Spider‐Silk‐Inspired Tough, Self‐Healing, and Melt‐Spinnable Ionogels

Abstract As stretchable conductive materials, ionogels have gained increasing attention. However, it still remains crucial to integrate multiple functions including mechanically robust, room temperature self‐healing capacity, facile processing, and recyclability into an ionogel‐based device with high potential for applications such as soft robots, electronic skins, and wearable electronics. Herein, inspired by the structure of spider silk, a multilevel hydrogen bonding strategy to effectively produce multi‐functional ionogels is proposed with a combination of the desirable properties. The ionogels are synthesized based on N ‐isopropylacrylamide (NIPAM), N, N ‐dimethylacrylamide (DMA), and ionic liquids (ILs) 1‐ethyl‐3‐methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMI][TFSI]). The synergistic hydrogen bonding interactions between PNIPAM chains, PDMA chains, and ILs endow the ionogels with improved mechanical strength along with fast self‐healing ability at ambient conditions. Furthermore, the synthesized ionogels show great capability for the continuous fabrication of the ionogel‐based fibers using the melt‐spinning process. The ionogel fibers exhibit spider‐silk‐like features with hysteresis behavior, indicating their excellent energy dissipation performance. Moreover, an interwoven network of ionogel fibers with strain and thermal sensing performance can accurately sense the location of objects. In addition, the ionogels show great recyclability and processability into different shapes using 3D printing. This work provides a new strategy to design superior ionogels for diverse applications.