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

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.