Molecular composites with enhanced energy density for electroactive polymers

Abstract

Actuators based on soft dielectric elastomers deform due to electric field induced Maxwell's stress, interacting with the mechanical properties of the material. The relatively high operating voltages of such actuators can be reduced by increasing the permittivity of the active material, while maintaining the mechanical properties and high electrical breakdown strength. Approaches relying on the use of highly polarizable molecules or conjugated polymers have so far provided the best results, however it has been difficult to maintain high breakdown strengths. In this work, a new approach for increasing the electrostatic energy density of a soft polymer based on molecular composites is presented, relying on chemically grafting soft gel-state π-conjugated conducting macromolecules (polyaniline (PANI)) to a flexible elastomer backbone SEBS-g-MA (poly-styrene-co-ethylene-co-butylene-co-styrene-g-maleic anhydride). The approach was found to result in composites of increased permittivity (470% over the elastomer matrix) with hardly any reduction in breakdown strength (from 140 to 120 V μm−1), resulting in a large increase in stored electrostatic energy. This led to an improvement in the measured electromechanical response as well as in the maximum actuation strain. A transition was observed when amounts of PANI exceeded 2 vol%, which was ascribed to the exhaustion of the MA-functionality of the SEBS-g-MA. The transition led to drastic increases in permittivity and conductivity, and a sharp drop in electrical breakdown strength. Although the transition caused further improvement of the electromechanical response, the reduction in electrical breakdown strength caused a limitation of the maximum achievable actuation strain.