Self-Healing, Remoldable, and Conductive Starch-Based Dual Reversible Cross-Linking Hydrogels for Strain Sensors

Polysaccharide-based hydrogels have been utilized as flexible strain sensors because of their renewability, biocompatibility, and biodegradability. However, their widespread application is hindered by the complexity of their manufacturing processes and the inevitable degradation of their mechanical properties with repeated use. The introduction of reversible bond chemistry offers the potential to impart self-healing properties to hydrogels, extending their functional lifespan. In this study, we prepared a starch-based conductive hydrogel (starch/poly(vinyl alcohol) (PVA)/cellulose nanocrystals (CNCs)) via a straightforward method using borax as a cross-linking agent. The hydrogel demonstrated improved strength and self-healing property because of the addition of CNCs, which formed dual reversible cross-links with starch and PVA via hydrogen and borate ester bonds. Additionally, the sodium ions (Na⁺) and borate ions (B(OH)₄^–) within the network enhanced the electrical conductivity and strain sensitivity of the hydrogel. The resulting hydrogel demonstrated potential for application as a wearable sensor capable of monitoring a range of human movements, sensing handwriting, and enabling Morse code communication. Notably, the hydrogel could be easily remolded at room temperature after being sectioned, highlighting its practical applicability. This work expands the scope of the use of starch-based hydrogels in sustainable wearable sensor technologies.