Intrinsic Elastomer with Remarkable Dielectric Constant via Elastification of Relaxor Ferroelectric Polymer

Abstract High‐dielectric‐constant elastomers always play a critical role in the development of wearable electronics for actuation, energy storage, and sensing; therefore, there is an urgent need for effective strategies to enhance dielectric constants. The present methods mainly involve adding inorganic or conductive fillers to the polymer elastomers, however, the addition of fillers causes a series of problems, such as large dielectric loss, increased modulus, and deteriorating interface conditions. Here, the elastification of relaxor ferroelectric polymers is investigated through slight cross‐linking, aiming to obtain intrinsic elastomers with high‐dielectric constants. By cross‐linking of the relaxor ferroelectric polymer poly(vinylidene fluoride‐ter‐trifluoroethylene‐ter‐chlorofluoroethylene) with a long soft chain cross‐linker, a relaxor ferroelectric elastomer with an enhanced dielectric constant is obtained, twice that of the pristine relaxor ferroelectric polymer and surpassing all reported intrinsic elastomers. This elastomer maintains its high‐dielectric constant over a wide temperature range and exhibits robust mechanical fatigue resistance, chemical stability, and thermal stability. Moreover, the ferroelectricity of the elastomer remains stable under strains up to 80%. This study offers a simple and effective way to enhance the dielectric constant of intrinsic elastomers, thus facilitating advancements in soft robots, biosensors, and wearable electronics.