Electroactive Artificial Muscles Based on Functionally Antagonistic Core–Shell Polymer Electrolyte Derived from PS‐b‐PSS Block Copolymer

Electroactive ionic soft actuators, a type of artificial muscles containing a polymer electrolyte membrane sandwiched between two electrodes, have been intensively investigated owing to their potential applications to bioinspired soft robotics, wearable electronics, and active biomedical devices. However, the design and synthesis of an efficient polymer electrolyte suitable for ion migration have been major challenges in developing high‐performance ionic soft actuators. Herein, a highly bendable ionic soft actuator based on an unprecedented block copolymer is reported, i.e., polystyrene‐b‐poly(1‐ethyl‐3‐methylimidazolium‐4‐styrenesulfonate) (PS‐b‐PSS‐EMIm), with a functionally antagonistic core–shell architecture that is specifically designed as an ionic exchangeable polymer electrolyte. The corresponding actuator shows exceptionally good actuation performance, with a high displacement of 8.22 mm at an ultralow voltage of 0.5 V, a fast rise time of 5 s, and excellent durability over 14 000 cycles. It is envisaged that the development of this high‐performance ionic soft actuator could contribute to the progress toward the realization of the aforementioned applications. Furthermore, the procedure described herein can also be applied for developing novel polymer electrolytes related to solid‐state lithium batteries and fuel cells. An unprecedented block copolymer, polystyrene‐b‐poly(1‐ethyl‐3‐methylimidazolium‐4‐styrenesulfonate), is designed and synthesized for electroactive ionic soft actuators. The membrane contains polystyrene spheres that provide mechanical stability and distribute in poly(1‐ethyl‐3‐methylimidazolium‐4‐styrenesulfonate) matrix forming a continuous ionic conducting phase. The corresponding actuator exhibits exceptionally good performance (rise time: 5 s, displacement: 8.2 mm at 0.5 V and 0.1 Hz, and durability: 14 000 cycles).