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Sima 2015
Sima 2015
ABSTRACT
The mechanisms by which conductive and dielectric nanoparticles (NPs) trap
electrons are explained by the potential well distribution caused by induced or
polarized charges on NPs. Thus, the distributions of surface and saturation charges
on conductive and dielectric NPs are determined. Given conductive Fe3O4,
semiconductive TiO2, and dielectric Al2O3 NPs, insulation performance tests are
conducted and ionization models of nanofluids (NFs) based on transformer oil are
developed. These models are compared with those of NFs based on pure oil. The NP
whose conductivity or permittivity does not match that of the dielectric liquid has a
potential well and an increased amount of saturation charges on its interface. This
NP influences streamer development strongly and enhances the breakdown of oil-
based NF.
Index Terms - Conductivity, nanoparticle, oil insulation, potential well,
permittivity, streamer.
DOI 10.1109/TDEI.2014.004277
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 22, No. 1; February 2015 381
To understand why different NPs can improve the 2.1 NANOFLUID PREPARATION
breakdown voltage of transformer oil, the effects of In this study, all of the experiments utilized #25 Karamay
different NPs on transformer oil still require further oil. The transformer oil-based NFs were prepared in the
investigation in terms of electrical performance and proper concentrations by adding specific amounts of
mechanism. modified NPs (average NP size d = 10 ± 0.1 nm) into the
In this study, the levels of withstand voltage of base oil. The surfaces of the NPs were modified with
switching impulse in pure oil and in three selected NFs are surface modifiers to enhance oil-wet behavior, as shown in
tested by a needle-plate electrode under both positive and Table 1.
negative voltages. In these NFs, conductive Fe3O4,
semiconductive TiO2, and dielectric Al2O3 NPs are
suspended. Conductive and either semiconductive or
dielectric NPs with high permittivity enhance the
breakdown performance of NFs based on transformer oil.
Thus, in consideration of the capability of NPs to trap
electrons, a positive streamer model is constructed which
is based on electrodynamic equations and is similar to the
model in Zahn’s work [5]. The results of this study
provide a reference with respect to the selection of NP
material. They also confirm the experimental and
theoretical feasibilities of the novel NFs based on
insulation oil in high voltage engineering.
2 EXPERIMENT
To determine the electrical property that predominantly Figure 1. Three different transformer oil-based NFs with NP suspensions
affects streamer dynamics in NFs based on transformer oil, of Fe3O4;TiO2 and Al2O3.
representative conductive, semiconductive, and
nonconductive NPs are chosen. Their electrical The NFs disperse steadily after ultrasonic dispersion,
conductivities and relative permittivities are listed in Table dehydration, and degassing, as presented in Figure 1. The
1. The electrical properties of the semiconductor are highly processed oil was sealed for months before testing and
dependent on temperature; therefore, the value ranges of experimenting.
conductivity and permittivity are extensive. TiO2 NP is 2.2 MEASUREMENTS OF BREAKDOWN
considered a dielectric insulator based on the experimental STRENGTH
condition (room temperature) and the low-temperature
plasma simulation in this study. This insulator may be high The gap of the needle–plate electrode was 5 mm. The
in permittivity and low in conductivity. needle possessed a curvature radius of 40 µm, whereas the
radius of the plate was 5 cm. The waveform of the
switching impulse voltage was 250 µs/2500 µs. This
Table 1. Electrical properties of representative conductive and dielectric waveform was generated by the customized impulse
NP materials. generator. The impulse breakdown voltages were also
NP type Fe3O4 TiO2 Al2O3 measured based on the standard procedures to test the
Relative permittivity 80 31 to 114 9.9 breakdown voltages of lightning impulse (IEC 60897-1987)
Conductivity (S·m−1) 104 10−8 to 101 10−12 [14]. The initially selected voltage, which was low, was
Relaxation time (s)
7.47 × 3.13 × 10−11 to
42.5 applied to the oil sample and then increased by 5 kV until
10−14 0.20 breakdown occurred. The process was repeated 10 times.
Material type Conductor Semiconductor Insulator The minimum interval between two successive tests was 1
Surface modifier Oleic acid Stearic acid Span 80 min. The crest values of the impulse voltages were recorded
Note: The italicized parameters are presented in this paper. by an oscilloscope. Their average values were considered
Table 2. Test results of switching impulse withstand voltage in a system with a 5 mm electrode gap system given pure oil and NFs.
the experimental results. The following conclusions can be In the time range of streamer development in NFs based
drawn from Table 2: on transformer oil (tens of nanoseconds), NP surfaces
1) During the switching impulse tests, the positive contain not only induced charges, but also polarized
voltage of electrical breakdown of the Fe3O4 NF is 44.3% charges. In other words, both induced and polarized charges
higher than that of the base oil. The increase in the positive are fast enough to follow the electric field during streamer
voltage of impulse breakdown of this NF is similar to the discharge in transformer oil.
increases in Al2O3 and TiO2 NFs at 33.3% and 35.5%, 3.1.2 SURFACE CHARGE DENSITY ON
respectively. NANOPARTICLES
2) The breakdown times of Fe3O4, TiO2, and Al2O3 NFs The electric field outside the conductive or dielectric
are 482, 392, and 323 µs, respectively. This finding spherical NP at its radial direction in transformer oil is
suggests that the discharge processes in all NFs are deduced in [5] and introduced in [15], and as shown in
significantly hindered by the addition of NPs. The standard Figure 2. These fields are expressed as follows:
deviations for all NFs are less than 7%.
2 R t
3
The insulation performances (especially the positive Er r R , E0 1 3 2 1 exp
withstand voltages) of all three NFs containing conductive, r 21 2 r
semiconductive, and dielectric NPs are significantly (1)
improved, compared to the breakdown strength of pure oil. 2R3 2 1 t
3 1 exp cos
Based on these results, we assume that both the r 2 1 2 r
conductivity and permittivity of NPs are significant in the
development of streamers. 21 2
r = (2)
2 1 2
3 CHARGING DYNAMICS OF
NANOPARTICLE where E0 is the applied electric field; R is the radius of the
In Section 2, we conclude that both NP conductivity and NP; ε1 and ε2 are the permittivities of transformer oil and
permittivity modify fundamental electrodynamic processes NP, respectively; and σ1 and σ2 are the conductivities. r is
in oil. The action mechanisms are deduced in Section 3. the charge relaxation time.
3.1 CHARGE ACCUMULATION ON
NANOPARTICLES (,
3.1.1 CONDUCTIVE AND DIELECTRIC
NANOPARTICLES IN A UNIFORM ELECTRIC
FIELD
_+ + +_
The massive electrons in the conductive metal oxides _ _
(such as the Fe3O4 NP used in this paper) move inversely _ _
__ _
along the direction of the local electric field, which
generates positive and negative charges at opposite sides of
_ __
the conductor. These surface charges are called induced
charges. Charge induction is almost instantaneous. Aside
from electrons, positive holes are involved in the
conduction of semi-conductors (such as the TiO2 NP used Figure 2. Sketch of nanoparticle surrounded by insulating transformer oil
under electric field, E0
in this study).
With dielectrics (such as the Al2O3 NP used in this The time constant τr describes the typical time that the
study), the bound charges are formed at the surface of NP redistribution of polarized charges on a NP needs, and is
due to the vertical electric field known as dielectric closely related to the electrical conductivity and
polarization. This process consists of displacement and permittivity. The simplest theoretical description of
turning-direction polarizations. The (electronic and ionic) relaxation as function of time t is an exponential law
displacement polarizations are generated very swiftly in exp(-t/τr). In a semiconductor, it is a measurement of
only 10−15 to 10−12 s. Turning-direction polarization how long it takes to become neutralized by conduction
(including dipole polarization) is highly dependent on process. The charge relaxation times are very small in
temperature and the applied local electric field. Thus, conductors and can be large in semiconductors and
polarization can only be obtained after 10−10 s to 10−2 s. insulators. The charge relaxation times of three different
Many important materials contain a sea of free NPs are listed in Table 1. For nanoparticles with
electrons that produce a finite conductivity value. These different dielectric parameters, some deductions can be
materials also possess tightly bound electrons that generate drawn from equations (1)-(2), as follows:
dielectric permittivity. Thus these materials serve as both (1). Given perfectly conductive material such as Fe3O4
conductors and insulators as well, such as the Fe3O4 NP NP, τr is 7.47 × 10−14 s. t is in ns (the timescales of interest
suspensions in transformer oil in this study. for streamer growth). Therefore, the exponential function is
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 22, No. 1; February 2015 383
exp t r 0 . The external radial electric field is significantly enhanced by the mismatch between
conductivity and permittivity and transformer oil. These
calculated as follows:
charges are similarly formed. We therefore predict that the
2 R 1
3
Er r R , E0 1 3 2
r
cos
2 1 2
influences of both conductive and dielectric NPs on the
electrodynamic process of streamer development in
(3) transformer oil are similar. The following sections
2 R3
E0 1 3 cos ir ( 2 1 ) introduce the charge accumulation in and the charging
r dynamics of NPs.
As shown in equation (3), the external radial electric 3.1.3 POTENTIAL WELL ON NANOPARTICLE
field is distorted by strong NP conductivity. Hence, the
Charges of opposite polarity mutually attract, whereas
induced surface charge density on the interface of the
similar charges repel each other. In this section, we explain
dielectric particle is written as:
the trapping of NPs by charge carriers in a novel and
s ir ( D1R D 2 R ) quantitative manner. Charge carriers are trapped by the
potential well distribution, which is induced by surface
1 Er r R , 2 Er r R , (4) charges on conductive and dielectric NPs. Hence, the
relation between the external potential and the modified
31 E0 cos
electric field outside the spherical NP is written as follows:
(2). The τr values of TiO2 and Al2O3 NPs are 0.2 and 42.5 s,
respectively. These NPs are spherical dielectric materials, and ext r =
r
E r R , d r = Er r R , dr (8)
r
the dielectric relaxations are negligible in both cases as a result
of the long τr relative to the timescale of interest for streamer By combining equation (3) with equation (8), the
growth. However, (oriented or distorted) dipole and ionic external potential distribution in a conductive NP can be
(displacement) polarizations can still be observed. As calculated as follows:
described in Section 3.1.1, the polarized charges from
2 1 3 1
displacement and dipole turning-direction polarizations are fast ext = E0 rcos R E0 2 cos (r R ) (9)
enough to follow the swift changes in the electric field of the 2 1 2 r
streamer (tens of nanoseconds). Therefore, the exponential
where E0 rcos is the potential produced by the applied
function is exp t r 1 (t has a nanosecond timescale). The
electric field. The potential well distribution induced by
external radial electric field is calculated as follows:
surface charge is
2R3
Er r R , E0 1 3 2 1 cos (5) p =
2 1 3 1
R E0 2 cos (r R)
r 21 2 (10)
21 2 r
The external radial electric field is distorted by strong NP Similarly, the potential distribution produced by the
permittivity, which is modified by polarized rather than free polarized surface charge on a dielectric NP is given as:
charges. In addition, the extent of modification by the
polarized charges on the surface is highly dependent on NP 2 1 3 1
p = R E0 2 cos (r R) (11)
permittivity and the surrounding dielectric liquid. 21 + 2 r
The electric field at the inner surface of the dielectric
sphere is introduced in [16] and is expressed as follows: As shown in equations (10) and (11), the potential well
31 distribution outside an NP is modified regardless of whether
E r R ,
21 2
E0 cos ir the NP surface contains induced or polarized charges. This
(6) phenomenon influences the charge carriers. The potential
31 well distribution that induces surface charges either along
+ E0 sin i
21 2 the same direction (θ = 0) as or in the opposite direction (θ
= π) from the applied electric field is provided as:
The density of these charges on the interface of the
dielectric particle is expressed as follows: x2 x1 3 1
2 x +x R E0 r 2 ( 0, r R )
s R + R
p E0 = 1 2 (12)
ir ( P R P R ) x2 x1 R 3 E 1 ( , r R )
2 x1 +x2 0 2
r
2 0 Er r R , 1 0 Er r R , (7)
where x1 and x2 are either the conductivity or permittivity of
3 0 2 1 E0 cos the transformer oil and NP, respectively.
21 2 The shapes at the top of Figure 3 depict the
As indicated in equations (4) and (7), the accumulated distributions of surface charges and the electrical potential
surface charges in both conductive and dielectric NPs are distributions outside different NPs in the direction of the
384 W. Sima et al.: Effects of Conductivity and Permittivity of Nanoparticle on Transformer Oil Insulation Performance
applied electric field along the axis. (a) denotes an NP The distributions of induced potential well on Fe3O4,
given constant permittivity and conductivity of TiO2 and Al2O3 NPs at the applied electric field direction
transformer oil; (b) represents an NP with various along the central axis of sphere are shown in Figure 4.
permittivities and conductivities of transformer oil, and (c) Assuming that the electric field is uniform, i.e., E0 = 100
corresponds to an NP with extremely high conductivity. (a) kV·mm−1 and r = R = 5 nm, the potential well depths on the
has a straight potential line [V(r) + V0(r)] and a potential surfaces of Fe3O4, TiO2, and Al2O3 NPs are 0.50, 0.47, and
well distribution [V(r)] of zero, as denoted by the shapes 0.27 V, respectively, using the parameters given in Table 1.
at the bottom of Figure 3. Based on this result, charges Accordingly, the potential wells of dielectric NPs are
were not generated on the NP surface. In (b), the potential shallower than those of conductive NPs. The positive
distribution deviates from the potential V0(r), thus potential well traps on conductive NPs can capture passing
indicating the induction of surface charges on the interface electrons rapidly and convert them into negatively charged
and the distribution of a shallow potential well in the NPs, which are slower, through repeated trapping. If the
vicinity. In (c), numerous charges are generated on the positive and negative potential wells are deep enough,
surface of the spherical conductive NP, thereby rendering positive and negative ions, respectively, cannot escape.
it equipotential. As a result, a deep potential well is Nevertheless, the trapping of electron carrier by NPs
distributes near the NP surface [V(r = R) = V0(r = R)]. significantly reduces the speed of streamer propagation and
The maximum potential depth of the well on the NP enhances the dielectric strength of transformer oil modified
interface is generally proportional to its radius. Therefore, by NPs.
NP materials with relatively large radii should be added to 3.2 CHARGING DYNAMICS OF NANOPARTICLES
the transformer oil on the condition that these NPs have
As described in Section 3.1, the NPs in transformer oil
extraordinary stable solubility without precipitation.
are induced or polarized under the applied electric field
Given this consideration, the ideal NP radius should not
(Figure 5a) in a very short timescale. Figure 5b indicates
exceed 10 nm.
that positive and negative charges are generated at the
lower and upper hemispheres of NPs, whereas no space
charge is observed in the bulk. The electrons that originate
from either ionization or injection move quickly in the
positively charged hemisphere (Figure 5c). As a result, the
distribution immediately evens out. This process
represents the charging dynamics of NPs. Upon
completion of this charging process, the spherical NP is
saturated with negative charges, and electrons are no
longer trapped (Figure 5d). The positive ions and negative
ions are not taken into consideration and are regarded
motionless during the charging process, for their mobility
(p = n = 1 × 10−9 m2·V−1·s−1 [17]) are five orders of
magnitude smaller than electron’s mobility (μe = 1 × 10−4
Figure 3. Electrical potential distributions V(r) + V0(r) (top shapes) and m2·V−1·s−1 [18]).
potential well distributions V(r) (bottom shapes) near (a) NP given
constant permittivity and conductivity of transformer oil, (b) NP with
various permittivities and conductivities of transformer oil, and (c) NP
with extremely high conductivity.
E0
0.6 + + ++++
+
Al2O3
0.2
a 植物绝缘油 b
(, )
0
___
_+ + +_ _ _
-0.2 _ _ _ _
_ _ _ _
__ __ _ _
_ _ __ _
-0.4
c d
-5 -15 0 -10 5 10 15 Figure 5. Electric field lines after a uniform z-directed electric field is
Axial distance(nm) activated at t = 0 around an NP with radius R, permittivity ε2, and
Figure 4. Potential well distributions in the direction of the applied electric conductivity σ2. This NP is surrounded by transformer oil with permittivity
field along the central axes of the spherical Fe3O4, TiO2, and Al2O3 NPs. ε1 and conductivity σ1.
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 22, No. 1; February 2015 385
Once the NPs are saturated with negative charges, the attachment. The time constant of attachment is given as
electron saturation charge for the nanoparticle is expressed follows:
as follows:
NP 2ns (17)
2
Qs 0 s R sin 2
R cos d
2
voltage; however, their effects on streamer development As depicted by the waveform in this figure, the step
rarely vary. Therefore, the voltage waveform used in the voltage reaches its maximum value in only 3 × 10−13 s,
simulation does not affect the analysis of NPs’ effect on which is far shorter than the timescale of the streamer (ns).
streamer development. And in this model, a step voltage is Thus, this time can be ignored. The application of the step
therefore applied to the needle electrode. The electrode voltage to the needle electrode generates a nonuniform
reaches its maximum value (90 kV) very quickly. Thus, distribution of Laplacian electric field at t = 4 × 10−13 s, as
streamer initiation time can be neglected. To avoid reaching shown in the 2D plot of electric field distribution in Figure
singularity, the step voltage to be integrated into the model 9. The field is most strongly enhanced near the sharp tip of
is determined using a hyperbolic tangent function. This the needle tip (7 × 108 V·m−1). This enhancement is
function increases quickly but smoothly, as shown in Figure adequate to induce local ionization in the oil and the
8 and expressed as follows:. immediate localization of main activities in the region of
the needle tip. The initial simulation is conducted at
V=90×tanh (1×1013×t [1/s]) kV. (19) atmospheric pressure (0.1 MPa) and at room temperature
(300 K).
4.2 GOVERNING EQUATIONS
The molecular ionization that is dependent on the electric
field directly ionizes streamer discharge. In this mechanism,
a highly electric field extracts an electron from a neutral
molecule. It then generates a free electron and a positive ion.
Negative ions are formed through the attachment of
electrons to neutral molecules in oil and to neutral NPs.
Thus, the drift-dominated equations of charge continuity for
the positive and negative ions, negative NP, and electron
are included in the model of molecular ionization that is
dependent on the electric field along with Poisson’s
equation [5]. These equations are given as follows:
( r 0 V ) e + NP ; E V (20)
e Re ( NP ) R
Figure 7. Geometrical model of positive streamer discharge.
t
E GI ( E )
e
e
(21)
100
e e Re e
80 t
e e E GI ( E )
e
a (22)
Applied step voltage(kV)
e
1 H (| NP || NPsat |)
60 NP
R
40
t
a e
E e
(23)
20
NP R
t
NP
NP NP E e 1 H (| NP || NPsat |) NP NP
e
0
0 0.2 0.4 0.6 0.8 1 (24)
Time(s) -12
x 10
Figure 8. Waveform of the step voltage applied to the needle electrode. where εr and ε0 are the relative permittivities of transformer
oil and the permittivity of vacuum, respectively, (ρ+, ρ-, ρe,
ρNP), (μ+, μ-, μe, μNP) are the charge density, and the drift
mobility of positive ion, negative ion, electron and
negatively charged nanoparticle. GI ( E ) is ionization
source, a (200ns) and NP (2ns) are the electron
attachment time to neutral molecules and nanoparticles,
respectively.
The model considers the trapping of electron carriers by
NPs according to the Heaviside function used in equations
(22) and (24). When the density of a negatively charged NP
Figure 9. 2D plot of Laplacian electric field distribution (i.e., 2 0 ) is lower than its limit ( | NP | | NPsat | , H | NP || NPsat | =0 ),
in the needle–plate electrodes (40 µm radius). The earth electrodenot the NP continues to charge. By contrast, the charging
shown here has the following properties: r = 0, z = 0 mm. process stops when the NP is saturated with negative
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 22, No. 1; February 2015 387
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[8] Y. Du , Y. Lu, C. Li, M. Chen, J. Zhou, X. Li, and T. Liu, Wenxia Sima was born in Henan province, China,
on 13 July 1965. She graduated from Chongqing
“Insulating Property and Mechanism of Semiconducting
University in 1988 and obtained the Ph.D. degree
Nanoparticles Modified Transformer Oils”, Proc. Chinese Soc.
in 1994 from Chongqing University. Her
Electr. Eng. (CSEE), Vol. 32, No. 10, pp. 177-182, 2012 (in employment experience includes the college of
Chinese). Electrical Engineering of Chonging University. Her
[9] Y.-X. Zhou, Y.-S. Wang, J.-H. Tian, Y. C. Sha , X. X. Jiang, S. Y. fields of interest include high voltage outdoor
Gao, and Q. Nie, “Breakdown Characteristics in Transformer Oil insulation and overvoltage protection
Modified by Nanoparticles”, High Voltage Eng., Vol. 36, No. 5, pp.
1155-1160, 2010 (in Chinese).
390 W. Sima et al.: Effects of Conductivity and Permittivity of Nanoparticle on Transformer Oil Insulation Performance
Jian Shi received the Bachelor degree in electrical Sisi Huang received the Bachelor degree in
engineering from Chongqing University in 2009. electrical and electronic engineering from
He is currently a Ph.D. candidate in the State Key Huazhong University of Science and Technology in
Laboratory of Power Transmission Equipment & 2010. She is currently a postgraduate student in the
System Security and New Technology, Chongqing State Key Laboratory of Power Transmission
University. His research interests include the Equipment and Security and New Technology,
measurement of space charge in liquid based on Chongqing University. Her research interests
Kerr effect and theoretical work on streamer include the measurement of space charge in liquid
discharge in liquid. based on Kerr effect.