Natural Phytic Acid-Assisted Polyaniline/Poly(vinyl alcohol) Hydrogel Showing Self-Reinforcing Features

Polyaniline (PANi) hydrogels that combine advantages of hydrogels and conductive PANi have recently emerged in areas of wearable devices and personal healthcare. Nevertheless, their mechanical performance often gradually degrades after being used for a period, caused by destruction of the inner structures when external forces are applied. Inspired by biological structures with persistent durability, we develop here a phytic acid-assisted PANi/poly(vinyl alcohol) (PVA) hydrogel that shows self-reinforcing features. As a natural product holding plenty of phosphate groups, phytic acid (PA) plays two crucial roles when preparing this hydrogel: (1) aniline is salinized by PA in aqueous solution to promote in situ polymerization, making the resulting PANi conductive; (2) PA/PANi particles form hydrogen bonds with PVA, acting as stress concentration points to induce structure orientation. The optimal PVA/PA/PANi hydrogel displays dark green color with a uniform distribution of PA/PANi particles. After experiencing repetitive 4 × 100 stretching at a strain of 10%, the hydrogel exhibits an enhanced fracture strength (20.35 MPa), Young’s modulus (22.66 MPa), and toughness (36.24 MJ·m–3) compared with the original hydrogel. This self-reinforcing feature is mainly attributed to the formation of anisotropic structures fixed by hydrogen bonds between PA/PANi particles and PVA chains upon repetitive external forces. Moreover, anisotropic structures can be disassembled by swelling the post-stretched hydrogel in water, and the swollen hydrogel shows similar self-reinforcing behaviors. The good mechanical durability and reusable characteristics make the PVA/PA/PANi hydrogel a reliable strain sensor. This work provides a structural growing-reviving approach for conductive hydrogels with persistent durability.