Intrinsic Tuning of Poly(styrene-butadiene-styrene)-Based Self-Healing Dielectric Elastomer Actuators with Enhanced Electromechanical Properties

The electromechanical properties of a thermoplastic styrene-butadiene-styrene (SBS) dielectric elastomer was intrinsically tuned by chemical grafting with polar organic groups. Methyl thioglycolate (MG) reacted with the butadiene block via a one-step thiol-ene "click" reaction under UV at 25 degrees C. The MG grafting ratio reached 98.5 mol % (with respect to the butadiene alkenes present) within 20 min and increased the relative permittivity to 11.4 at 10(3) Hz, with a low tan delta. The actuation strain of the MG-grafted SBS dielectric elastomer actuator was 10 times larger than the SBS-based actuator, and the actuation force was 4 times greater than SBS. The MG-grafted SBS demonstrated an ability to achieve both mechanical and electrical self-healing. The electrical breakdown strength recovered to 15% of its original value, and the strength and elongation at break recovered by 25 and 21%, respectively, after 3 days. The self-healing behavior was explained by the introduction of olar MG groups that reduce viscous loss and strain relaxation. The weak CH/pi bonds through the partially charged (delta+) groups adjacent to the ester of MG and the delta- center of styrene enable polymer chains to reunite and recover properties. Intrinsic tuning can therefore enhance the electromechanical properties of dielectric elastomers and provides new actuator materials with self-healing mechanical and dielectric properties.