Polypyrrole-Doped Conductive Supramolecular Elastomer with Stretchability, Rapid Self-Healing, and Adhesive Property for Flexible Electronic Sensors

Although recent years have witnessed intense efforts and innovations in the design of flexible conductive materials for the development of next-generation electronic devices, it remains a great challenge to integrate multifunctionalities such as stretchability, self-healing, adhesiveness, and sensing capability into one conductive system for practical applications. In this work, for the first time, we have prepared a new electrically conductive elastomer composite that combines all these functionalities by triggering in situ polymerization of pyrrole in a supramolecular polymer matrix cross-linked by multiple hydrogen-bonding 2-ureido-4[1 H]-pyrimidinone (UPy) groups. The polypyrrole (PPy) particles were uniformly dispersed and imparted to the composite desirable conductive properties, while the reversible nature of the dynamic multiple hydrogen bonds in the polymer matrix allowed excellent stretchability, fast self-healing ability, and adhesiveness under ambient condition. The elastomer composite with the incorporation of 7.5 wt % PPy displayed a mechanical strength of 0.72 MPa with an elongation over 300%, where the rapid self-healing of the mechanical and electrical properties was achieved within 5 min. The elastic material also exhibited strong adhesiveness to a broad range of inorganic and organic substrates, and it was further fabricated as a strain sensor for the detection of both large and subtle human motions (i.e., finger bending, pulse beating). The novel PPy-doped conductive elastomer has demonstrated great potential as functional sensors for wearable electronics, which provides a facile and promising approach to the development of various flexible electronic materials with multifunctionalities by combining conductive components with supramolecular polymers.