Molecular Rationale for the Design of Instantaneous, Strain-Tolerant Polymeric Adhesive in a Stretchable Underwater Human–Machine Interface

Strain-tolerant reversible adhesion under harsh mechanical deformation is important for realizing long-lasting polymeric adhesives. Despite recent advances, cohesive failure within adhesives remains a critical problem that must be solved to achieve adhesion that is robust against humidity, heat, and mechanical stress. Here, we report a molecular rationale for designing an instantaneous polymeric adhesive with high strain tolerance (termed as iPASTE) even in a stretchable human–machine interface. The iPASTE consists of two biocompatible and eco-friendly polymers, linearly oligomerized green tea extracts, and poly­(ethylene glycol) for densely assembled networks via dynamic and reversible hydrogen bonds. Other than the typical approach containing nanoclay or branched adhesive precursors, the linear configuration and conformation of such polymer chains within iPASTE lead to strong and moisture-resistant cohesion/adhesion. Based on the strain-tolerant adhesion of iPASTE, it was demonstrated that a subaqueous interactive human–machine interface integrated with a robot arm and a gold nanomembrane strain-sensitive electronic skin can precisely capture a slithery artificial fish by using finger gesture recognition.