The Polymer Society of Korea

Abstract

Synthetic hydrogels typically face a trade-off where high water content acts as a plasticizer, significantly reducing mechanical stiffness. Inspired by the Extracellular Matrix (ECM)—which utilizes collagen networks to convert osmotic swelling into stiffness— we present a novel hydrogel architecture that achieves hydration-mediated reinforcement through in-situ structural reconfiguration. Our system strategically employs a poly(lipoic acid/lipoate) matrix crosslinked by PEGDA. Upon physiological hydration, the network undergoes controlled disulfide cleavage, triggering thermodynamically driven micro-phase separation. This process forms rigid hydrophobic clusters that constrain the swollen matrix, effectively transforming water from a plasticizer into a structural reinforcer. This breakthrough bridges the gap between high hydration and mechanical strength, offering a promising platform for iontronics and high-performance hydrovoltaic devices.