Boosting the Actuation Performance of a Dynamic Supramolecular Polyurethane–Urea Elastomer via Kinetic Control

The ongoing soft actuation has accentuated the demand for dielectric elastomers (DEs) capable of large deformation to replace the traditional rigid mechanical apparatus. However, the low actuation strain of DEs considerably limits their practical applications. This work developed high-performance polyurethane–urea (PUU) elastomers featuring large actuation strains utilizing an approach of kinetic control over the microphase separation structure during the fabrication process. Additionally, disulfide (DS) bonds were incorporated as dynamic chemical linkages to effectively heal the mechanical damage in the resulting elastomer (PUUDS). Alteration in processing conditions creates notable differences in the rate of phase separation among the multiphase materials. A faster phase separation rate is associated with a reduced degree of microphase separation, increased spacing within hard domains, a higher proportion of disordered hydrogen bonds, and hydrogen bonding index. These changes synergistically improved the electromechanical properties of the PUUDS elastomers, thereby enhancing their actuation performance. The sample processed under the fastest phase separation condition showed the lowest Young’s modulus and a pronounced dielectric response at low frequencies. The electrostriction effect accounts for 89% of the total electromechanical coupling, achieving a significant reduction in the driving voltage during actuation. The maximum actuation strain recorded was 21.6% at an electric field of 45 MV/m. Benefiting from the fully reversible dynamic network, the damaged PUUDS elastomer can be healed and restored to its original elongation at break after 3 h at room temperature. Practical application was demonstrated through the development of a miniature butterfly model constructed from a single-layer PUUDS elastomer, showcasing potential applications in soft robotics. These findings highlight the critical role of kinetic control in optimizing the performance of advanced DEs.