Semipermeable Membrane‐Mediated Hydrogen Bonding Interface for Fabricating High‐Performance Pure PEDOT:PSS Hydrogels

Abstract Conductive poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) hydrogels are potential bioelectronic interface materials because of their favorable mechanical properties and tunable electrochemical performances. Owing to intrinsic core‐shell colloidal microstructure composed of insulative phase and conductive phase, inducing phase separation via diverse methods are proposed to improve their performances. However, fabrication of high‐performance pure PEDOT:PSS hydrogels via a simple, mild strategy remains challenges. Here, we report a straightforward strategy to yield high‐performance pure PEDOT:PSS hydrogels via the formation of semipermeable membrane‐mediated hydrogen bonding interface. In this method, ethanol‐attracted PSS is free to accumulate at the man‐made interface provided by the semipermeable membrane, to realize controllable hierarchical PEDOT and PSS two‐phase distribution. The separated PEDOT aggregates via π–π conjugation, followed by the removal of rearranged insulative PSS phase easily, to form PEDOT:PSS hydrogels with satisfactory mechanical and electrochemical performances. This work presents a universal, effective, and controlled strategy to design conductive hydrogels for bioelectronic applications.