Muscle-Mimetic Highly Tough, Conductive, and Stretchable Poly(ionic liquid) Liquid Crystalline Ionogels with Ultrafast Self-Healing, Super Adhesive, and Remarkable Shape Memory Properties.

Here, we report a simple method for preparing muscle-mimetic highly tough, conductive, and stretchable liquid crystalline ionogels which contains only one poly(ionic liquid) (PIL) in an ionic liquid via in situ free radical photohomopolymerization by using nitrogen gas instead of air atmosphere. Due to eliminating the inhibition caused by dissolved oxygen, the polymerization under nitrogen gas has much higher molecular weight, lower critical sol-gel concentration, and stronger mechanical properties. More importantly, benefiting from the unique loofah-like microstructures along with the strong internal ionic interactions, entanglements of long PIL chains and liquid crystalline domains, the ionogels show special optical anisotropic, superstretchability (>8000%), high fracture strength (up to 16.52 MPa), high toughness (up to 39.22 MJ/m 3 ), and have ultrafast self-healing, ultrastrong adhesive, and excellent shape memory properties. Due to its excellent stretchability and good conductive-strain responsiveness, the as-prepared ionogel can be easily applied for high-performance flexible and wearable sensors for motion detecting. Therefore, this paper provides an effective route and developed method to generate highly stretchable conductive liquid crystalline ionogels/elastomers that can be used in widespread flexible and wearable electronics.