A Mesostructure Multivariant‐Assembly Reinforced Ultratough Biomimicking Superglue

Abstract

The imitation of mussels and oysters to create high‐performance adhesives is a cutting‐edge field. The introduction of inorganic fillers is shown to significantly alter the adhesive's properties, yet the potential of mesoporous materials as fillers in adhesives is overlooked. In this study, the first report on the utilization of mesoporous materials in a biomimetic adhesive system is presented. Incorporating mesoporous silica nanoparticles (MSN) profoundly enhances the adhesion of pyrogallol (PG)–polyethylene imine (PEI) adhesive. As the MSN concentration increases, the adhesion strength to glass substrates undergoes an impressive fivefold improvement, reaching an outstanding 2.5 mPa. The adhesive forms an exceptionally strong bond, to the extent that the glass substrate fractures before joint failure. The comprehensive tests involving various polyphenols, polymers, and fillers reveal an intriguing phenomenon—the molecular structure of polyphenols significantly influences adhesive strength. Steric hindrance emerges as a crucial factor, regulating the balance between π‐cation and charge interactions, which significantly impacts the multicomponent assembly of polyphenol‐PEI‐MSN and, consequently, adhesive strength. This groundbreaking research opens new avenues for the development of novel biomimetic materials.