Photocured Liquid-Crystalline Polymer Electrolytes with 3D Ion Transport Pathways for Electromechanical Actuators

Self-assembly of ionic molecules into hierarchical ordered structures is a promising route to new types of solid electrolytes with enhanced ion transport. Herein, we report a liquid-crystalline polymer electrolyte membrane that contains three-dimensionally (3D) interconnected ionic pathways. To build this membrane, we used wedge-shaped amphiphilic molecules that have two ionic heads and a lipophilic tail. These molecules were combined with a low content of ionic liquid (5.6 wt %) to form a hexagonal columnar phase, where the self-assembled lipophilic cylinders were surrounded by the ionic shell. Photopolymerization of this phase produced flexible nanostructured films with 3D ionic pathways, which can serve as an electrolyte layer in soft robotic actuators. Ionic transport in the 3D pathways leads to shape memory capability as well as durable bending actuation with a voltage-controllable blocking force. Furthermore, we find a significant enhancement of actuation for the nanostructured electrolyte compared with the corresponding amorphous electrolyte.