Solvent-Free and Recyclable Polyether/Polyphenol Supramolecular Adhesives with Robust, Water- and Low-Temperature-Resistant Properties

Adhesives are widely used in everyday life; however, traditional polymer adhesives pose unavoidable hazards to the environment and living organisms due to their extensive use of toxic organic solvents, heavy reliance on fossil resources as synthetic raw materials, and lack of recyclability. Furthermore, they are incapable of maintaining a stable adhesion performance in harsh conditions. In this work, we present a facile yet powerful noncovalent bonding strategy for successfully constructing poly(glycidol-co-1,2-butylene oxide)/tannic acid supramolecular adhesives (PG-co-PBO/TA SAs) through hydrogen-bonding interactions between hyperbranched PG-co-PBO and natural TA. The SAs demonstrate an adhesion strength of 2.15 MPa at ambient temperature and maintain an adhesion strength of 1.53 MPa even at −196 °C. Moreover, it can be easily recycled through thermal treatment and retains stable adhesion strength even after undergoing multiple recycling cycles. The investigation of the structure–property relationship of SAs and molecular dynamics simulations has clarified that short alkyl chains of PG-co-PBO effectively protect the hydrogen-bonding networks from damage by repelling water at the adhesive interface. Consequently, SAs even maintain robust and long-lasting adhesion strength in acidic, alkaline, and seawater solutions. Importantly, unlike conventional adhesives, SAs do not employ organic solvents throughout the synthesis, bonding, and recycling processes. By designing functionalized polymers and utilizing polyphenolic compounds, this work provides a green and feasible strategy for the development of next-generation powerful supramolecular adhesives.