Interfacial Hydrogen Bond-Reinforced Adhesion and Cohesion Enabling an Ultrastretchable and Wet Adhesive Hydrogel Strain Sensor

Historically, research on silicotungstic-acid–based hydrogels has primarily focused on their adhesive properties, often at the expense of mechanical strength (cohesion). In this study, we present a novel approach to fabricate a polysaccharide hydrogel that harmoniously balances both adhesion and cohesion via interfacial hydrogen bonds. This hydrogel, composed of carboxymethyl cellulose (CMC), polyacrylamide (PAM), silicotungstic acid (SiW), and lithium chloride (LiCl), showcases a unique combination of properties: strain-responsive ionic conductivity, superior transparency, remarkable stretchability, and robust adhesion. Contrary to conventional PAM hydrogels, our PAM-SiW networked hydrogel addresses the common challenge of achieving good adhesion without compromising on cohesion. Specifically, our hydrogel demonstrates a maximum toughness of 20.3 MJ/m 3 and a strain of 4079%, an accomplishment rarely observed in other adhesive hydrogel. Furthermore, the hydrogel’s adhesion is both reversible and versatile, adhering effectively to a variety of wet and dry substrates. This makes it a promising candidate for advanced healthcare applications, particularly as a mechanically reinforced underwater adhesive with unparalleled stability. We also provide insights into the role of LiCl in the hydrogel matrix, emphasizing its influence on electrostatic interactions without affecting the hydrogen bonds. This study serves as a testament to the potential of harmonizing adhesive and cohesive properties in hydrogels, paving the way for future innovations in the field.