2004 Annual Report Conference on Electrical Insulation and Dielectric Phenomena

Comparison between Silicone Rubber containing Micro- and Nano- Size Silica Fillers
A. H. El-Hag S.H. Jayaram E.A. Cherney

Electrical and Computer Engineering Department University of Waterloo Waterloo. Ontario, Canada

Abstract: In this study the influence of nanesize silica filler is compared with micro-size filler in silicone rubber using the ASTM 2303 inclined plane tracking and erosion test. Silicone rubber samples filled with 5 pm mean size ground silica are compared with silicone rubber filled with 12 nm average size fumed silica. Both the low frequency components of leakage current and eroded volume are used to evaluate the performance of the two types of composites. While the fundamental component of leakage current does not correlate with the erosion, the third harmonic component of the leakage current shows good correlation to the erosion, in terms of volume, and for both composites. Based on the results of the eroded volume, it is observed that 10% by weight of nano-size filler in the silicone rubber gives a performance that is similar to that obtained with 50% by weight of micro-size filler. The paper discusses the merits of nano-size filler in silicone composites.

samples using the ASTM 2303 standard inclined plane IT. tracking and erosion test ( P ) A companion paper discusses the underlying physicochemical properties of fumed silica filled SIR composites [7].

Materials and Methods

The test procedure followed the ASTM 2303 standard, with an initial voltage of 2.0 kV and a constant contaminant flow rate of 0.15 mVmin for four hours [SI. The voltage was increased at a rate of 250Vhour. At the end of the test, the samples were taken from the test bay and the eroded volume was estimated by filling the eroded volume with a soft putty of known density. The weight of the putty was determined using a microbalance and used in the eroded volume calculations. The base rubber (elastomer) used was a two-component room temperature vulcanized (RTV) SIR material which contained no inorganic filler of any type. The filler typelconcentration used is presented in Table 1.
Table I: Chemical composition of the tested samples in IPI test.

Introduction
Silicone tubber (SIR) has been used as an insulating material for outdoor applications for more than 30 years. Compared to ceramic insulators, SIR insulators have advantages of g o d pollution performance, reduced weight and lower cost [I]. However, aging is still considered the main problem facing SIR insulators. To improve the aging performance of silicone rubber insulators various types of fillers are needed. Fillers are added to silicone rubber to reduce cost, improve dry band arcing resistance and to improve mechanical properties. Extensive research has been conducted to study the influence of filler size, concentration and type on the aging performance of SIR insulators f3-51. However, much of the previous efforts have concentrated on micro-size fillers. With the growing interest in using nano-size tillers in polymeric materials, the use of these fdlers could have a strong influence on the performance of SIR insulators. Although fumed silica has been extensively used for reinforcement of silicone rubber, its role on the erosion and tracking resistance has not been studied. This paper presents a comparison between nano-size silica filled SIR with micro-size silica filled SIR

A PC based data acquisition system, composed of voltage dividers, overvoltage and overcurrent protection circuits, and a 100 IcHz, 16-channel data acquisition card, recorded the source voltage, and voltage and current for each sample. During the test, for every second, four 60 Hz cycles of data were acquired at a sampling rate of 7580 samples per second. These four cycles were processed by the Fast Fourier Transform (EFT)technique for the leakage current (LC). Then, the LC current data were averaged and smoothed using the moving average technique. The software for analyzing

0-780585845/04/$20.00 m004 IEEE

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the data recorded by the data acquisition system was built on a LabVIEWC3 platform. The results presented in the following section are average values from three samples for each test case. Figure 1 shows the schematic of inclined plane setup and the data acquisition system.

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Figure I Experimenel setup [6]

Results and Discussion

Both the fundamental and third harmonic components of LC were monitored continuously for the nano- and micro- size silica filled SIR as shown in Figures 2 and 3. Also, the eroded volumes for all the tested samples were measured and are depicted in Figure 4. It is evident from Figure 4 that as the filler concentration increased, the eroded volume decreased. Also, the weight loss for a 10% nano-size silica filled SIR is comparable to a 50% micro-size silica filled SIR.
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Figure 3 Third harmonic component of leakage cUrren1 during the U T t e ~ f(a) (a) Nano-size filled SIR, (b) Micro-sire filled SIR.

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Figure 4 Comparison between micro- nan-size composites in terms of ercded volume.

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It is evident from Figures 2 and 3 that the fundamental component of leakage current does not show any difference between the tested samples regardless of the eroded volume. Also, the average value of fundamental However, the component saturates around 6 mA. 0 50 rw 150 203 250 levels of both the fundamental component of the LC, as r m c (rn,"ubn) well as the third harmonic component, are correlated (b) n Figure 2 Fundamental compOnent of leakage current during the F' with the degree of the surface erosion i a salt-fog test l [9]. This could be attributed to the controlled flow of test, (a) Nano-sire f i e d SIR, (b) Micro-size filed SIR.

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contaminant on the material surface in the P T , which results in a controlled surface resistance. On the other hand, the third harmonic component of the LC shows a better correlation with the eroded volume, Figure 3. This is because dry band arcing is well correlated to both surface damage and the thud harmonic of the LC [91. As reported in the companion paper, a TGA analysis was conducted on nano-size silica filled SIR and compared to unfilled SIR [7]. Also, the TGA analysis was conducted on micro-size filled silica samples as shown in Figure 5. Comparing the TGA results of nanoand micro- size silica filled SIR, Figures 5 and [7], as the filler concentration increases, the weight loss decreases in both composites. However, comparing the TGA results of nano- and micro- size silica filled SIR Figure 6 do not agree with the ET results. The TGA analysis show that both the 10% nano- and micro- size silica filled SIR materials show a reduction in weight of about 30%. On the other hand, the eroded volume for 10% nano-size silica filled SIR is about one sixth of its weight compared to micro-size silica filled SIR.

in Figure 7. There is a significant difference between the surfaces of the damaged nano- and micro-size silica filled SIR. While it was not possible to see the dispersion of the nano-size filler in the undamaged sample, Figure 7 d , the fumed silica tended to agglomerate during the dry hand arcing, forming a silica-like layer, Figure 7-c. The formation of this type of a layer was not apparent in the micro-size silica filled samples, as shown in Figure 7-a. It can therefore he stated that the formation of silica like layer with nanosize silica filled composites aids to resist further degradation of SIR during dry hand arcing.

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Figure 7 SEM Images for different SIR filled mterials: (a) Damaged

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Figure 5 E A h l y s i s for different micro filled silicone rubba
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10% micro-size silica fdled, (b) Undamaged 10% micro-size silica fdled, (c) Damaged 10% nano-sire silica filled, (d) Undamaged 10% nano-size silica filled.

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Conclusions
The third harmonic component of LC is well correlated with the surface damage of both micro-size silica filled and nano-size silica filled silicone rubber samples tested in IF'T test, although the fundamental component of LC is defined by the contaminant flow. Also, weight loss measurements using IF'T test results confirm that the nano-size silica filled SIR composites depict significant resistance to erosion compared to micro-size silica filled SIR composites with comparable amounts of fillers, by weight, in SIR.

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Figme 6 TGA Analysis fM 10%nano and micro f i e d sdicone rubba
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To further understand the difference between nanoand micro-size silica filled SIR, a detailed scanning electron microscopy (SEM) investigation was conducted on both the damaged and undamaged 10% nano- and micro-size silica filled SIR samples as shown

References
[I] R.S. GMU, E.A. Cherney and I.T. Burnham Outdoor Insulators, Ravi S. Gorur, Inc.,1999. Chapter 8.
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S. S i m n s . M . Shah, 1. Mackevich. and R. I. Chang. "Polymer Outdoor Insulating Materials Part III - Silicone Elastomer

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Considerations. IEEE Electrical Insulation Magazine. vol. 13, pp. 25-32, Sep/Oct 1997.
131 Deng, H.: C h e y , E.A.: Hackam R. Effects of panicles size of ATH fillers on the performance of RTV rubber coatings IEEE Electrical hulation and Dielectric Phenomena 0, Conference, pp. 598 6 4 1993.

141 Kim S.-H.; Cherney, E.A.: Hackam R.Therml characteristics of RTV silicone rubber coatings as a function of f i e r level IEEE CEDP-1992, pp. 713-718, 18-21/Octobed1992.

151 Meyer, L.; Grishko, V.; Jayaram S.; Chemey, E.; Duley, W.W. Thermal characteristics of silicone rubber filled with ATH and silica under laser heating IEEE CEIDP-2002, 2024/October/2002 .pp. 848-852.
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R. Omranipour. L. Meyer, S. H. layaram E.A. Chemey Inclined plane wcking and erosion evaluation of filled and unfilled silicone rubbei IEEE CEIDP 2001, 14-17 Oct. 2M)I. pp. 632 - 635

[7] A. H.U-Hag, S . Jayaram and E. A. Chemey. Physicochemical properties of silicone rubber nanc+composites for outdoar applications paper accepted and to be presented at CEIDP 2004. 181 ASTWD2303 Slandard Test Method for Liquid-Contaminan4 Inclined-Plane Tracking and Erosion of Insulating Materials. [9] A.H. El-Hag, S . Jayararn & E.A. Chemey Fundamental and Low Frequency Harmonic Components of Leakage Current as a Diagnostic Tool to Study Aging of RTV and HTV Silicone Rubber in Salt-Fog IEEE Transaction on Dielectrics and Electrical Insulation. Vol. IO, No. I . February 2W3, pp. 128136.

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