Highly Stretchable Conjugated Polymer/Elastomer Blend Films with Sandwich Structure

The physical blending of high‐mobility conjugated polymers with ductile elastomers provides a simple way to realize high‐performance stretchable films. However, how to control the morphology of the conjugated polymer and elastomer blend film and its response to mechanical fracture processes during stretching are not well understood. Herein, a sandwich structure is constructed in the blend film based on a conjugated polymer poly[(5‐fluoro‐2,1,3‐benzothiadiazole‐4,7‐diyl)(4,4‐dihexadecyl‐4H‐cyclopenta[2,1‐b:3,4‐b″]dithiophene‐2,6‐diyl)(6‐fluoro‐2,1,3‐benzothiadiazole‐4,7‐diyl)(4,4‐dihexadecyl‐4H‐cyclopenta[2,1‐b:3,4‐b″]dithiophene‐2,6‐diyl)] (PCDTFBT) and an elastomer polystyrene‐block‐poly(ethylene‐ran‐butylene)‐block‐polystyrene (SEBS). The sandwich structure is composed of a PCDTFBT:SEBS mixed layer laminated with a PCDTFBT‐rich layer at both the top and bottom surfaces. During stretching, the external strain energy can be effectively dissipated by the deformation of the crystalline PCDTFBT domains and amorphous SEBS phases and the recrystallization of the PCDTFBT chains. This endows the blend film with excellent ductility, with a large crack onset strain exceeding 1100%, and minimized the electrical degradation of the blend film at a large strain. This study indicates that the electrical and mechanical performance of conjugated polymer/elastomer blend films can be improved by manipulating their microstructure. A sandwich structure with the mixed poly[(5‐fluoro‐2,1,3‐benzothiadiazole‐4,7‐diyl)(4,4‐dihexadecyl‐4H‐cyclopenta[2,1‐b:3,4‐b″]dithiophene‐2,6‐diyl)(6‐fluoro‐2,1,3‐benzothiadiazole‐4,7‐diyl)(4,4‐dihexadecyl‐4H‐cyclopenta[2,1‐b:3,4‐b″]dithiophene‐2,6‐diyl)] (PCDTFBT):polystyrene‐block‐poly(ethylene‐ran‐butylene)‐block‐polystyrene (SEBS) mixed layer laminated with PCDTFBT‐rich layers at top and bottom surfaces can effectively dissipate the external stress by the deformation of crystalline PCDTFBT domains and amorphous SEBS phases and the recrystallization of PCDTFBT chains, endowing the blend film with a large crack onset strain exceeding 1100%.