Liquid Crystal Electrolyte with Lamellar Ionic Channels for All‐In‐One Gel Flexible Supercapacitor

Abstract Liquid crystalline hydrogels with nanoscale order are an attractive soft material to transport ions or electrons with high efficiency. By employing noncovalent interactions between amphiphiles and solvents, defined anisotropic ordered structures can assemble that serve as interior transmissible channels. Herein, the phase behaviors of a polymerizable amphiphile of 1‐vinyl‐3‐alkylimidazolium bromide (VC n IMBr, n = 12, 14, 16) are investigated at different concentrations in a deep eutectic solvent. The aggregation such as micelle, hexagonal, and lamellar liquid crystal phase is created. Through in‐phase polymerization, the lamellar structures within an an isotropic liquid crystal can be well solidified to obtain a conductive gel electrolyte. A sandwich‐structured all‐in‐one gel flexible supercapacitor is then built with this specific gel electrolyte. With greatly increased adhesion and minimized interfacial resistance between electrode and electrolyte, the approach will be able to create energy‐storage devices with anisotropic ionic and electronic charge transportations envisioned for various electrochemical applications.