transactions on Dielectrics and Electrical Insulation Vol. 19, No. 2; April 2012 517
4 ANALYSIS AND DISCUSSION
4.1 THE INFLUENCE OF MOISTURE AND
TEMPERATURE ON THE DIELECTRIC
FREQUENCY RESPONSE OF OIL-PAPER
COMPOSITE INSULATION
From Figures 6 and 11, an agreement between the
measured and fitted responses could be reached. Therefore,
the response of oil-paper could be represented by the
proposed fitting method. From the Tables 3 and 5, the
center frequencies of the two relaxations are 10
-2
-10
2
Hz
and 10
11
-10
12
Hz, respectively.
With the increase of moisture content, the real part of
complex permittivity of oil-paper composite insulation
increases below 10 Hz. The value of the imaginary part of
complex permittivity becomes larger. Their shapes remain
unchanged.
1
tends to increase.
2
has a slightly
increment also. The time constant
1
is highly sensitive to
the moisture content.
1
significantly decreases with the
increase of moisture content. The polarization at low
frequency moves to the high frequency direction. It can be
clearly distinguished in Figure 6. On the other hand,
increasing moisture content causes a light increment of
2
.
The polarization at high frequency slightly shifts to lower
frequency.
Figure 11 shows the dielectric response of oil-paper with
2% moisture content at different temperature. The changes
of
1
are not obvious, which represent that the
temperature has little effect on the low frequency
polarization.
2
are almost unchanged. But the time
constants
1
and
2
are very sensitive to temperature. They
all decrease with increasing temperature. The overall
responses move to the high frequency direction. Figure 11
reflects this tendency.
4.2 THE INFLUENCE OF ADDING
NANOPARTICLES ON THE DIELECTRIC
FREQUENCY OF OIL-PAPER
From Figures 10 and 12, there is a relaxation at low
frequency range. The relaxation center frequency is
corresponding to about 10
-4
Hz. Comparing with normal
oil-paper composite insulation system, the '' also increases
at the frequency range. At the same time' greatly
increases after adding nanoparticles. The
1
,
2,

1
,
2
of oil-paper composite insulation modified by nanoparticles
present the same trends with normal oil-paper. The
3
increases with the increase of temperature and moisture
content. The
3
increases with increase of temperature, the
center frequency of the low frequency relaxation shifted to
lower frequency. The
3
decreases with the increase of
moisture content, the center frequency of the low frequency
relaxation shifts to high.
The addition of metal oxide nanoparticles produces a
new polarization mechanism. It increases the real and
imaginary part of the complex permittivity of oil-paper
composite insulation. Figure 13 shows that the ac (50 Hz)
breakdown strength of the oil fluids with and without
nanoparticles, measured in accordance with IEC-156
standard, using the MJD-3 oil breakdown voltage tester
manufactured by the Zhuhai Sanchang electric appliance
company in China. Figure 14 shows that the partial
discharge inception voltage (PDIV) of oil-paper composite
insulation with and without nanoparticles. The needle and
sphere electrodes were used to test the partial discharge.
The gap is about 1 mm, which is equal to the thickness of
the oil impregnated paper. The samples were the same with
the ones be measured their dielectric responses in the
preceding text.

5 10 15 20 25 30 35
30
35
40
45
50
B
r
e
a
k
d
o
w
n

V
o
l
t
a
g
e

(
V
)
moi s t ur e c ont ent ( ppm )
nor mal oi l
nanopar t i c l s modi f i ed oi l
Figure 13. The ac (50 Hz) breakdown strength of the oil fluids with and
without nanoparticles

0. 0 0. 5 1. 0 1. 5 2. 0 2. 5 3. 0 3. 5 4. 0 4. 5
6
7
8
9
nor mal oi l - paper
nanopar t i c l s modi f i ed oi l - paper
p
a
r
t
i
a
l

d
i
s
c
h
a
r
g
e

i
n
c
e
p
t
i
o
n

v
o
l
t
a
g
e

(
V
)
moi s t ur e c ont ent i n i mpr egnat ed paper ( % )

Figure 14. The partial discharge inception voltage (PDIV) of oil-paper
composite insulation with and without nanoparticles

As Figure 13 shows that the ac breakdown voltage
decreases for both the oil with and without nanoparticles
when moisture content increases. The nanoparticles
improved withstand field strength of the oil. The
nanoparticles modified oil shows much less dependence of
electric breakdown on the moisture. Adding nanoparticles
could be responsible for alleviating the detrimental effect of
moisture on the electric breakdown. As Figure 13 shows,
the partial discharge inception voltage (PDIV) of oil-paper
518 J. Liu et al.: Dielectric Frequency Response of Oil-paper Composite Insulation Modified by Nanoparticles
with and without nanoparticles confirmed that the
nanoparticles improved withstand field strength of the
oil-paper composite insulation.
The dielectric loss tan was calculated by the formula
(3.5) in [20] the comparison of the oil-paper composite
insulation system before and after adding nanoparticles was
shown in Figure 15.
10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
0.7% Normal
0.7% Modified
1% Normal
1% Modified
1.5% Normal
1.5% Modified
2.1% Normal
2.1% Modified
2.3% Normal
2.3% Modified
t
a
n

Frequency (Hz)

(a) Dielectric loss of oil-paper with different moisture contents at 50 C
before and after modified by nanoparticles.

10
-4
10
-3
10
-2
10
-1
10
0
10
1
10
2
10
3
10
4
10
5
10
6
10
-3
10
-2
10
-1
10
0
10
1
10
2
t
a
n

Frequency (Hz)
10C Normal
10C Modified
30C Normal
30C Modified
50C Normal
50C Modified
70C Normal
70C Modified

(b) Dielectric loss of oil-paper with 2% moisture content at different
temperature before and after modified by nanoparticles

Figure 15. Comparison of oil-paper dielectric loss before and after
modified by nanoparticles.

Figure 15a shows the dielectric loss of oil-paper with
different moisture contents at 50 C before and after
modified by nanoparticles. Compare to normal oil-paper
insulation, the dielectric loss of oil-paper modified by
nanoparticles decrease below 10
-2
Hz or above 10 Hz,
while increase within the frequency range from 10
-2
Hz to
10 Hz. The moisture content do not changes this rule. As
Figure 16a, the addition of nanoparticles is propitious to
reduce the dielectric loss of the transformer which works in
the power frequency, although the moisture content
increases.
Figure 15b shows the dielectric loss of oil-paper with 2%
moisture content at different temperature before and after
modified by nanoparticles. The same rule could be
concluded comparing to Figure 15a. However, when the
temperature gets 70 C, the dielectric loss of nanoparticles
modified oil-paper insulation is more than the normal one
from 10
-2
Hz to 10
2
Hz. The high temperature makes the
adverse impact to the oil-paper insulation modified by
nanoparticles work in the power frequency, as shown in
Figure 16b.
0. 0 0. 5 1. 0 1. 5 2. 0 2. 5 3. 0 3. 5 4. 0 4. 5
0. 00
0. 02
0. 04
0. 06
0. 08
0. 10
0. 12
0. 14
moi s t ur e c ont ent ( ppm)
nor mal oi l - paper
nanopar t i c l s modi f i ed oi l - paper
t
a
n


(a) Dielectric loss of oil-paper with different moisture contents at 50 C
before and after modified by nanoparticles at 50 Hz.

10 20 30 40 50 60 70
0. 000
0. 005
0. 010
0. 015
0. 020
0. 025
0. 030
0. 035
0. 040
0. 045
0. 050
0. 055
0. 060
0. 065
nor mal oi l - paper
nanopar t i c l s modi f i ed oi l - paper
t
a
n

t emper at ur e ( C)

(b) Dielectric loss of oil-paper with 2% moisture content at different
temperature before and after modified by nanoparticles at 50 Hz

Figure 16. Comparison of oil-paper dielectric loss before and after
modified by nanoparticles at 50 Hz.
5 CONCLUSIONS
1. The relaxation function built based on Cole-Cole
expression with two relaxation times can better reflect the
relaxation process of oil-paper composite insulation and
micro-polarization mechanism of relaxation. The relaxation
parameters are related to the moisture content and
temperature.
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 19, No. 2; April 2012 519
2. By adding nanoparticles, a new low frequency
relaxation phenomena appeared. There are changes of the
dielectric frequency response of the oil-paper. The
Cole-Cole expression with three relaxation times could be
fitted.
3. The nanoparticles improved withstand field strength of
the oil. The nanoparticles modified oil shows much less
dependence of electric breakdown on the moisture. Adding
nanoparticles could be responsible for alleviating the
detrimental effect of moisture on the electric breakdown.
The partial discharge inception voltage (PDIV) of oil-paper
composite insulation with and without nanoparticles
confirmed that the nanoparticles improved withstand field
strength of the oil-paper composite insulation.
4. Comparing with the normal oil-paper, the real and
imaginary part of the complex permittivity of oil-paper
composite insulation modified by nanoparticles are
increased. The addition of nanoparticles is propitious to
reduce the dielectric loss of the transformer which works in
the power frequency, although the moisture content
increases. However, the high temperature (above 70 C)
makes the adverse impact to the oil-paper insulation
modified by nanoparticles work in the power frequency.
ACKNOWLEDGMENT
This project is supported by National Nature Science
Foundations of China (51177136, 51107105/E0705),
Sichuan youth Science and Technology Foundation
(2011JQ0009) and the Sustaining Fund of China Southern
Power Grid. The authors would like to thank Electrical Test
and Research Institute of Sichuan Province, China for their
technical support. The authors would also like to thank
Xuancheng Jingrui New Material Co., Ltd for the
nanoparticles test.
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Lijun Zhou was born in Hangzhou, China, on 8
May, 1978. He received the B.Sc., M.Sc. and
Ph.D. degrees in electrical engineering,
respectively in 2001, 2004 and 2007 from
Southwest Jiaotong University, Chengdu, where
he is a associate professor of electrical
engineering. His fields of interest are condition
monitoring, fault diagnosis and insulation
life-span evaluation for electric power equipment.
Jun Liu was born in Chengdu, China, on 17
September 1984. He received the B.Sc. degree
from the Southwest Jiaotong University,
Chengdu, China in 2006. He is currently pursuing
the Ph.D. degree in the school of Electrical
Engineering at Southwest Jiaotong University. He
is engaged in research on fault diagnosis for
electric power equipment.
520 J. Liu et al.: Dielectric Frequency Response of Oil-paper Composite Insulation Modified by Nanoparticles




























Guangning Wu M97-SM07 was born in
Nanjing, China, on 26 July, 1969. He received the
B.Sc., M.Sc. and Ph.D. degrees in electrical
engineering, from Xian Jiaotong University,
respectively in 1991, 1994 and 1997. Currently,
he is a Professor in the School of Electrical
Engineering, Southwest Jiaotong University. His
research interests include condition monitoring,
fault diagnosis and insulation life-span evaluation
for electric power equipment.
Yingfeng Zhao was born in ZhejiangChinaon
18 August 1988. He received the B.Sc. degree
from the Southwest Jiaotong University,
Chengdu, China in 2010. He is now a
postgraduate student of the College of Electrical
Engineering of the Southwest Jiaotong
University. He is engaged in research on the
on-line monitoring and fault diagnosing for
electric power equipment.
Ping Liu was born in GuanganSichuan, China,
in January 1971. He received the Master's
degree from the Chongqing University,
Chongqing, China, in 2009. He is the
superintendent of the high-voltage technology
department, Electrical Test and Research
Institute of Sichuan Province, mainly engage in
high voltage insulation equipment testing and
technical management.
Qian Peng was born in Jingzhou, Hubei, China,
on 4th February 1983. He received the Master's
degree from the Southwest Jiaotong University,
Chengdu, China in May 2009. He joined
Electrical Test and Research Institute of Sichuan
Province in 2009. He is engaged in research on
high voltage and insulation technology.

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