Matching combination of amorphous ionic hydrogel with elastic fabric enables integrated properties for wearable sensing

The combination of hydrogels and fabrics opens up significant opportunities for flexible materials, particularly in biomedicine and wearable technology. However, the weak interface caused by insufficient interactions between the different phases and the substantial modulus mismatch limit their broader application. In this research, flexible and amorphous polyvinyl alcohol (PVA) hydrogels were integrated with polar and elastic fabrics to create multifunctional composites via in-situ freeze-thawing technology. First, by incorporating antifreeze inorganic salts into the precursor solution, we effectively suppressed ice crystal growth during the cooling process, promoting a uniform and loosely aligned PVA chain structure. This led to the formation of an amorphous crosslinked network while simultaneously releasing free hydroxyl groups. These hydroxyl groups facilitate the formation of robust interfaces within the composite. In addition, an elastic fabric composed of a polyester-polyurethane fiber blend was selected. The polyester fibers, rich in carbonyl groups along their polymer chains, form strong hydrogen bonds with the free hydroxyl groups from the PVA hydrogel, creating a highly resilient interface. The polyurethane fibers contribute to a lower Young's modulus, as well as excellent elasticity and ductility, reducing the fabric's inherent stiffness and mitigating fiber pull-out failure. Further, the incorporation of CaCl₂ not only created an environment rich in free ions, but also provided the amorphous structure with increasing spacing between adjacent polymer chains, facilitating the transportation of ions. Therefore, the composite exhibits adept sensing capabilities for intricate human body movements, fostering auspicious prospects in smart sensor applications.