Promising Synthesis Route of Ultra‐Conductive Porous Polypyrrole via Template‐Free Polymerization

Abstract The electrical stability and biocompatibility of conducting polymer polypyrrole (PPy), combined with its low‐cost synthesis, position PPy as a promising material for flexible electronics and bioelectronics. Despite recent progress, scalable PPy synthesis remains challenging due to limitations in traditional chemical and electrochemical polymerization methods. Herein, we introduce a deep eutectic solvent (DES)‐mediated interface polymerization strategy that achieves template‐free PPy synthesis without requiring additional oxidants or specialized equipment. This facile approach yields high‐conductivity porous PPy with a record 98% conversion efficiency in less than 3 h at room temperature, surpassing the capabilities of conventional synthesis protocols. The resultant PPy exhibits a conductivity of 67 S/cm and a specific surface area comparable to PPy aerogels, enabling efficient ion/electron transport and outstanding specific capacitance for flexible supercapacitor applications. This environmentally friendly, operationally simple, and readily scalable method represents a significant advancement toward the commercialization of high‐performance PPy materials.