Rev.Adv.Mater.Sci. 16(2007) pp.

10-24

Hydrophobicity of Silicone Rubber Used for Outdoor Insulation (An Overview)

Salman Amin, UET Taxila, Pakistan. ABSTRACT: Among the new insulating materials widely used in high voltage outdoor insulations systems, silicon rubber materials also called polymeric materials are very important ones. These have been widely used since last 20 years for making outdoor insulators. These materials are organic in nature and are prone to decomposition under different environmental conditions. The most important of these when considered w.r.t. to high voltage electrical insulation is the Hydrophobicity which is resistance to formation of conducting water tracks which in turn increases leakage current activity, chances of flashover and other deterioration effects. The superior contaminant performances of polymer outdoor insulating materials are regarded as the contribution of their hydrophobic surfaces. In other words it is the formation of water beads on surface which resists the flow of water in continuous conducing track. In this paper hydrophobicity theory, its importance for polymeric silicon rubber insulators, methods of hydrophobicity measurements especially by leakage current, low molecular weight component chains responsible for hydrophobicity recovery, chemistry of hydrophobicity loss and recovery, hydrophobicity recovery related with temperature, humidity, UV radiation, corona, electric field and dry band arcing are overviewed from materials point of view. Keywords: - Leakage current, Contact angle, Dynamic LMW chains, Out door high voltage insulators. 1.0 What is Hydrophobicity? Hydrophobicity of any material is its resistance to flow of water on its surface. A material is highly hydrophobic if is resists flow of water dropped on it and is least hydrophobic if dropped water flows in form of tracks on its surface. One showing behavior intermediate between the above two has specific contact angle of water on its surface. The hydrophobic surface is water repellent contrast of which is a hydrophilic surface that is easily wetted. The contact angle (c) that liquid drop makes when it comes into contact with a solid surface is a measure of the surface wettability. The material which is easily wettable allows water to touch a large surface area and hence makes a contact angle of less than 90 degree and a material which resists to wet its surface allows less water surface contact and thus makes a contact angle greater than 900 as shown in Figure 1.
A) Hydrophobic surface. B) Less Hydrophobic surface

The contact angle gives information about surface energies, surface roughness, and surface heterogeneity. Contact angle is also a measure of the surface contamination. The surface hydrophobicity of insulation material is often quantitatively evaluated by the value of contact angle formed between water droplet and material surface, which is direct representation of the tension between interfaces of water and the material atoms [38]. The shape of the liquid droplet depends on the material of the solid and the physical and chemical states of the surface. It is made clear in Figure 1 that the smaller the contact angle surface is more wettable and vice Versa. If the contact angle of the liquid on the surface is less than 350 is assumed to be hydrophilic. For contact angles greater than 900 the surface is assumed to be hydrophobic. Between 350 and 900 the surface is partially wettable. It should be also clear that term hydrophobic represents resistance to water but it is used generally to represent resistance to any liquid. 2.0 Importance of Hydrophobicity for Polymeric Insulators The most of all obvious drawback of reduction in hydrophobicity for an electrical insulator is increase in surface leakage current activity and increased dryness of surface due to this. This is a major insulation performance factor for ceramic insulators, but when we say about polymeric or non-ceramic insulators

Figure 1:- The shape of a liquid Droplet on a

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hydrophobicity loss or reduction causes other serious effects also as discussed now. Hydrophobicity affects the polymeric silicon rubber materials/insulators in two ways. Firstly loss of hydrophobicity causes reduction in electrical insulation and pollution withstand performance. Secondly it also prominently influences the aging process of SIR insulators [1]. For polymeric insulators operating in polluted condition, hydrophobicity involves two types of measurement. Static hydrophobicity measurement and dynamic hydrophobicity measurement. Static hydrophobicity means hydrophobicity of raw material or hydrophobicity of material under normal constant magnitude of stresses. Whereas the dynamic hydrophobicity measurement involves monitoring of hydrophobicity transfer, loss and recovery. The mechanisms involved in parameters causing dynamic change in hydrophobicity transfer, loss and recovery are not clear up to now. Therefore, counter measures to improve the design, selection and maintenance of operating Silicon Rubber insulators are not successful till now. Many investigations are in progress systematically, to learn the actual hydrophobicity status of SIR insulators in various polluted areas [2, 3]. All have the aim to provide guidance to power companies for the usage and maintenance of composite insulators in contaminated areas. Results from various testing sites show that all insulators still preserve very good hydrophobicity properties even after ten years operation in some heavily polluted areas. It is interesting that a clear correlation exists between the deterioration of hydrophobicity and the local strengthening of electric field. On the basis of the new findings in the field, detailed laboratory research on hydrophobicity transfer, recovery and loss properties have been conducted concurrently [9,10, 22, 23] The aging test continuing in artificial, normal outdoor and heavily polluted environment of Pakistan also includes measurement of hydrophobicity using STRI classification and leakage current measurement techniques. Three years aging performed in extremely polluted field of Pakistan have shown various results of hydrophobicity ranging from HC1 to HC7 [33]. From results one plate of rubber material showing extreme hydrophobicity loss (HC6 to HC7) and another plate of same material which maintained good hydrophobicity in same conditions are shown in Figure 2. This figure Is showing surface of insulating material under water spraying for hydrophobicity classification as discussed in section 3 following. The results reported from Pakistan also verify the fact that more the surface area, more are chances

of hydrophobicity loss as compared to less surface area samples of same material. But this fact does not requires to pay much attention for manufacturers because insulators are always in round shape, and hence cylindrical surface has least surface to volume ratio, so we can safely say that all circular shapes are best suitable for insulator construction and this is already a practice followed by manufacturers since long.

Figure 2:- The hydrophobicity of two different silicon

rubber plates tested in field environment of Pakistan. A) Extreme Loss of hydrophobicity (HC 7). B) Good Hydrophobicity (HC 2)

The Figure 2 also provides a clear way to understand what happens to leakage current activity over the surface of a material with high loss of hydrophobicity under rain. The water tracks a shown in figure 2 (A) provide a clear continuous path for current under rain conditions and obviously this may easily lead to flashover causing major degradation. The surface of un aged (Un-exposed to environment) composite (Silicon rubber) insulators shows a hydrophobic behavior. In pure state the various material groups such as RTV, HTV, EPDM etc., vary slightly in surface roughness, hydrophobicity or axial molding line. Silicon rubber when exposed to environmental conditions and/or partial discharges, their hydrophobicity is reduced. An excellent advantage of SIR consists is its high resistance to retain its hydrophobicity even after removal of harsh conditions. In case of a temporary reduction or loss, the hydrophobicity will recover. The dynamic processes behind this recovery are more or less summarized by the term 'recovery'. This is discussed in following sections with detail.

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3.0 Methods of Hydrophobicity Measurement There are many methods; some widely used methods will now be discussed. 3.1 STRI Hydrophobicity Classification It is a simple procedure for manually obtaining a collective measure of the hydrophobic properties of insulating surfaces in outdoor environment. For practical purposes the degree of the water repellency of an insulator surface may be divided into seven hydrophobicity classes (HCs) according to the STRI classification guide [40, 41]. HC1 is the most water repellent class whereas HC7 refers to completely hydrophilic surfaces. The intermediate classes are defined by receding angles of the majority of the droplets and size of wetted areas in each case. One of the manual methods for obtaining a measure of hydrophobic properties of surfaces is STRI hydrophobicity classification valid for use in outdoor environment. First, the surface to be studied (50-100 cm2) is sprayed with water. The obtained drop pattern is observed and attributed to one of the seven hydrophobicity classes. As help, the examiner has a set of reference images of typical wetting patterns representing each HC class [2, 12, 23]. Disadvantage of the method is that the measure is dependent on human judgment. To deal with this problem digital image analysis is used. In such a procedure, computer software interprets the image, taken by a high resolution digital camera, makes the examination while increasing its accuracy. To deploy and calibrate the software for this method aged samples can be used or artificial methods like sand blasting can be used which reduces hydrophobicity to HC7 in short time. Then the images of these samples can be taken and imported in software to calibrate image analysis for the first time. One thing to consider while spraying for hydrophobicity test is to keep samples at inclinations of 10 to 35 from the horizontal. These inclinations should be chosen as they represent well typical inclinations of insulator surfaces in actual service. In order to make measurements comparable all directions and distances between camera, illumination levels and sample position should also be fixed. To take this factor in account taking a large number of photographs for each HC is a good practice. Reliability of image analysis by softwares increases if the images are stored and reviewed at least twice at different times. Tokoro et al [16] have also applied image analysis to study hydrophobic properties of SIR. , they used a high-speed camera equipped with a high

magnification lens to observe behavior of water drops on small areas (1.5 x 1.5 mm). Small drops were chosen as influence of gravity became low compared to the effect of surface free energy, and thus problems associated with varying inclinations could thus be reduced. SIR samples were immersed in distilled water for different times to reduce hydrophobic properties. Images, made after the samples had been exposed to mist of different solutions, were analyzed with respect to size and shape distributions of created droplets. Observation was that more smaller and circular drops are formed on hydrophobic surfaces as compared to hydrophilic surfaces [16, 25]. 3.2 Sessile Drop Technique The hydrophobicity of silicone rubber materials is also measured by measuring contact angles between the material and water drops on its surface. The most commonly used method is the so-called sessile drop technique. In this technique a water drop is placed on the surface using a syringe. The static contact angle is then measured manually using a goniometer or in an image using a camera fitted to a microscope or a computer with some image analysis software like MATLAB etc. Addition of more water drops on an already sprayed surface results in an increase of contact angle, finally causing the drop to advance over the surface. This angle is called advancing contact angle. Similarly, the angle at which the drop starts to recede during removal of water is called receding contact angle. The difference between these two angles depends on parameters like: surface roughness, surface heterogeneity, contact time of surface and water, and drop volume. There is correlation between tropical weather of natural environment and the contact angle. The pollution accumulates on the surface to result a contact angle increase rapidly due to the higher roughness of the surface. The samples having lower pollution on surface result in lower contact angle. On the contrary, some of the sample types which were exposed with shielding showed slightly increases their contact angles. These phenomena indicated that the natural pollutants strongly affect the change of the contact angle of silicone rubber. The sessile drop method is applicable in laboratory environment only, since it requires good illumination and optimal view of single drops on flat horizontal samples. This lack of methods for estimating hydrophobicity of insulators in the field led to popularity of STRI hydrophobicity classification method.

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The receding contact angles measurements of different polymer materials before and after being dripped in artificial acid rain in a lab aging chamber at UET Taxila, Pakistan are shown in Table 1. The value of contact angle for virgin sample is also mentioned against each material type. The contact angles decrease with soaking time in the solution of acid rain in to some extent. It is clear that the surface hydrophobicity of insulator also becomes worse with decease in receding contact angle measurement.
Material HTV SIR Plate HTV SIR Reinforced Rod RTV SIR Plate Epoxy Virgin 960 1080 1120 1040 Receding Contact angle measurement Ist 2nd 3rd Average 930 880 940 91.60 0 0 0 93 91 101 9500 1060 920 104 900 990 930 1030 91.60

The most popular method for continuous unattended monitoring of hydrophobicity changes under energized conditions in field or lab aging is use of leakage current. There are three reasons for this. 1) Leakage current is directly proportional to hydrophobicity loss. More the loss of Hydrophobicity more the leakage current becomes. This has been reported from many sites [10, 17, 20, 22]. It as parameter that follows change in hydrophobicity properties very dynamically. So reduces the error as involved in other methods due to delay in measurements. The method of leakage current monitoring is costly as compared to STRI Classification but very cheap as compared to SEM, Kerr effect measurement etc. The procedure is without having need to use complex image processing software or do programming for image matching as required in sessile drop or STRI methods if done with a computer. The measurement of leakage current just needs the computer to record its values after a certain time intervals or after some certain changes in value of current as discussed in following.

2)

3) Table 1:- Change in receding contact angle measurement of different surfaces. Three readings are taken for each sample to get an average value. 3.5 Other methods to Monitor Hydrophobicity changes. The effect of hydrophobicity can be quantified by many other methods such as sensitive optical measurements of surface utilizing Kerr effect, by Hydrophobic Interaction Chromatography (HIC), by salt aggregation test (SAT), by electrical values such as leakage current, flashover voltage measurement (also called cross over voltages COV), by water immersion tests etc. 3.6 Instructions for Hydrophobicity Measurements. Hydrophobicity measurements of any surface whether done by Sessile drop or STRI method should be done immediately if samples are removed from a field. However, if it is measured by leakage current or COV method, while using a chamber in laboratory or special purpose test station in outdoor environment it can be done directly on surface and no delay time is involved. The requirement to do this early is because of very dynamic nature of surface of silicon rubbers. This dynamic behavior immediately starts to recover surface hydrophobicity when stress is removed and may have changed to a large value if a sample removed from field is analyzed later and this leads to false results or unreliable good performance predictions[50]. 4.0 Hydrophobicity Monitoring using Leakage Current Activity.

Many methods of measurement of leakage current to monitor hydrophobicity loss have been reported in literature. The most easy and typical approach is to deploy a current transducer in series with insulator at dead end and measure the voltage across it by a precision amplifier and record them manually after a few days period or by a computer after any desired interval. The measurement by a computer involves conversion of analog volt reading to digital and then to RS232 format. This all can be easily done by cheap hardware. The reading is imported in computer software by reading its ports and saving it in some file. So the reading reaches in computer continuously. A typical issue which arises is the interval between two readings stored. If reading after every five seconds is stored it results a huge record for a month. Since computers today are still large in storage to hold such data for years but analysis and utilization of such a huge data about leakage current is impossible. So a very common practice adopted by many researchers all over the world is to save a reading only if exceeds a certain level (say 10 micro ampere or so) [42]. This will result only those readings where some change has occurred due to change in surface properties of insulator. This is what meant by monitoring of current according to change in value as mentioned earlier. A typical of such apparatus setup is shown in Figure 4.

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There should be enough amount of LMW in total bulk so as to continue process of their diffusion for many years to maintain LMW concentration at surface. According to many laboratory tests most of the commercial silicone rubbers available today for making composite insulators have enough LMW to sustain excellent property of hydrophobicity transfer. The artificial increase of LMW, through artificially adding low molecule silicone oil into the raw silicone rubber, cannot remarkably improve the hydrophobicity property. However, effect of adding fillers like alumina trihydrate has been observed positive [2]. Material allowance for diffusion activity Figure 4:- A typical leakage current monitor system. There should be enough flexibility in silicon rubber material to allow a continuous activity of LMW diffusion. This flexibility depends upon content, cross linking and weight distribution of molecules in the raw silicone rubber. There is still large space left for the optimization of hydrophobicity performance through the good balance between these factors chemically. To get control over above two factors requires in depth knowledge of chemical engineering utilized accordance with recommendations of different researchers in this field. Physical & Chemical Properties of Pollutants If the two factors stated above are positively present it means insulator is ready to give LMW to pollution layer when it will be deposited, but the important thing is that will pollution also allow exchange of LMW from the bulk of insulator material? This solely depends on chemical & physical properties of pollution layer deposited. Pollution layer chemical proprieties and physical morphology can never be predicted nor artificially controlled, since it have to come from atmosphere and could be anything. How ever it can be anticipated in advance by choosing more insulation redundancy and extra cautions are necessary during the selection and maintenance. For SIR insulators, areas near alkali plants and the sea shores seem more severe due to higher content of salt and possibly less hydrophobicity. 6.2 Reason for LMW Diffusion The cause responsible for LMW diffusion is based on the fact that all systems try to minimize their total internal energy. This means that all atoms/molecules should be involved in as many intermolecular interactions as possible to achieve same level of energy throughout their distribution in that material. At

6.0 Chemistry of Hydrophobicity Transfer of LMW from inside bulk of SIR material to its surface can be thought of as combined effect of surface energy, filler type, pollution layer chemistry, thickness of pollution layer deposited, extent of electric field and energized to relaxed time ratio [50]. It has not been possible yet to formulate all or even a few of these effects in one strict relation, however a lot of work is in progress on evaluating equations representing transfer of LMW under three or four of these combined effects for two or three combined effects. However two major factors surface energy and pollution layer chemistry if considered reasonably represent LMW transfer phenomena. The affinity of pollution on the surface to increased leakage current and arcing does not completely suppress by diffusion of a few or a thin layer of LMW from the inside to surface, particularly in case of thick pollution and increased humidity. So to estimate, what will be transfer speed, whether or not the pollution layer deposited on the surface of silicone rubber will obtain sufficient hydrophobicity, and what will be the value of maximum final hydrophobicity achieved, we have to consider following factors. 6.1 Material Dependency 1) Physical & Chemical Properties of Rubbers Persistence of Mobile LMW Material allowance for diffusion activity 2) Physical & Chemical Properties of Pollutants Persistence of Mobile LMW

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surfaces and some interfaces the possibility for successful intermolecular interactions is heavily reduced to about half because no molecule can leave the material so this causes energy imbalance at surface or interfaces. This type of energy interface is called surface free energy if material is solid. For liquids is called surface tension, both these terms tell how much uncancelled energy is present on the surface or interface. An example of this can be illustrated by the binary and completely mixable system of water and glycol where it has been shown that the concentration of glycol is much higher in the surface layer compared with the bulk [22], in order to decrease the surface tension. In general, even for solid materials sufficient flexibility for intermolecular diffusion is present; the constituent with the lowest intermolecular forces will be enriched at the surface. Further, if one applies a liquid droplet on a solid surface, the surface tension will show repellence to liquid spreading or we can say surface will show good hydrophobicity [23]. Almost all types of Non polar organic materials have a free surface energy half or less as compared to liquid water, therefore, water will not spread on such surfaces. This low surface energy, for the same reason, also leads to low adhesion to solid particles, such as those brought by field pollution. Conclusion Pollution performance of polymer insulators is closely related to their hydrophobicity property. Pollution severity levels also play an important role. UV radiation and temperature contribute strongly to hydrophobicity transfer speed and gain of LMW by pollution layer. Heavy acidic rains reduce the speed of recovery of the hydrophobicity because of the breaking of LMW (by acid action) on surface or on pollution layer that has gained LMW. The pollutants effect on changing the contact angle of silicon rubber surface is very noticeable. It has been observed that more pollution on the surface results in increase in contact angle and also the surface roughness. In general, lower surface of sheds accumulates more pollutants than upper surface, and therefore, exhibits poor hydrophobicity It is confirmed by many authors [2, 15, 27, 34, 47] that hydrophobicity status has not any prominent relationship with the years of service. It only corresponds to the particular environment where it is investigated.

The sum of results achieved from experiments on hydrophobicity is that water droplets induced discharges are main reason for the hydrophobicity degradation of Silicon Rubber insulators in service [10, 6]. To achieve good performance of these insulators, electric field distribution should be equalized in all sections over the surface of insulator especially near the end-fittings. This can be done by increasing overall surface leakage distance or in other words decreasing the KVolt/ Cm stress over the surface. A suitable level is to keep it a maximum of 5-6 K Volt/Cm. References 1.
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