Self-healable, high-permittivity elastomers for dielectric elastomer actuators

Abstract

Polar group-modified polysiloxanes obtained by anionic ring-opening polymerization possess high dielectric permittivity and are of great interest for application in dielectric elastomer actuators (DEAs). A self-healing elastomer can be obtained by in situ polymerization and cross-linking using a cyclic siloxane monomer with polar side groups and a cross-linker consisting of multiple connected siloxane rings. In previous works, a non-polar cross-linker has been used, which requires the addition of a solvent for compatibilization with the polar monomer. In polymerization reactions of siloxanes, the addition of solvent leads to a more pronounced formation of cyclic by-products. These cycles impair the mechanical properties of the elastomer and cannot be removed after the reaction, as the material is already cross-linked. Therefore, in this work, we use a polar cross-linker that can be mixed with the polar monomer without adding solvent. Nitrile groups have been studied extensively for increasing the permittivity of the polysiloxane backbone. For a functionalization of 100%, a dielectric permittivity of ~18 was reached. In most cases, the nitrile group was attached to the siloxane backbone in the form of cyanopropyl groups. Still, the influence of the alkyl spacer on the material's dielectric and mechanical properties has not been studied. In this work, we synthesize cyanoalkyl-functional cyclic siloxanes with different lengths of the alkyl spacer and polymerize them solvent-free to high-permittivity polysiloxanes.