Nacre-Mimetic Structure Multifunctional Ion-Conductive Hydrogel Strain Sensors with Ultrastretchability, High Sensitivity, and Excellent Adhesive Properties

Recently, conductive hydrogels have emerged as promising materials for smart, wearable devices. However, limited mechanical properties and low sensitivity greatly restrict their lifespan. Based on the design of biomimetic-layered structure, the conductive hydrogels with nacre-mimetic structure were prepared by using layered acrylic bentonite (AABT) and phytic acid (PA) as multifunctional "brick" and "mortar" units. Among them, the unique rigid cyclic multihydroxyl structure of the "organic mortar" PA preserves both ultrastretchability (4050.02%) and high stress (563.20 kPa) of the hydrogel, which far exceeds most of the reported articles. Because of the synergistic effect of AABT and PA, the hydrogel exhibits an excellent adhesive strength (87.74 kPa). The role of AABT in the adhesive properties of hydrogels is proposed for the first time, and a general strategy for improving the adhesive properties of hydrogels by using AABT is demonstrated. Furthermore, AABT provides ion channels and PA ionizes abundant H⁺, conferring a high gauge factor (GF = 14.95) and excellent antimicrobial properties to the hydrogel. Also, inspired by fruit batteries, simple self-powered flexible sensors were developed. Consequently, this study provides knowledge for functional bentonite filler modified hydrogel, and the prepared multifunctional ionic conductive hydrogel shows great application potential in the field of intelligent wearable devices.