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ABSTRACT
Room temperature vulcanized (RTV) silicone rubber coatings are used increasingly on
outdoor high voltage (HV) insulators subjected to heavy pollution. An important
property of the RTV coatings is the ability to restore the surface hydrophobicity after a
pollutant layer has built up on the surface, which can suppress the development of
leakage currents, dry band arcing and flashover. The present study analyzes the
hydrophobicity and the hydrophobicity transfer of RTV coatings and the factors that
affected the hydrophobicity. A modification of absorption and cohesion theory was
used to analyze the hydrophobicity transfer mechanisms and the influences of
temperature, polydimethylsiloxane (PDMS) molecular weight, degree of cross-linking,
extent of soluble and non-soluble components, and the pollutant properties. The
hydrophobicity transfer of RTV coatings was also investigated with various conditions
of contaminations and various factors, which affect the hydrophobicity transfer,
including the composition of RTV coatings and the outside conditions. Results show
that the hydrophobicity transfer of RTV coatings is not only dependent on
compositions but also on factors of circumstance. The analysis also explains the obvious
difference between the hydrophobicity transfer of RTV coatings to kieselguhr and
kaolin based on a particle and surface analysis using the Brunauer, Emmett and Teller
(BET) method, which explains the relationship between a BET surface area and the
hydrophobicity transfer of the RTV coatings.
Index Terms — RTV silicone rubber, hydrophobicity, absorption and cohesion.
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1318 Z. Jia et al.: Study on Hydrophobicity Transfer of RTV Coatings Based on a Modification of Absorption and Cohesion Theory
hydrophobicity and hydrophobicity transfer, which can restore protractor. For silicone rubber surfaces, the contact angle is
the hydrophobicity after a pollutant layer has built up on their approximately 100°, while for glass and porcelain surfaces,
surface. Numerous investigations [9-18] to describe the the contact angle is not more than 40°.
hydrophobicity mechanism have shown that the diffusion and The surface hydrophobicity is not a static property. The
transfer of low molecular weight (LMW) silicones in the hydrophobicity can be lost and recovered according to the
polymer from the bulk to the surface plays a decisive role in the surface conditions, the silicone rubber properties and the
hydrophobicity recovery. The LMW components are produced in outside conditions. Since the hydrophobicity transfer is the
both the polymerization of the silicone rubber and its degradation. most important property affecting the performance of RTV
Some previous researches have indicated that the silicone rubber coatings, the contact angle was measured at certain elapsed
is the single factor explaining the hydrophobicity and time in various test conditions. A hydrophobicity transfer
hydrophobicity transfer. The influences of thickness, substrate curve defined as a function of contact angle with time was
type, amount of silicone fluid, and solvent type on the then used to represent the hydrophobicity transfer of the RTV
electrical performance of RTV silicone rubber coatings have coatings.
also been investigated [19, 20]. However, most of these
hydrophobicity transfer investigations processed on RTV
coatings have neglected the influences of outer factors and the 3 ABSORPTION AND COHESION THEORY
dynamics of the LMW components which are the key parameters
affecting the outdoor insulating performance of RTV coated The first and the second laws of thermodynamics can be
insulators. used to indicate that a gas will be absorbed when it contact
with a solid surface. The absorbed amount on the solid surface
In the present study, the theory of absorption and cohesion per gram V is related to the gas and the solid surface
between a solid and air was modified to explain how deposited properties, the absorption equilibrium temperature, T, and the
contamination on a RTV coated surface can acquire the pressure, P.
hydrophobicity and to summarize factors which will affect the
hydrophobicity transfer. V= f (T, P, gas, solid) (2)
The attached forces of the solid surface will attach and hold
gas molecules to the solid surface; however, the attached gas
2 DESCRIPTION OF HYDROPHOBICITY molecules are not stationary in the center of the solid surface.
AND HYDROPHOBICITY TRANSFER The gas adsorbed molecules can move freely even
A hydrophobic surface is a surface that is not easily wet, on perpendicular to the solid surface even if there are strong
which water does not form a continuous film but forms interactions between the gas and the solid surface.
individual droplets. For outdoor insulation, the most important
properties of silicone rubber are its hydrophobicity and 3.1 ABSORPTION OF MONOLAYER
hydrophobicity transfer. If the solid surface is very smooth and the gas is absorbed
The hydrophobicity of surfaces is determined by the ratio of as a single layer of molecules, the absorption rate is inversely
the cohesive tension of water to the adhesive tension between related to the gas pressure. If the gas pressure is P and the
the water and the solid material. The simplest way to quantify percent of molecules without gas on the solid surface is 0, the
the hydrophobicity of a surface is by measuring the static absorption rate, Ra, can be expressed as:
contact angle of a water droplet on the surface. The contact
θ0
angle is defined as the angle formed between the tangent to Ra = a
the water droplet and the horizontal surface through the liquid, P (3)
c in Figure 2. The contact angle depends on the interfacial Where a is a proportionality factor.
forces on three boundaries, sw (between the solid and the
The desorption rate is directly related to the percent of solid
water), wa (between the water and the air), and as (between
molecules attached to gas molecules, , and the percent of
the air and the solid), which are related by the Young’s
attached gas molecules with sufficient energy to separate from
equation:
the solid molecules. Assuming that the minimum energy to
as = sw + wa cos c (1) separate from a solid molecule is a, which is the heat of
absorption, the number of attached molecules, Na, and the
percent of molecules, Na*, with energies over a is:
N a*
= fe ε a kT (4)
Na
Figure 2. Illustration of the interfacial surface tensions and equilibrium where f is a proportionality factor and k is the Boltzmann
contact angle in the Young’s equation. constant. The desorption rate, Rd, can then be expressed as:
R d = a 'θe ε a kT
(5)
In the static contact angle tests, a droplet of distilled water
(2.5 ± 0.5 s/cm) with a volume of 10 L was dropped on the where a’ is a proportionality factor and is the percentage of
test surface, and then the contact angle was measured with a solid molecules with attached gas molecules on the surface.
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IEEE Transactions on Dielectrics and Electrical Insulation Vol. 13, No. 6; December 2006 1319
When the absorption and desorption rates are equal: colloid, they are in contact or at a very short distance. Focused
θ0 on the hydrophobicity transfer between the RTV coating and
a = a'θe ε a kT (6)
the pollutants, the process of the pollutants acquire the
p
hydrophobicity is the same process that pollutants adsorb the
The sum of the percentage of solid molecules with gas on colloid matter, viz. the LMW. During this process, the
their surfaces, , and the percentages of the molecule without pollutants deposited on the surface of silicone rubber are
gas on their surface, 0, must be 1: solids, while the LMW acts as the colloid. Since RTV
0+ =1 (7) coatings mainly consists of the main polymer (PDMS), the
Therefore combining the equation (6) and (7) gives the catalyst, the cross linking agent and the fillers, the properties
absorption percentage as of the colloid, such as the LMW that exists in the coatings,
b will also be affected by these parameters. Since the catalyst
θ= strongly influences the vulcanized process but has less effect
b+P (8) on the LMW, the colloid properties are mainly affected by
a −ε a kT other parameters. Therefore, the degree of cross linking, p,
where b is e .
a' which describes the LMW movement, will be used to replace
the parameter P in equation (2), with the adsorption and
3.2 ABSORPTION OF MULTIPLE LAYERS cohesion between the solid and the colloid assumed to be
Since Brunauer, Emmett, and Teller carried out a derivation functions of the temperature, T, the degree of cross linking, p,
of the isotherm equation for multiple layers adsorption by a the colloid properties and the solid pollutant properties:
method that is a generalization of Langmuir's treatment of the V= f (T, p, colloid, solid) (12)
monolayer [21], the absorption occurs as cohesion of the Equations (4) to (11) can also be modified by replacing the
second and additional layers to the first layer with the heat of gas pressure, P, with the degree of cross-linking, p. Thus, the
absorption equal to the heat of cohesion, if the solid surface is absorption is directly related to the environmental temperature,
smooth and the gas is absorbed as several layers of molecule. the cross linking of the polymer, and the properties of the
When the absorption reaches equilibrium, the absorption colloid and the solid pollutants.
rate on the second layer is equal to the desorption rate of the The solid parameters include the particle sizes and surface
first layer. And the absorption rate on each layer i-1 is equal areas, which can be represented by a parameter defined as
to the desorption rate on layer i. If i (i = 0, 1, 2 …) is the surface areas per unit weight. Generally, a big solid piece with
percentages of molecules in layer i with total molecules, the a regular shape has a small surface area per unit weight since
adsorption and desorption rates for each layers are related by: the surface area of the solid is proportional to the square of the
θ diameter, while the weight of a solid is proportional to the
a1 0 = a1'θ 1e ε kT 1
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1320 Z. Jia et al.: Study on Hydrophobicity Transfer of RTV Coatings Based on a Modification of Absorption and Cohesion Theory
the same as the normal coatings developed in the lab but little molecular weight on the contact angle. Four these conditions
changed with one variable at active but others fixed. with four PDMS molecular weights, the larger PDMS
The 0.5 mm thick, 15 cm long and 7.5 cm wide RTV coating molecular transferred the hydrophobicity more effectively to
was applied to a glass plate. Then a pollution layer with a non- the pollutant layer.
soluble deposit density (NSDD) of 1.0 mg/cm2 was then Degree of cross linking The amount of cross linking agent
deposited on the specimens to analyze the hydrophobicity was expressed as the percentage of the PDMS in the tests.
transfer. Kieselguhr and kaolin were used as the pollutant Figure 4 shows that the pollutant layer acquires the
according to the recommendations IEC 60507 [22]. hydrophobicity more slowly on specimens with larger
amounts of cross linking agent, which increases the degree of
4.2 EXPERIMENTAL METHOD cross linking that will slow the molecular movement and
The effects of temperature, molecular weight of the PDMS, reduces the hydrophobicity transfer.
degree of cross linking and contamination type on the
Table 1. Effect of temperature on the hydrophobic transfer
hydrophobicity transfer of the RTV coating were studied through
the hydrophobicity transfer test. Temperature 2 17 60
Temperature The temperature affects the movement of Time for hydrophobicity transfer h 30 16 2
molecules on the surface which influences the hydrophobicity
transfer, the effect of temperature was investigated using
temperature at respectively chosen at 2, 17, and 60 . 120
0
Contact angle /
determined from its viscosity. Four kinds of PDMS with
various molecular weights were used to study the effect of the 60
PDMS while keeping other parameters constant.
40 148000 mPaS
Degree of cross-linking The catalyst and cross linking agents
are also important ingredients in the RTV coatings, which will 11300 mPaS
20 4800 mPaS
not form a film without them. The cross-linking agent controls 3000 mPaS
the degree of cross-linking in the coating. These tests used a 0
fixed kind of PDMS with 11300 mPaS, but the various 0 10 20 30 40 50 60 70
amounts of cross-linking agent. Time / h
Soluble and non-soluble pollutant components The first set
of samples used a NSDD at 1.0 mg/cm2 (kieselguhr and kaolin Figure 3. Hydrophobicity transfer of samples with various PDMS molecular
respectively) and various NaCl densities (equal soluble weights. NSDD: 1 mg/cm2.
deposit densities, ESDD) of 0, 0.05, 0.1 and 0.2 mg/cm2 in the
contaminated layer. The effect of deposit density on the
hydrophobicity transfer was investigated using kieselguhr 160
with NSDD of 0.5, 1.0, 1.5, 2.0 and 3.0 mg/cm2 respectively. 140
120
5 RESULTS AND DISCUSSIONS
0
100
Contact angle /
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IEEE Transactions on Dielectrics and Electrical Insulation Vol. 13, No. 6; December 2006 1321
kaolin surface, which is only about 100°. Increases in ESDD electrons to the incident electrons to be unity. If this ratio is
slowed the acquisition of the hydrophobicity. For the greater than unity, the surface becomes positively charged as
kieselguhr, the NaCl content had little effect on the final indicated by a white image on the screen. When this ratio is
contact angle for the ESDD below 0.2 mg/cm2, while for less than unity, the surface becomes negatively charged as
kaolin, the final contact angle was reduced by about 10° when indicated by a black image on the screen. The energy of the
the ESDD was increased from 0.05 mg/cm2 to 0.2 mg/cm2. incident beam is varied gradually until cross over occurs. The
SEM used in the present study was a JEOL JXA-840 machine.
Figure 7 shows SEM photographs of kieselguhr with and
140
without hydrophobicity. Figure 8 shows SEM photographs of
D Kieselguhr kaolin with and without hydrophobicity.
120
100 C
Kaolin
o
Contact Angle /
80 H
A: ESDD-0.2
B B: ESDD-0.1
60
G C: ESDD-0.05
D: ESDD-0
40 E: ESDD-0.2
A
F F: ESDD-0.1
20 G: ESDD-0.05
E H: ESDD-0 (a) Virgin kieselguhr (b) hydrophobic kieselguhr
0
1 10 100 1000 Figure 7. Structure of kieselguhr with and without hydrophobicity.
Time / h
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1322 Z. Jia et al.: Study on Hydrophobicity Transfer of RTV Coatings Based on a Modification of Absorption and Cohesion Theory
the particle sizes. The data show that the particle sizes of Since the kieselguhr and the kaolin are normally deposited
kieselguhr were reduced after acquiring the hydrophobicity as on the surface with distilled water in the artificial pollution
some organic matters filled in the holes. Figure 10 shows the test and the hydrophobicity transfer test, to avoid the effects of
particle distribution of kaolin with and without hydrophobicity distilled water on the results of BET surface area analysis, the
with Table 3 giving the statistical distribution of the particle original BET surface area of pollutants, BET S1, and the
sizes. The particle sizes of the virgin kieselguhr are bigger than treated BET surface area of pollutants with immersed in
the particle sizes of virgin kaolin, which might be a reason why distilled water, BET S2, were measured respectively, as listed
the kaolin acquires hydrophobicity slower than the kieselguhr. in Table 4. Results show that the distilled water has little
The results also show that the particle sizes of the hydrophobic effects on BET surface area though the BET surface area
kaolin are increased due to the conglobation and the increased little, and the increase trends on three samples are
hydrophobicity transfer. similar. Therefore the effects of distilled water during the test
Table 2. Particle sizes of kieselguhr in various states
can be ignored in the following study. From Table 4, the BET
virgin with hydrophobicity surface areas of pollution powers are different with the
Particle Size of
probability distribution / m / m amount of the pollutant contents, which means the BET
surface area is a function of the pollutant. So the relationship
d(0.1) 2.884 4.495
between the BET surface area and the hydrophobicity transfer
d(0.5) 14.192 13.867 of RTV coatings was studied.
d(0.9) 49.779 36.414
6 Virgin kaolin
Virgin kieselgur With hydrophobicity
6
With hydrophobicity 5
5
4
4
Volume /%
Volume /%
3
3
2
2
1
1
0
0
0.01 0.1 1 10 100 1000
0.1 1 10 100 1000 Particle size /μm
Particle size/μm
Figure 10. Particle distribution of kaolin with and without hydrophobicity
Figure 9. Particle distribution of kieselguhr with and without hydrophobicity
Table 4. BET surface of kieselguhr, kaolin and their mixture
Table 3. Particle sizes of kaolin in various states Kieselgur Kaolin BET S1 BET S2
Particle Size of virgin with hydrophobicity /% /% / ( m2 / g ) / ( m2 / g )
probability distribution / m / m Pollutant A 100 0 2.74±0.04 2.84±0.05
d(0.1) 1.690 18.783 Pollutant B 0 100 24.16±0.06 24.89±0.24
d(0.5) 6.106 191.74 Pollutant C 50 50 12.55±0.08 13.34±0.11
d(0.9) 32.812 1046.153
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IEEE Transactions on Dielectrics and Electrical Insulation Vol. 13, No. 6; December 2006 1323
transfer than the pollutants with large BET surface areas. surface, the interaction between the liquid and the solid is also
Therefore, the BET surface might be a key reason for the related to the BET surface area since the pollutants are
different hydrophobicity transfer rate between kaolin and commonly hydrophilic. To restrain this interaction and
kieselguhr. represent hydrophobicity, more LMW components are
required to cover the pollutant surfaces. Some points should
be emphasized here that this conclusion applies only to the
small pollutant particles with micro-structures and similar
140
particle diameters. If the particle diameters are too large, the
120 LMW components will have to move a long distance so the
A surface can not easily acquire the hydrophobicity.
100
o
Contact angle /
B
80
6 CONCLUSION
C
60
A : Kieselguhr-100%, Kaolin-0% The RTV coatings can transfer the hydrophobicity to the
D contamination deposited on their surfaces. Based on the
40 B : Kieselguhr-75%, Kaolin-25%
E C : Kieselguhr-50%, Kaolin-50% modification of absorption and cohesion theory, the
20 D : Kieselguhr-25%, Kaolin-75%
E : Kieselguhr-0%, Kaolin-100% hydrophobicity transfer of RTV coatings is found to be related
0 to many factors, including the temperature, the ingredients of
1 10 100 1000
silicone rubber, the degree of cross linking, the content of the
Time / h soluble salt and the type of contamination. The results also
show that the hydrophobicity transfer of RTV coatings is
Figure 11. Hydrophobicity transfer of various mixture samples. NSDD: 1 related to the micro-structure of the pollutants. The SEM,
mg/cm2, ESDD: 0.1 mg/cm2. particle analysis and BET analysis results show that the
Table 5. Components of mixed pollutants kieselguhr acquires the hydrophobicity more quickly than the
Kieselgur Kaolin Cement kaolin due to its micro structure with many small which
/% /% /% creates a particle distribution, BET surface area, and
Pollutant #1 100 0 0 absorption and cohesion properties that improve the
Pollutant 2 #
0 100 0
hydrophobicity transfer of RTV coatings. The BET surface
area is an important parameter of pollutants representing the
Pollutant #4 50 0 50
absorption capability of the solid surfaces, which will affect
Pollutant #5 0 50 50 the hydrophobicity transfer of the RTV coatings and can be
Pollutant 6 #
0 0 100 changed by various pollutants and the amount of the pollutant
contents. The hydrophobicity transfer to pollutants with larger
BET surface areas takes longer on same RTV coatings.
140
ACKNOWLEDGMENTS
120 The authors acknowledge the financial support from the
100 National Natural Science Foundation of China (No.
o
1
Contact Angle /
4
50277022). The authors also would like to thank the Analysis
80 Center of Tsinghua University for doing some of the
6 measurements.
60 #
1: Pollution 1
#
40 2: Pollution 2
2 #
4: Pollution 4
#
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20 5 5: Pollution 5
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