Polyaniline-Decorated Supramolecular Hydrogel with Tough, Fatigue-Resistant, and Self-Healable Performances for All-In-One Flexible Supercapacitors

It is a challenge to realize high strength, toughness, and energy storage, as well as excellent capacitive self-recovery, fatigue-resistant, and self-healing performances simultaneously in a single all-in-one supercapacitor aiming for wearable electronics. Herein, based on the self-crosslinking and molecular template, a supramolecular poly(vinyl alcohol)/poly (N-hydroxyethyl acrylamide) (PVA/PHEA) hydrogel electrolyte (HGE) decorated by polyaniline (PANI) was prepared by in situ rapid polymerization of high-concentration aniline on the PVA/PHEA gel containing H₂SO₄. The multiple hydrogen bonds, rapid polymerization, and decoration endowed PANI-decorated PVA/PHEA HGE-based all-in-one flexible supercapacitor with the integrated high performances, which include high specific capacitance, good cycling stability, high strength, excellent toughness, rapid self-recovery, excellent fatigue-resistant, and self-healing capabilities, as well as high capacitance retention during or after the large deformations or after the self-healing. Thus, the current work presents a novel and promising strategy to design the integrated high-performance supercapacitors aiming for wearable electronics.