Robust Supramolecular Adhesives Based on Natural Small Molecules Through Hydrogen Bonding

The environmental persistence and widespread application of conventional polymer adhesives raise critical concerns regarding network design complexity and long-term residue accumulation. Herein, we present a water-soluble supramolecular adhesive synthesized from natural small molecules. Unlike traditional polymer networks relying on weak intermolecular forces, this system establishes a robust ordered architecture through dynamic disulfide bond ring-opening polymerization and carboxylate ion electrostatic interactions. Water-soluble hexamethylenetetramine (HMTA) strategically increases hydrogen-bonding site density while stabilizing the network topology, efficiently reducing chain entanglement. These synergistic effects endow the material with strong adhesion capability even at minimal usage (∼0.4 mg/cm²), achieving a maximum adhesion strength capable of supporting up to 10⁷ times its weight while maintaining considerable resistance to various environmental factors, including thermal extremes (-80°C to 120°C) and exposure to organic solvents. This supramolecular design paradigm offers an eco-friendly alternative to conventional polymeric adhesives.