Design of Self-Healing and Electrically Conductive Silk Fibroin-Based Hydrogels

Self-healing and electrically conductive silk fibroin (SF)-based hydrogels were developed based on the dynamic assembly/disassembly nature of supramolecular complexes and the conductive nature of polypyrrole (PPy). The self-healing properties of the hydrogels were achieved through host–guest interactions between β-cyclodextrin and amino acid side chains (tyrosine, tryptophan, phenylalanine, and histidine) on SF. PPy deposition was achieved via in situ polymerization of pyrrole using ammonium persulfate as an oxidant and laccase as a catalyst. The PPy-coated hydrogels behaved as an elastomer and displayed excellent electrical properties, with adjustable electrical conductivities ranging from 0.8 ± 0.2 to (1.0 ± 0.3) × 10–3 S·cm–1. Furthermore, possibility of potential utilization of the hydrogels in electrochemistry applications as flexible yet self-healable electrode materials was explored. This study not only shows great potential in expanding the role of silk-based devices for various applications but also provides a useful approach for designing multifunctional self-healing protein-based hydrogels.