Tailoring Dielectric Properties using Designed Polymer-Grafted ZnO Nanoparticles in Silicone Rubber

Polymer grafts were used to tailor the interphases between ZnO nanoparticles (NPs) and silicone matrices. The final electrical properties of the nanocomposites were tuned by the grafted interphases, by controlling the inter-particle distance and the NP-morphology. The nanocomposites can be used in electrical applications where control of the resistivity is desired. Hansen's solubility parameters were used to select a semi-compatible polymer for grafting to obtain anisotropic NP morphologies in silicone, and the grafted NPs self-assembled into various morphologies inside the silicone matrices. The morphologies in the semi-compatible nanocomposites could be tuned by steering the graft length of poly(n-butyl methacrylate) via entropic matrix-graft wetting using surface-initiated atom-transfer radical polymerization. Image analysis models were developed to calculate the radius of primary NPs, the fraction of aggregates, the dispersion, and the face-to-face distance of NPs. The dielectric properties of the nanocomposites were related to the morphology and the face-to-face distance of the NPs. The dielectric losses, above 100 Hz, for nanocomposites with grafted NPs were approximately one decade lower than those of pristine NPs. The isotropic nanocomposites increased the resistivity up to 100 times compared to that of neat silicone rubber, due to the trapping of charge carriers by the interphase of dispersed NPs and nanoclusters. On the other hand, the resistivity of anisotropic nanocomposites decreased 10–100 times when the inter-particle distance in continuous agglomerates was close to the hopping distance of charge carriers. The electrical breakdown strength increased for compatible isotropic nanocomposites, and the temperature dependence of the resistivity and the activation energy were ∼50% lower in the nanocomposites with grafted NPs. These flexible dielectric nanocomposites are promising candidates for low-loss high-voltage transmission cable accessories, mobile electronic devices, wearables and sensors.

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