Self‐Healable and Stretchable Ionic‐Liquid‐Based Thermoelectric Composites with High Ionic Seebeck Coefficient

Abstract The advancement of wearable electronics, particularly self‐powered wearable electronic devices, necessitates the development of efficient energy conversion technologies with flexible mechanical properties. Recently, ionic thermoelectric (TE) materials have attracted great attention because of their enormous thermopower, which can operate capacitors or supercapacitors by harvesting low‐grade heat. This study presents self‐healable, stretchable, and flexible ionic TE composites comprising an ionic liquid (IL), 1‐ethyl‐3‐methylimidazolium trifluoromethanesulfonate (EMIM:OTf); a polymer matrix, poly(vinylidene fluoride‐ co ‐hexafluoropropylene) (PVDF‐HFP); and a fluoro‐surfactant (FS). The self‐healability of the IL‐based composites originates from dynamic ion–dipole interactions between the IL, the PVDF‐HFP, and the FS. The composites demonstrate excellent ionic TE properties with an ionic Seebeck coefficient ( S i ) of ≈38.3 mV K −1 and an ionic figure of merit of ZT i = 2.34 at 90% relative humidity, which are higher than the values reported for other IL‐based TE materials. The IL‐based ionic TE composites developed in this study can maintain excellent ionic TE properties under harsh conditions, including severe strain (75%) and multiple cutting–healing cycles.