Binary Co-Gelator Strategy: Toward Highly Deformable Ionic Conductors for Wearable Ionoskins

Stretchable ionic conductors have been actively developed due to the increasing demand for wearable electrochemical platforms. Herein, we propose a convenient and effective strategy for tailoring the mechanical deformability of ionic conductors. The mixing of poly(methyl methacrylate) (PMMA, polymer gelator) and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BMI][TFSI], ionic liquid) produces mechanically stiff ionic conductors. To reduce the chain entanglement of polymer gelators and induce effective dissipation of applied stresses, flexible poly(butyl acrylate) (PBA) with a low glass-transition temperature is additionally doped into the ionic conductor. An extremely stretchable (∼1500%) homogeneous ternary ionic conductor is obtained without a notable change in electrochemical characteristics, unless the content of PBA exceeds the macrophase separation limit of 3 wt %. In addition, the mechanical elasticity (1.8 × 10⁵Pa) and durability (e.g., recovery ratio of ∼86.3% after 1000 stretching/releasing cycles) of the conductor further support its suitability as a strain sensory platform. In contrast to conventional ionoskins that have to fit the area of target body parts, even a small piece of the ternary ionic conductor successfully monitors human motion over large areas by taking advantage of its superior deformability.