Conductive and Tough Hydrogels Based on Biopolymer Molecular Templates for Controlling in Situ Formation of Polypyrrole Nanorods

Conductive hydrogels (CHs) have gained significant attention for their wide applications in biomedical engineering owing to their structural similarity to soft tissues. However, designing CHs that combine biocompatibility with good mechanical and electrical properties is still challenging. Herein, we report a new strategy for the fabrication of tough CHs with excellent conductivity, superior mechanical properties, and good biocompatibility by using chitosan framework as molecular templates for controlling conducting polypyrrole (PPy) nanorods in situ formation inside the hydrogel networks. First, polyacrylamide/chitosan (CS) interpenetrating polymer network hydrogel was synthesized by UV photopolymerization; second, hydrophobic and conductive pyrrole monomers were absorbed and fixed on CS molecular templates and then polymerized with FeCl₃ in situ inner hydrophilic hydrogel network. This strategy ensured that the hydrophobic PPy nanorods were uniformly distributed and integrated with the hydrophilic polymer phase to form highly interconnected conductive path in the hydrogel, endowing the hydrogel with high conductivity (0.3 S/m). The CHs exhibited remarkable mechanical properties after the chelation of CS by Fe³⁺ and the formation of composites with the PPy nanorods (fracture energy 12 000 J m^-2 and compression modulus 136.3 MPa). The use of a biopolymer molecular template to induce the formation of PPy nanostructures is an efficient strategy to achieve conductive multifunctional hydrogels.