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energies

Article
Breakdown Voltage and Its Influencing Factors of
Thermally Aged Oil-Impregnated Paper at Pulsating
DC Voltage
Jing Zhang 1 , Feipeng Wang 1, *, Jian Li 1, *, Hehuan Ran 1 , Xudong Li 1 and Qiang Fu 2
1 State Key Laboratory of Power Transmission Equipment & System Security and New Technology,
School of Electrical Engineering, Chongqing University, Chongqing 400044, China;
zhangjing2012@cqu.edu.cn (J.Z.); ranhehuan@cqu.edu.cn (H.R.); lixudong@cqu.edu.cn (X.L.)
2 Electric Power Research Institute of Guangdong Power Grid Co., Ltd., Guangzhou 510080, China;
13926402226@163.com
* Correspondence: fpwang@cqu.edu.cn (F.W.); lijian@cqu.edu.cn (J.L.);
Tel.: +86-23-6511-1795 (F.W.); +86-23-6510-2430 (J.L.)

Academic Editors: Akhtar Kalam and Tapas Mallick


Received: 27 July 2017; Accepted: 12 September 2017; Published: 15 September 2017

Abstract: Breakdown strength is an important electrical property of insulating paper.


Oil-impregnated paper of various aging states was prepared. Its breakdown voltage was then
measured at pulsating direct current (DC) voltage with various ripple factors, and alternating current
(AC) and DC voltage for comparison, respectively. The AC breakdown voltage is the smallest, and
pulsating DC (r = 1/5) breakdown voltage is the greatest before the paper reaches its end of life. A
dielectric model was adopted to investigate the difference in magnitude of breakdown voltage at
different voltage waveforms. Meanwhile, it was found that breakdown voltage fluctuated and even
increased occasionally during the thermal aging process, and a somewhat opposite changing tendency
versus aging time was observed for breakdown voltage at DC voltage and pulsating DC voltage with
small ripple factors (r = 1/5 and 1/3), compared with AC voltage. The degree of polymerization (DP)
and moisture content of the paper were measured, and the characteristics of the pores and cracks
of the paper were obtained to investigate the possible influencing factors of breakdown voltage at
different aging states. The results showed that the moisture content, oil absorption ability associated
with pores and cracks of paper, and the damage to paper structure all contributed to the variation
of the breakdown voltage versus aging time, while the importance of their influence differed as the
aging state of paper varied.

Keywords: breakdown voltage; pulsating DC voltage; thermal aging; double-composite dielectric


model; oil absorption ability; oil-impregnated paper

1. Introduction
Power transformers are essential to power transmission networks [1]. As the insulating medium
of power transformers, oil-impregnated paper (OIP) degrades under interaction with heat, moisture,
oxygen, and acids [2,3]. Among those aging factors, heat is the main cause of insulation aging, and
thus reduces its mechanical strength and electrical performance. Therefore, condition assessment of
OIP using its dielectric and physicochemical characteristics is essential to the safe operation, planned
maintenance, and replacement of transformers [4]. Breakdown voltage is an important property of
insulating paper, and thermal aging is the main form of OIP aging. Investigation into the breakdown
characteristics of thermally aged OIP is conducive to understanding the influencing mechanism of
aging on its insulating performance.

Energies 2017, 10, 1411; doi:10.3390/en10091411 www.mdpi.com/journal/energies


Energies 2017, 10, 1411 2 of 16

Meanwhile, as the direct current transmission system is developing rapidly, the converter
transformer has attracted much attention by researchers. The valve-side windings in a converter
transformer withstand the voltage of complex waveforms [5]. The turn-to-ground insulation of the
valve-side wingdings withstands pulsating DC voltage [5,6], also known as combined AC-DC voltage
or AC and DC combined voltages [7–10]. The breakdown characteristics of OIP at pulsating DC
voltage show many differences compared with that at AC voltage [6]. Therefore, it is necessary to
investigate the breakdown voltage of aged OIP at this type of voltage waveform.
The breakdown voltage of OIP or oil-paper insulation has been widely studied at various voltage
waveforms, including AC voltage [11,12], DC voltage [13,14], impulse voltage [12,15–18], and pulsating
DC voltage [6,19,20]. In [6], the breakdown voltage of OIP at pulsating DC voltage (with a ripple factor
of 1 and 1/3) was measured. It was found that the pulsating DC breakdown voltage lies between AC
and DC breakdown voltage when temperature varies from 60 ◦ C to 110 ◦ C. Chen et al. [20] theoretically
calculated the distribution of electric field strength for the oil-paper insulation when it was subjected
to pulsating DC voltage. Experiments showed that the breakdown voltage reaches its maximum value
when a small ratio of AC component is contained in the applied voltage, and this maximum value
shows no significant difference compared with that at individual DC voltage. The papers used were
all unaged insulating papers. There are few publications investigating the breakdown voltage of
thermally aged paper at AC voltage [12,21,22], let alone investigation into that at pulsating DC voltage.
Sun et al. [12] found the AC breakdown voltage of thermally aged OIP increases with the increased
duration of thermal aging. The increase in breakdown voltage was attributed to the emergence of
micro globules and the breakdown of the cellulose fibers, which improved the electric field distribution
in the OIP. Liao et al. [21] measured the AC breakdown strength of oil-impregnated pressboards
thermally aged in both mineral and vegetable insulating oil at 110 ◦ C. The breakdown voltage of
the pressboard fluctuates with the increase of thermal aging duration and no clear correlation with
degree of polymerization (DP) was found. Tang et al. [22] investigated the AC breakdown voltage
of thermally aged paper in both mineral and vegetable insulating oil at 90 ◦ C, 110 ◦ C, and 130 ◦ C,
and no pronounced correlation between AC breakdown voltage with the DP of the paper or thermal
aging temperature was observed. The breakdown voltage firstly exhibited a small decrease but then
increased during the thermal aging process. It remains to be seen, however, whether the breakdown
voltage of thermally aged OIP at pulsating DC voltage exhibits the same changing tendency as that at
AC voltage.
This work aims at investigating the breakdown voltage of thermally aged OIP at pulsating DC
voltage and the possible influencing factors. Firstly, the Kraft insulating paper was thermally aged
in oil at a temperature of 120 ◦ C and 130 ◦ C. Next, breakdown voltage of paper of different aging
states at pulsating DC voltage was measured. For comparison, identical experiments were carried
out at AC and DC voltage. Lastly, the difference in magnitude of breakdown voltage at those three
kinds of voltage waveforms was interpreted with the double-composite dielectric model. The moisture
content of the paper and oil absorption ability associated with the pores and cracks of the paper, and
the structural damage of the paper were adopted to explain the changing tendency of breakdown
voltage versus aging time.

2. Experiments

2.1. Accelerated Thermal Aging Experiments


OIP of different aging states were obtained through accelerated thermal aging experiments. The
naphthenic-based mineral oil Karamay 25# from Petrolchina and Kraft insulating paper from Taizhou
Xinyuan Electrical Equipment Co., Ltd., China were used to conduct the experiments. The paper has a
thickness of 0.13 mm and a diameter of 80 mm, respectively. To simulate the processing procedures
of oil-paper in an actual transformer and to control the initial state of experimental samples, the oil
and paper were separately degassed and dehydrated in a vacuum drying chamber at 50 Pa/80 ◦ C for
Energies 2017, 10, 1411 3 of 16

Energies 2017, 10, 1411 3 of 16


48 h. Then the paper went through an oil impregnation process for 48 h at 50 Pa/60 ◦ C. Thereafter,
they
of oilwere transferred
to paper beinginto a stainless
10:1 by weight. steelFigure
container, with the ratio
1 illustrates the of oil to paper
sample being 10:1
processing by weight.
procedure for
Figure 1 illustrates the sample processing procedure for accelerated thermal aging.
accelerated thermal aging. Lastly, the sealed containers were put into an oven, which was heated to Lastly, the sealed
containers
120 °C or 130were°C.putTable
into an oven,
1 lists thewhich wasaging
thermal to 120 ◦ C or and
heatedtemperatures 130 ◦corresponding
C. Table 1 listsaging
the thermal
times.
aging temperatures and corresponding aging times. The temperature
The temperature for accelerated thermal aging experiment was determined according to for accelerated thermal aging
the
experiment was determined according to the following two principles. Firstly, the
following two principles. Firstly, the temperature should not be too low (say below 90 °C), as a lowtemperature should
not be too low
temperature (say below
results 90 ◦long
in a very C), astime
a lowtotemperature
accomplish the results in a very
thermal aginglong time to accomplish
experiment. Secondly, thethe
thermal agingshould
temperature experiment.
not beSecondly,
too high,theastemperature should notmay
a high temperature be too high,the
exceed as aflash
high point
temperature
of the
may exceedoilthe
insulating flash
(say point
above 140of °C).
the insulating
Based on the oil (say
two above 140 ◦and
principles C). Based on theaging
the thermal two principles
temperaturesand
the thermal aging temperatures adopted by other researchers, 120 ◦ C and 130 ◦ C were finally chosen
adopted by other researchers, 120 °C and 130 °C were finally chosen for the thermal aging
for the thermal aging experiment.
experiment.

Figure 1. Sample processing procedure.


Figure 1. Sample processing procedure.

Table 1. Thermal aging temperature and corresponding aging time.


Table 1. Thermal aging temperature and corresponding aging time.
Thermal Aging Temperatures (°C) Aging Time (Day)
Thermal Aging Temperatures ◦
120 ( C) 2, 4, 7, 10,Aging
22, 35,Time (Day)
60, 120, 180
120 130 0.5,2,
2,4,4,7,7,10,
10,22,
22,35,
35,60,
60,120,
90 180
130 0.5, 2, 4, 7, 10, 22, 35, 60, 90
At each due time, one container was removed from the aging oven to obtain aged OIP samples
for the
Atfollowing test items:
each due time, breakdown
one container wasvoltage,
removed moisture
from thecontent, DP, nitrogen
aging oven to obtaingas adsorption
aged and
OIP samples
desorption tests, and scanning electron microscope (SEM) test. The moisture content and DP of paper
for the following test items: breakdown voltage, moisture content, DP, nitrogen gas adsorption and
were measured to see if it was strongly correlated with the variation of breakdown voltage of OIP.
desorption tests, and scanning electron microscope (SEM) test. The moisture content and DP of paper
Measurement of the moisture content of OIP was accomplished with a Karl-Fischer coulometric
were measured to see if it was strongly correlated with the variation of breakdown voltage of OIP.
titrator (Metrohm moisture meter 851 and oven 885, Herisau, Switzerland), following IEC 60814.
Measurement of the moisture content of OIP was accomplished with a Karl-Fischer coulometric titrator
Measurement of the DP of the paper was conducted according to IEC 60450. The gas adsorption and
(Metrohm moisture meter 851 and oven 885, Herisau, Switzerland), following IEC 60814. Measurement
desorption test, and SEM test were conducted to investigate the mesoporous distribution, and pores
of the DP of the paper was conducted according to IEC 60450. The gas adsorption and desorption test,
and cracks of the paper during the thermal aging process, respectively.
and SEM test were conducted to investigate the mesoporous distribution, and pores and cracks of the
paper during the thermal aging process, respectively.
2.2. Experimetnal Setup for Breakdown Voltage Test
2.2. Experimetnal Setup for
Figure 2 illustrates theBreakdown Voltage
experimental Testfor the breakdown voltage test. It consists of a power
setup
source, an oil
Figure vessel, anthe
2 illustrates electrode system,
experimental and for
setup some
the measurement instruments.
breakdown voltage The power
test. It consists of a source
power
includedana oil
source, function
vessel,generator and asystem,
an electrode high voltage power
and some amplifier (TREK
measurement 50 kV/12 The
instruments. mA).power
The function
source
generatora provides
included the required
function generator and avoltage signal,power
high voltage and the high voltage
amplifier (TREK 50 power
kV/12 amplifier
mA). Theraises the
function
voltage to the required level. An asymmetric electrode system was designed [23] to measure
generator provides the required voltage signal, and the high voltage power amplifier raises the voltage the
breakdown
to voltage
the required level.ofAn
OIP, as depicted
asymmetric in Figure
electrode 3.
system was designed [23] to measure the breakdown
voltage of OIP, as depicted in Figure 3.
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16

Figure 2.
Figure 2. The
The setup
setup of
of breakdown
breakdown voltage
voltage test
test at
at different
different voltage
voltage waveforms.
waveforms.
Figure 2. The
Figure2. The setup
setup of
of breakdown
breakdownvoltage
voltagetest
testat
atdifferent
differentvoltage
voltagewaveforms.
waveforms.

Figure 3.
Figure 3. The electrode
electrode system.
system.
Figure3.3.The
Figure Theelectrode
The electrodesystem.
system.

2.3. Breakdown
2.3. Breakdown Voltage
Voltage Test
Test
2.3. Breakdown
2.3. BreakdownVoltage
VoltageTest
Test
For OIP
For OIP ofof each
each aging
aging time,
time, breakdown
breakdown voltages voltages of of 10
10 specimens
specimens were were measured
measured to to obtain
obtain 10 10
For OIP
For OIP of ofeach
eachaging
agingtime,time, breakdown
breakdown voltages voltages of of 10
10 specimens
specimens were were measured
measured to to obtain
obtain 10 10
breakdown
breakdown voltage
voltage data
data at room
atatroom temperature.
temperature. For
For the
the convenience
convenience of description,
ofofdescription, the
the peak
peak value
value of
of
breakdown
breakdown voltage
voltage data
data atand room
room temperature.
temperature. For
For the
the convenience
convenience description,
of description, the peak
the peak value
value of
of
the
the voltage was recorded considered to be the breakdown voltage when the OIP broke down.
thevoltage
the voltagewas
voltage wasrecorded
recordedand andconsidered
consideredto tobebethethebreakdown
breakdownvoltage voltagewhenwhenthe theOIP
OIPbroke
brokedown.down.
The
The positivewas
positive
recorded
pulsating
pulsating DC
and
DC voltage considered
voltage with various
with
to
various be the
ripple
ripple
breakdown wasvoltage
factors was
factors appliedwhen
applied thethe
to the
to OIP
OIP
OIP broke
during
during the
the
down.
test,
test,
The
The positive pulsating
positive pulsating DC
DC voltage
voltage with
with various
various ripple
ripple factors was
factors was applied
appliedto the OIP during
to the OIP during the test,
the
respectively.
respectively. The
The ripple
ripple factor
factor r is the
rr isis the ratio
ratio of the
ofof the amplitude
amplitude of the
ofof the AC
AC component
component U AC to the
UUACAC toto the
respectively.
test, respectively. The ripple
The factor the
ripple factorUrDCis, the ratio
ratio the
of the amplitude
amplitude(1). the
of the AC component
AC 4component UACtypical the
to the
magnitude
magnitude of the DC component as is shown in Equation Figure illustrates the
magnitudeof ofthetheDCDCcomponent
componentU UDCDC, ,,as
asisis
isshown
shownin inEquation
Equation(1). (1).Figure
Figure444illustrates
illustratesthe thetypical
typical
magnitude
waveform
waveform for
of
for the DC
pulsating
pulsating
component
DC voltageUwith
DC voltage DC as
with shown
aaaripple
ripple factor
factor
in Equation
of
of 1. In
1. this(1).
In this work,
work,
Figure illustrates
pulsating
pulsating
the
DC voltages
DC voltages typical
with
with
waveform
waveform for
for pulsating
pulsating DC voltage
DC voltage with
with ripple factor
a ripple factor of 1. In this work,
of 1. In this pulsating
work,ofpulsatingDC voltages
DC voltages with
an
an rr of
of 1/5,
1/5, 1/3,
1/3, and
and 1
1 were
were chosen
chosen to
to investigate
investigate the
the breakdown
breakdown voltage
voltage of OIP
OIP at
at pulsating
pulsating DC
an r an
with of r1/5,
of 1/3, 1/3,
1/5, and and
1 were1 werechosen
chosen to to investigate
investigate thethe breakdown
breakdown voltage
voltage ofof OIP
OIP at
at pulsatingDC
pulsating DC
DC
voltage [5].
voltage [5].
voltage
voltage [5].[5].
U AC
r==UU
r r= UAC (1)
(1)
r =UAC AC
(1)
(1)
UU
DC
DCUDC
DC

Figure 4.
Figure 4. Typical
Typical pulsating
pulsating direct
direct current
current (DC)
(DC) voltage
voltage waveform.
Figure 4. Typical
Figure 4. Typicalpulsating
pulsatingdirect
directcurrent (DC) voltagewaveform.
current(DC) waveform.
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3. Breakdown Voltage of Thermally Aged OIP


3. Breakdown Voltage of Thermally Aged OIP
Figure 5 depicts the mean value of the breakdown voltage of OIP of different aging states with
Figure
one standard 5 depicts the In
deviation. mean value
most of the
cases, the AC
breakdown
breakdown voltage of OIP
voltage wasofthe
different aging
smallest, andstates with
pulsating
one standard deviation. In most cases, the AC breakdown voltage was the smallest,
DC (r = 1/5) breakdown voltage the greatest. No pronounced difference was found, however, in the and pulsating
DC (r = 1/5)ofbreakdown
magnitude breakdown voltage theamong
voltage greatest. No pronounced
pulsating DC voltage difference
(r = 1/5was
andfound, however,
1/3) and in the
DC voltage.
magnitude of breakdown voltage among pulsating DC voltage (r = 1/5 and 1/3) and
The standard deviation of breakdown voltage at pulsating DC and DC voltage was greater than that DC voltage. The
standard deviation of breakdown voltage at pulsating DC and DC voltage was
at AC voltage, regardless of the thermal aging time or temperature. Nevertheless, those trends greater than that at
AC voltage,
became regardless when
inconspicuous of the paper
thermal aging its
reached time
endorof
temperature.
life (taken asNevertheless,
DP = 150–200 those
[24,25]trends
in thisbecame
work),
inconspicuous when paper reached its end of life (taken as DP = 150–200 [24,25] in this
i.e., papers aged for 180 days at 120 °C and 90 days at 130 °C. In those aging states, minute differences work), i.e.,
papers aged for 180 days at 120 ◦ C and 90 days at 130 ◦ C. In those aging states, minute differences
were observed in breakdown voltage and corresponding standard deviation among the three types
were observed
of voltage in breakdown voltage and corresponding standard deviation among the three types of
waveforms.
voltage waveforms.

(a)

(b)
Figure 5. Breakdown voltage of oil-impregnated paper (OIP) after thermal aging with one standard
Figure 5. Breakdown voltage of oil-impregnated paper (OIP) after thermal aging with one standard
deviation: (a) 120 °C; (b) 130 °C.
deviation: (a) 120 ◦ C; (b) 130 ◦ C.
Energies 2017, 10, 1411 6 of 16

Energies
Figure 2017, 10, 1411
6 presents the changing tendency of breakdown voltage against aging time at 6different of 16

voltage waveforms. Before reaching its end of life, the breakdown voltage at pulsating DC voltage
Figure 6 presents the changing tendency of breakdown voltage against aging time at different
stayed in a relatively high level and did not necessarily decline. Instead, it exhibited some fluctuations
voltage waveforms. Before reaching its end of life, the breakdown voltage at pulsating DC voltage
with occasional increase versus the aging time regardless of the thermal aging temperature. The
stayed in a relatively high level and did not necessarily decline. Instead, it exhibited some fluctuations
fluctuation in breakdown
with occasional increase voltage
versusatthe individual
aging timeDC regardless
or AC voltage of thewas also observed.
thermal Nevertheless,
aging temperature.
the changing tendency
The fluctuation of breakdown
in breakdown voltage
voltage versus aging
at individual DC time
or AC at voltage
DC andwas pulsating DC voltage
also observed.
withNevertheless,
small ripplethe factors (r = 1/5 and 1/3) was opposite to the trend at AC
changing tendency of breakdown voltage versus aging time at DC and pulsatingvoltage. This changing
tendency was especially
DC voltage with smallobvious for papers
ripple factors inand
(r = 1/5 the 1/3)
earlywasor opposite
middle stageto theoftrend
aging, i.e., voltage.
at AC papers agedThis for
no more thantendency
changing 35 days wasat 120 ◦ C andobvious
especially no more forthan 22 in
papers days
the at 130or◦ middle
early C. For example, in Figure
stage of aging, 6b, from
i.e., papers
aged for
an aging no of
time more
fourthan 35 days
days at 120days,
to seven °C and noAC
the more than 22 days
breakdown at 130 °C.
voltage For example,
increased comparedin Figure 6b,that
with
from an aging time of four days to seven days, the AC breakdown voltage
of the previous aging state, while the DC breakdown voltage and pulsating DC breakdown voltage increased compared with
withthat of ripple
small the previous
factorsaging
(r = 1/5state,
andwhile
1/3)the DC breakdown
decreased, thoughvoltage
they alland pulsating
stayed DC breakdown
at a relatively high level
voltage with small ripple factors (r = 1/5 and 1/3) decreased, though
compared with that of unaged OIPs. All the above tendencies became inconspicuous they all stayed at a relatively
whenhigh the OIP
level compared with that of unaged OIPs. All the above tendencies became inconspicuous when the
reached its end of life. It should be noted that the changing tendencies of the AC breakdown voltage at
OIP reached its end of life. It should be noted that the changing tendencies of the AC breakdown
both temperatures were not in line with that obtained in reference [12], while they were similar to that
voltage at both temperatures were not in line with that obtained in reference [12], while they were
in reference
similar to[21].
that in reference [21].

(a)

(b)
Figure 6. Breakdown voltage of OIP versus thermal aging time: (a) 120 °C; (b) 130 °C.
Figure 6. Breakdown voltage of OIP versus thermal aging time: (a) 120 ◦ C; (b) 130 ◦ C.
Energies 2017, 10, 1411 7 of 16
Energies 2017, 10, 1411 7 of 16

4.
4. Discussion
Discussion

4.1.
4.1. Difference
Difference in
in Magnitude
Magnitude of
of Breakdown
BreakdownVoltage
Voltageat
atDifferent
DifferentVoltage
VoltageWaveforms
Waveforms
In
In this
this section,
section, the
the double-composite
double-composite dielectric
dielectric model
model is is used
used to to interpret
interpret the the difference
difference in
in the
the
magnitude of breakdown voltage of OIP at pulsating DC voltage at each aging
magnitude of breakdown voltage of OIP at pulsating DC voltage at each aging state from that at AC state from that at AC or
DC voltage.
or DC voltage.
The
Theinsulating
insulating paper contains
paper plentyplenty
contains of pores offilled
poreswith gases.with
filled Aftergases.
degassing Afteranddegassing
impregnation,
and
those pores are filled with insulating oil. The OIP can be equivalent to a
impregnation, those pores are filled with insulating oil. The OIP can be equivalent to a composite composite dielectric with
two layers,with
dielectric as modeled
two layers,in Figure 7, where
as modeled ε1 , γ1 ,7,d1where
in Figure and εε2 ,1,γγ21,, dd21 are
andthe equivalent
ε2, γ permittivity,
2, d2 are the equivalent
conductivity, and thickness of the oil and paper, respectively; R 1 , R 2 , C1 , and C
permittivity, conductivity, and thickness of the oil and paper, respectively; R1, R2, C1, and equivalent 2 are their C2 are their
resistance
equivalentand capacitance,
resistance respectively;
and capacitance, U1 and U2Uare
respectively; the voltages applied on insulating oil and
1 and U2 are the voltages applied on insulating
insulating paper, respectively.
oil and insulating paper, respectively.

(a) (b)
Figure 7.
Figure 7. The
The (a)
(a) double-composite
double-composite dielectric
dielectric model
model and
and (b)
(b) corresponding
correspondingequivalent
equivalentcircuit.
circuit.

The electric field in the OIP is co-determined by permittivity of oil and paper at AC voltage while
The electric field in the OIP is co-determined by permittivity of oil and paper at AC voltage while
it is co-determined by the conductivity at DC voltage. Therefore, the electric field strength in oil and
it is co-determined by the conductivity at DC voltage. Therefore, the electric field strength in oil and
paper, i.e., EOil and EPaper, can be obtained at pulsating DC voltage, which are as follows [19,26]:
paper, i.e., EOil and EPaper , can be obtained at pulsating DC voltage, which are as follows [19,26]:
2 2
EOil  U AC   U DC  (2)
EOil = U AC ·  2εd21  1d 2 + U ·2 d1   1γ
d 22
(2)
DC
ε 2 d1 + ε 1 d2 γ2 d1 + γ1 d2
 1
E U  ε 1 U  γ (3)
U AC · AC  2 d11   1d 2 + UDCDC·2 d1   1d 21
EPaper =Paper (3)
ε 2 d1 + ε 1 d2 γ2 d1 + γ1 d2
And the
And the following
following relationship
relationshipcan
canbe
beeasily
easilyobtained:
obtained:
U0  U1 +U2 =U AC +U DC (4)
U0 = U1 + U2 = U AC + UDC (4)
For the convenience of later description, we define EOb and EPb as the dielectric breakdown
For the
strength convenience
of oil of later description, we define EOb and EPb as the dielectric breakdown
and paper, respectively.
strength
For of oilvoltage,
AC and paper, therespectively.
electric field strength is inversely proportional to their permittivities for
For AC voltage, the electric
paper and oil. At room temperature, field strength is inversely
ε1/ε2 is about proportional
1/2. Therefore, mosttooftheir permittivities
the electric for paper
field strength is
and
withstood by insulating oil. As 1U0 2increases, EOil is always greater than EPaper. Because EPaper/EOil is
oil. At room temperature, ε /ε is about 1/2. Therefore, most of the electric field strength is
withstood
smaller thanby insulating
EPb/EOb, before theUinsulating
oil. As 0 increases, oilEOil is always
breaks down,greater
EPaper isthan EPapersmaller
always . Because EPaper
than EPb/E Ob is
. EOil is
smaller than E
much smaller Pb /E
thanOb , before the insulating oil breaks
EPb, so the oil breaks down prior to the paper, down, E is always smaller
Paperwhen EOil reaches EOb. than EPb . E Ob is
muchForsmaller than EPbthe
DC voltage, , soelectric
the oil field
breaks down prior
strength to the paper,
is inversely when Eto
proportional reaches
Oiltheir EOb .
conductivities for oil
and For DC Without
paper. voltage, the electric field
considering strength isofinversely
the influence moistureproportional to theirγconductivities
and other factors, 1/γ2 is about 100. for
oil and paper. Without considering the influence of moisture and other factors,
Therefore, most of the electric filed strength is withstood by the paper. Because E1 Paper2/EOil is greater γ /γ is about 100.
Therefore,
than EPb/EObmost
, as of U0 the electric Efiled
increases, strength
Paper firstly is withstood
reaches by the
EPb before EOil paper. EOb. TheEPaper
reachesBecause paper/EOil is greater
then breaks
than E /E
down Pbprior , as U increases, E firstly
Ob to the oil. Because EPb at DC voltage
0 Paper reaches E before E
Pb is a lot Oil reaches E . The paper then
greater thanObEOil, the corresponding breaks
down prior tovoltage
breakdown the oil.exceeds
Becausethat EPb atat DC voltage.is a lot greater than EOil , the corresponding breakdown
AC voltage
voltage
Forexceeds
pulsating thatDC at AC voltage.
voltage, Equations (2) and (3) can be rewritten as follows using Equations (1)
and (4):
Energies 2017, 10, 1411 8 of 16

For pulsating DC voltage, Equations (2) and (3) can be rewritten as follows using Equations (1)
and (4):
   
U0 rε 2 γ2 U0 2r 1
EOil = · + ≈ · + (5)
1+r ε 2 d1 + ε 1 d2 γ2 d1 + γ1 d2 1+r 2d1 + d2 d1 + 100d2
   
U0 rε 1 γ1 U0 r 100
EPaper = · + ≈ · + (6)
1+r ε 2 d1 + ε 1 d2 γ2 d1 + γ1 d2 1+r 2d1 + d2 d1 + 100d2
When r is very small, i.e., the DC component in pulsating DC voltage is dominant, which is
similar to that at DC voltage—the paper breaks down prior to the oil. When r is very large, i.e., the AC
component in pulsating DC voltage is dominant, which is similar to the situation for AC voltage, and
the oil breaks down prior to the paper.
Suppose the DC (r = 0) breakdown voltage of the OIP is UD . When r increases from 0 to infinite,
Equations (7) and (8) are permanently satisfied, i.e., the value of Equation (7) is always greater than 0,
while the value of Equation (8) is always smaller than 0. In other words, the electric field strength in
paper decreases while that in oil increases. If the increment in voltage applied to oil is greater than
the decrease in voltage applied to paper, then the breakdown voltage increases and exceed UD . Note,
however, that the breakdown voltage does not necessarily increase all the time, as r increases from 0 to
infinite, or the AC breakdown voltage is the greatest. It is actually the smallest. Therefore, it is obvious
that an r exists for the breakdown voltage to reach a maximum value, and it is greater than the DC
breakdown voltage. The maximum value is obtained when Equation (9) is satisfied.

dEOil 199d2 U0
= 2
>0 (7)
dr (1 + r ) (2d1 + d2 )(d1 + 100d2 )

dEPaper −199d1 U0
= <0 (8)
dr (1 + r )2 (2d1 + d2 )(d1 + 100d2 )
EOil E
= Ob (9)
EPaper EPb
In other words, the breakdown voltage reaches its maximum value when the paper and oil break
down at the same time. The corresponding r can be obtained with Equations (5), (6), and (9), and it is
as follows:
( E /E − 100)(2d1 /d2 + 1)
r ≈ Pb Ob (10)
(1 − 2EPb /EOb )(d1 /d2 + 100)
It is evident from Equation (10) that r is dependent on d1 , d2 , EOb , and EPb . Additionally, EOb and
EPb are not constants for oil and paper of different thicknesses and different voltage waveforms [20]. In
other words, it depends on the interaction between d1 /d2 and EPb /EOb when the breakdown voltage of
OIP reaches its maximum value. In this experiment, the maximum value was observed for an r of 1/5,
except the insulating paper that reached its end of life when few differences existed in the breakdown
voltage at the three types of voltage waveforms.

4.2. Possible Influencing Factors for Variation of Breakdown Voltage Versus Aging Time
In this section, the variation of breakdown voltage versus aging time is analyzed, including the
opposite changing tendencies between AC voltage, and pulsating DC voltage with small ripple factors
(r = 1/5 and 1/3) and DC voltage. Possible influencing factors such as DP, moisture content of paper
and oil absorption associated with the pores and cracks of aged paper are investigated.
Energies 2017, 10, 1411 9 of 16
Energies 2017, 10, 1411 9 of 16

4.2.1. DP
4.2.1. DP of
of Paper
Paper
Figure 88 presents
Figure presents the DP of
the DP of the
the paper.
paper. The
The first-order
first-order kinetic
kinetic model
model was
was used to fit
used to fit the
the DP
DP versus
versus
the aging time, which is shown in Equation (11) as follows
the aging time, which is shown in Equation (11) as follows [27]:[27]:

11 1
− =ktkt (11)
(11)
PtP PP0
t 0

where P
where and PPtt are
P00 and arethe
theDP
DPofofunaged
unagedpaperpaperandandpaper
paperaged
agedfor
foran durationofoft, t,respectively;
anduration k is
respectively;k is a
a constant. DP decreased dramatically at both aging temperatures, whereas
constant. DP decreased dramatically at both aging temperatures, whereas it decreased relativelyit decreased relatively
slowly when
when approaching
approaching about
about 500.
500. Note
Note that
that DP
DP of
of paper
paper aged
aged for
for 180
180 days
days at
at 120 ◦ C, and for
120 °C,
slowly and for
90 days ◦ C, reached a level less than 250. No clear correlation was found, however, between
90 days atat 130
130 °C, reached a level less than 250. No clear correlation was found, however, between
DP and
DP and the
the breakdown
breakdown voltage. Even when
voltage. Even when the
the DP
DP decreased
decreased from
from 1265
1265 toto less
less than
than 400,
400, no
no marked
marked
reduction in breakdown voltage was observed. Therefore, the decrease in
reduction in breakdown voltage was observed. Therefore, the decrease in DP had no reason to DP had no reason to be
be
considered for
considered for the
the small
small variation
variation ofof breakdown
breakdown voltage
voltage of of OIP,
OIP, and
and in
in turn
turn the
the breakdown
breakdown voltage
voltage
could not be taken as an indicator of the aging state of paper, which was in accordance
could not be taken as an indicator of the aging state of paper, which was in accordance with [22]. with [22].
However, this was not applicable to the life-end stage of the OIP, because the DP reached
However, this was not applicable to the life-end stage of the OIP, because the DP reached a seriously a seriously
small level.
small level. The
The structural
structural damage
damage of of paper
paper atat this
this stage
stage together
together with
with the
the high
high level
level of
of moisture
moisture
content was significant enough to contribute to the sudden decrease of breakdown
content was significant enough to contribute to the sudden decrease of breakdown voltage. This voltage. This was
was
not in
not in line
line with
with publication [12] mainly
publication [12] because of
mainly because of the
the difference
difference in
in the
the moisture
moisture level and paper
level and paper
structural damage.
structural damage.

Figure 8. DP of aged paper.


Figure 8. DP of aged paper.

4.2.2. Moisture Content


4.2.2. Moisture Content
Figure 9 shows the moisture content in OIP. It fluctuated during the aging process and increased
Figure 9 shows the moisture content in OIP. It fluctuated during the aging process and increased
sharply when the paper nearly reached its end of life. Moisture content was considered to influence
sharply when the paper nearly reached its end of life. Moisture content was considered to influence
the breakdown strength of paper [28]. That might be the reason why the obtained results were not all
the breakdown strength of paper [28]. That might be the reason why the obtained results were not all
in line with those obtained in [12], as the moisture content for some of the aged papers were relatively
in line with those obtained in [12], as the moisture content for some of the aged papers were relatively
higher than that in [12]. However, it could not explain why some OIPs with a relative high level of
higher than that in [12]. However, it could not explain why some OIPs with a relative high level of
moisture content had a relatively high AC breakdown voltage. For example, for paper subject to
moisture content had a relatively high AC breakdown voltage. For example, for paper subject to
thermal aging for two and 60 days at 120 ◦°C and for two, seven, and 10 days at 130 °C, the breakdown
thermal aging for two and 60 days at 120 C and for two, seven, and 10 days at 130 ◦ C, the breakdown
voltage, especially the AC breakdown voltage, did not decline much, or even increased compared
voltage, especially the AC breakdown voltage, did not decline much, or even increased compared
with that of unaged paper, and was even higher than some other papers whose moisture level was
with that of unaged paper, and was even higher than some other papers whose moisture level was
relatively low. This implies that there could be some other factors offsetting the influence of moisture
relatively low. This implies that there could be some other factors offsetting the influence of moisture
content on AC breakdown voltage of those thermally aged paper.
content on AC breakdown voltage of those thermally aged paper.
Energies 2017, 10, 1411 10 of 16
Energies 2017, 10, 1411 10 of 16

Energies 2017, 10, 1411 10 of 16

Figure 9. Moisture content of OIP.


Figure 9. Moisture content of OIP.
Figure 9. Moisture content of OIP.
4.2.3. Oil Absorption Ability of Paper Associated with Pores and Cracks
4.2.3. Oil Oil
4.2.3. Absorption
Absorption Ability
Ability ofofPaper
PaperAssociated
Associated with Pores and
with Pores andCracks
Cracks
Insulating paper consists of large numbers of cellulose fibers and it has a lot of pores, the
Insulating
Insulatingpaper consists
paper consists of large numbers
of large numbersof cellulose fibers
of cellulose and it
fibers hasitahas
and lot of pores,
a lot the diameter
of pores, the
diameter of which ranges from tens of nanometers to thousands of nanometers. In this paper, the
diameter of which ranges from tens of nanometers to thousands of nanometers.
of which ranges from tens of nanometers to thousands of nanometers. In this paper, the mesoporous In this paper, the
mesoporous
mesoporous
distribution
distribution
ofofinsulating
insulating
paper was
paperwith
measured with
wasnitrogen
measured
withnitrogen
nitrogengasgas adsorption
adsorptionmethod,
and
and
distribution of insulating paper was measured gas adsorption and desorption
desorption method, and itsitsmacropores were observed with
withSEMSEMtotoassociate
associate thetheoil oil absorption
anddesorption
its macropores method,
wereand observed macropores
with SEM wereto observed
associate the oil absorption ability with absorption
some of the
ability with some
abilitytendency
with some of the changing tendency of the breakdown voltage. For simple discussion and
changing ofof
thethe changing tendency
breakdown of the
voltage. For breakdown
simple voltage.
discussion For simple
and analysis discussion
in this paper, and
papers
analysis in
analysis this paper, papers aged at 130 °C are selected as an example, and are the same as those
aged at 130 ◦inCthis
are paper,
selected papers
as anaged at 130and
example, °C are
areselected
the same asas
anthose
example,
agedand are ◦the
at 120 C. same as those
aged at 120
aged °C.°C.
at 120
The nitrogen gas adsorption and desorption measurements were conducted to examine the porous
TheThenitrogen
nitrogengas
gasadsorption
adsorptionand and desorption measurementswere
desorption measurements wereconducted
conducted to to examine
examine the the
nature of the insulating paper. The pore-size distribution and pore volume were obtained following
porous nature of the insulating paper. The pore-size distribution and pore
porous nature of the insulating paper. The pore-size distribution and pore volume were obtained volume were obtained
the Barrett-Joyner-Halenda (BJH) method [29], and the specific surface area was obtained with the
following
following thethe Barrett-Joyner-Halenda(BJH)
Barrett-Joyner-Halenda (BJH) method
method [29],
[29],and
andthethespecific
specificsurface
surfacearea
areawaswasobtained
obtained
Brunauer-Emmett-Teller
with (BET) method [30].method
Figure 10 shows the typical nitrogen gas nitrogen
adsorption gasand
with thethe Brunauer-Emmett-Teller
Brunauer-Emmett-Teller (BET)
(BET) method [30].
[30]. Figure
Figure1010shows
showsthethetypical
typical nitrogen gas
desorption
adsorptionisotherm
and of insulating
desorption paper.
isotherm of insulating paper.
adsorption and desorption isotherm of insulating paper.

Figure 10. Typical nitrogen adsorption and desorption isotherm of insulating paper.
Figure 10. Typical nitrogen adsorption and desorption isotherm of insulating paper.

The Figure 10. Typical nitrogen adsorption and desorption isotherm of insulating paper.
BJH analyses showed that the insulating paper exhibited no pore sizes of less than 15
nanometers, and there showed
The BJH analyses thatmost
were various the probable
insulating paper
pore sizes exhibited
for papers ofnodifferent
pore sizes
agingofstates,
less as
than
The BJH
15 nanometers, analyses
and 11.
shown in Figure there showed
Forwere that
OIPs various the
most
with aging insulating
probable
time paper
of 0, 2, 7,pore exhibited
sizes
10, 22, andfor no
90 papers pore sizes
of different
days, they had marked of less
aging than 15
states, as
probable
nanometers,
shown
poreinsizes,and
Figure there
11.the
and were various
Forcorresponding
OIPs with agingmost
peaktimeprobable
of of
value 0, 2, pore sizes
7, 10,was
dV/dD for
22, and papers
90 days,
greater of different
theyof
than that had aging
marked
other states,
OIPs, as
aged probable
shown
porewhichin Figure
sizes, 11.they
indicates
and the Forhad
OIPs with
large
corresponding aging
pore sizetime
peak and of
value of0,dV/dD
2, 7,which
volume, 10, 22,
wasisand 90 days,
consistent
greater they
with
than had
the
that marked
results
of other probable
presented
aged OIPs,
pore
which sizes,
in Figure and the
12. The
indicates corresponding
theyBEThadspecific peak
surface
large pore value
sizearea of
andofvolume, dV/dD
insulating was greater
paperisof
which than that
different aging
consistent of other
states
with the aged
is presented
results OIPs,
presented
which indicates they had large pore size and volume, which is consistent with the results presented
in Figure 12. The BET specific surface area of insulating paper of different aging states is presented
Energies 2017, 10, 1411 11 of 16

Energies 2017, 10, 1411 11 of 16


in Figure 12. The BET specific surface area of insulating paper of different aging states is presented
in
in Figure
Figure
Energies 13.
13. It
It10,exhibited
Energies 2017, exhibited
1411
aa fluctuation
fluctuation during
during the
the thermal
thermal aging
aging process,
process, following
following almost the
almost 11
the
11 same
same
of of
16 16
variation
variation tendency
tendency withwith that
that of
of pore
pore volume.
volume.
in Figure 13. It exhibited
exhibited aa fluctuation
fluctuationduring
duringthe
thethermal
thermalaging
agingprocess,
process,following
followingalmost
almostthe
the same
same
variation tendency with with that
that of
of pore
porevolume.
volume.

Figure 11. Pore distribution of paper thermally aged for various durations at 130 ◦°C.
Figure 11. Pore
Figure distribution ofofpaper thermally aged
aged forvarious
various durations at 130 C.
Figure 11.
11. Pore
Pore distribution
distribution ofpaper
paperthermally
thermally agedfor
for variousdurations
durationsatat130 °C.
130 °C.

Figure 12. Pore volume of paper thermally aged for various durations at 130 °C.
◦ C.
Figure 12.12.
Figure Pore volume
Pore ofofpaper
volume paperthermally
thermallyaged
agedfor
for various
various durations at130
durations at 130
130°C.
°C.

Figure 13. Specific surface area of paper thermally aged for various durations at 130 °C.
Figure 13. Specific surface area of paper thermally aged for various durations at 130 °C.◦
Figure 13.
Figure Specific surface
13. Specific surface area
area of
of paper
paper thermally
thermally aged
aged for
for various
various durations
durations at
at 130 C.
130 °C.
Energies 2017, 10, 1411 12 of 16

Energies 2017, 10, 1411 12 of 16


Figure 14 shows typical SEM images of insulating paper thermally aged for various durations at
Figure
130 ◦ C. 14 showsortypical
Macropores cracksSEM
withimages of insulating
a diameter paper
of several thermallybegan
micrometers aged to
forappear
variousindurations
insulatingat
130 °C.after
paper Macropores
22 days or
of cracks
thermalwith a diameter
aging. of several
The diameter of micrometers beganexhibited
pores and cracks to appearaninincreasing
insulating
paper after 22 days of thermal aging. The diameter
tendency along with the increase of thermal aging time. of pores and cracks exhibited an increasing
tendency along with the increase of thermal aging time.

(a) (b)

(c) (d)

(e) (f)
Figure 14. Scanning electron microscopy (SEM) images of paper thermally aged for various durations
Figure 14. Scanning electron microscopy (SEM) images of paper thermally aged for various durations
at 130 °C. (a) 0 day; (b) 10 days; (c) 22 days; (d) 35 days; (e) 60 days; (f) 90 days.
at 130 ◦ C. (a) 0 day; (b) 10 days; (c) 22 days; (d) 35 days; (e) 60 days; (f) 90 days.

The increased oil absorption associated with the pores and cracks of paper had different effects
The increased oil
on the breakdown absorption
voltage of OIP associated
at DC and with the pores
AC voltage, and cracks
which of paper
is discussed had different effects
below.
on theAs
breakdown voltage
is well-known, theofrelation
OIP at DC and AC
between thevoltage,
electric which is discussed
field strength below.
E(l) and the voltage applied to
As is well-known, the relation between
the OIP sample U0 can be expressed as [12]: the electric field strength E(l) and the voltage applied to
the OIP sample U0 can be expressed as [12]:
U 0 Z E  l  dl (12)
U0 = E(l ) dl (12)
where l is the distance at the direction of electric field. For simplicity, EOil and EPaper are considered to
be uniform. When the applied voltage is AC voltage, the relationship between the both can be
written as [22]:
EOil 
 2 (13)
EPaper 1
Energies 2017, 10, 1411 13 of 16

where l is the distance at the direction of electric field. For simplicity, EOil and EPaper are considered to
be uniform. When the applied voltage is AC voltage, the relationship between the both can be written
as [22]:
EOil ε
= 2 (13)
EPaper ε1
Combining (12) and (13) yields the electric field in oil and paper as [12]:

U0
EOil =   (14)
ε1 ε1
1− lo +
ε2 ε2 l

U0
EPaper =   (15)
ε2
ε1 − 1 lo + l

where lo is the total equivalent thickness of oil along the electric field. For the case that more oil
is absorbed by the paper, i.e., the increased lo , it causes the decrease of electric field strength, this
should obviously create better electric field distribution in the OIP. Consequently, the breakdown
voltage increases.
In the case of applying a DC voltage, (13) can be rewritten as [6]:

EOil γ
= 2 (16)
EPaper γ1

Combining (12) and (16), yields the electric field in oil and paper as [12]:

U0
Eoil =   (17)
γ1 γ1
1− γ2lo + γ2 l

U0
EPaper =   (18)
γ2
γ1 − 1 lo + l

When more oil is contained in the paper, i.e., lo is increased, the electric field in oil and paper
increase resultantly. This leads to a decreased breakdown voltage. It is therefore seen that the
application of DC voltage make the breakdown voltage develop in an opposite fashion to that of
AC voltage.
For the OIP samples aged for less than 35 days, the increased pore volume and specific surface
area were expected to have a higher capacity of oil absorption. This would result in quite different AC
and DC breakdown voltage values upon the case that more oil would be absorbed into the insulating
paper. This should account for that the AC breakdown voltage of OIPs aged for two, seven, 10, and
22 days did not drop much, or even increased a bit compared with that of unaged OIPs, although the
moisture content in some of those OIP samples remained relatively high at around 1.8%. However,
as the oil absorbed had opposite effects on breakdown voltage at AC and DC voltage, the changing
tendencies of DC voltage and pulsating DC voltage with small ripple factors (r = 1/5 and 1/3) were
different from that of AC voltage. For example, from an aging time of four days to seven days, the AC
breakdown voltage increased compared with that of its previous aging state while the DC breakdown
voltage and pulsating DC breakdown voltage with small ripple factors (r = 1/5 and 1/3) decreased.
For the OIP samples aged for 35 and 60 days, mesopores pore size and volume in insulating paper
were not the dominant factors influencing breakdown voltage. Instead, the influence of macropores or
cracks of cellulose fibers were considered, as shown in Figure 14. They were filled with oil, improving
the electric field distribution in OIP samples at AC voltage. Damage to paper structure might reduce
the breakdown voltage, whereas the improvement in electric field distribution somewhat balanced
this effect. Consequently, the AC breakdown voltage showed limited reduction compared with that of
Energies 2017, 10, 1411 14 of 16

unaged OIPs. However, the breakdown voltage at pulsating DC with small ripple factors (r = 1/5 and
1/3) and DC voltage exhibited a greater decrease compared with that of unaged OIPs, as the oil in
paper had adverse effects on it.
For the OIP samples aged for 90 days, DP of paper was very small (around 160) and the structure
of paper was seriously damaged in this state. Therefore, the breakdown voltage reduced sharply,
regardless of the pores and cracks that were filled with oil. In this aging state, the damage to paper
structure became the dominant factor influencing the breakdown voltage. It should also be noted
that the moisture content was very high (about 2%) at this aging state, which also contributed to the
decrease of breakdown voltage.

5. Conclusions
This paper investigates the breakdown voltage and its influencing factors of thermally aged OIP
at pulsating DC voltage. The main conclusions are summarized as follows.
Breakdown voltage at pulsating DC voltage and DC voltage was far greater and had a greater
standard deviation than AC breakdown voltage. It was co-determined by the electric field distribution
in paper and oil, and their breakdown strengths. The analysis results by the double-composite dielectric
model showed that a ripple factor r existed for the breakdown voltage to reach its maximum value.
The difference in magnitude of breakdown voltage among pulsating DC (r = 1/5 and 1/3) and DC
voltage, however, was not so pronounced.
The breakdown voltage of aged OIP at pulsating DC voltage fluctuated during the thermal aging
process as the AC breakdown voltage did, but showed a somewhat opposite changing tendency,
especially for the breakdown voltage at pulsating DC voltage with small ripple factors (r = 1/5 and
1/3) in the early and middle stage of aging. The moisture content, oil absorption ability associated
with pores and cracks of paper, and the damage to paper structure all contributed to the variation
of the breakdown voltage versus aging time with different weights of importance as the aging state
of paper varied. For OIPs in the early or middle stage of aging, the variation in breakdown voltage
versus aging time was considered to be influenced by moisture content and the oil absorption related
to the mesopore volume of paper. The oil filled the pores and improved the electric field distribution
at AC voltage, and thus had a positive effect on the AC breakdown voltage, while it had an adverse
effect on the DC breakdown voltage. Therefore, the breakdown voltage at pulsating DC voltage
with small ripple factors (r = 1/5 and 1/3) and DC voltage showed an opposite changing tendency
compared with that at AC voltage. For OIPs in the middle-late stage of aging, the macropores or cracks
between cellulose fibers rather than the mesopores were considered to have influenced the breakdown
voltage of OIP together with moisture content and structural damage of paper. For OIPs that reached
its end of life, the damage to the paper structure and the high level of moisture were the dominant
influencing factors. Both factors resulted in the sharp decrease of breakdown voltage at the three types
of voltage waveforms.

Acknowledgments: The authors thank the National Natural Science Foundation of China (Grant No. 51425702)
and the 111 Project of China (Grant No. B08036) for the financial support provided.
Author Contributions: The research work presented in this paper was collaboratively conducted by all authors.
Feipeng Wang and Jian Li designed the experiment; Jing Zhang carried out the experiments with Hehuan Ran
and Xudong Li; Jing Zhang analyzed the test results with Feipeng Wang and Qiang Fu; Jing Zhang wrote this
paper; Feipeng Wang revised the manuscript.
Conflicts of Interest: The authors declare no conflict of interest.

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