A Mesostructure Multivariant-Assembly Reinforced Ultratough Biomimicking Superglue.

The imitation of mussels and oysters to create high-performance adhesives has been a cutting-edge field. The introduction of inorganic fillers has been shown to significantly alter the adhesive's properties. However, the potential of mesoporous materials as fillers in adhesives has been overlooked, and there is a lack of research on the synergistic interactions between inorganic particles and organic polymers. In this study, we present the first report on the utilization of mesoporous materials in a biomimetic adhesive system. 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 five-fold improvement, reaching an outstanding 2.5 mPa. At higher MSN concentrations, the adhesive forms an exceptionally strong bond, to the extent that the glass substrate fractures before joint failure. Our 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 multi-component assembly of polyphenol-PEI-MSN and, consequently, adhesive strength. Furthermore, we assess the stability of this biomimetic adhesive under challenging conditions, including freezing, sunlight exposure, and water immersion, confirming its practical application potential. This groundbreaking research not only advances our understanding of interactions between organic and inorganic components in composite materials but also opens new avenues for the development of novel biomimetic materials. This article is protected by copyright. All rights reserved.