Bioinspired Conductivity-Enhanced, Self-Healing, and Renewable Silk Fibroin Hydrogel for Wearable Sensors with High Sensitivity

The development of silk fibroin-based hydrogels with excellent biocompatibility, aqueous processability, and facile controllability in structure is indeed an exciting advancement for biological research and strain sensor applications. However, silk fibroin-based hydrogel strain sensors that combine high conductivity, high stretchability, reusability, and high selectivity are still desired. Herein, we report a simple method for preparing double-network hydrogels including silk fibroin and poly(acrylic acid) sodium-polyacrylate (PAA-PAAS) networks. The conformation and aggregate of silk fibroin could be facilely tuned by both ions and pH resulting from the PAA-PAAS network. The optimized hydrogel exhibits intriguing properties, such as high conductivity (3.67 S/m) and transparency, high stretchability (1186%) with a tensile strength of 110 kPa, good adhesion properties, reversible compression, self-healing, and high sensitivity (GF = 10.71). This hydrogel strain sensor can detect large-scale and small human movements in real time, such as limb movements, heartbeats, and pulse. Additionally, its ability to adsorb water and recover effectiveness after losing water from air with 90% humidity along with the capability for low-temperature motion detection facilitated by ethylene glycol further enhance its practical utility. This work offers a novel and simple approach to design flexible bionic strain sensors.