The development of environmentally friendly, green, and nontoxic adhesives with excellent dry and wet adhesion properties is of great attraction. In nature, barnacles and mussels exhibit strong adhesion by secreting a hydroxyl-rich dopa. Inspired by their adhesion mechanism, a simple biobased MAG-PETMP (MP) adhesive was prepared from magnolol (MAG) and pentaerythritol tetra (3-mercaptopropionate) (PETMP) by a thiol–ene click chemistry reaction. MP as an adhesive exhibits high bond strength with other substrates due to hydrogen bonds formed by the abundant hydroxyl groups at the interface and shows an inherent thermosetting network structure. Since MP has a thermosetting network, it exhibits excellent thermal stability, solvent resistance, and high mechanical strength, which make the adhesive stable in a humid environment. The cross-linking degree of MP can be easily controlled by adjusting the molar ratio of MAG and PETMP. Among the synthesized samples, the elongation at break of the MP 1 formulation is 174.27%, which makes it promising for use as a flexible adhesive. Moreover, the inherent antibacterial properties of MAG enable MP to exhibit antimicrobial properties and antibacterial adhesion to some extent. This work provides a simple biomimetic strategy that could enable the application of MAG for adhesives.
Abstract Hyaluronic acid hydrogels are promising materials for diverse applications, yet their potential is hampered by limitations such as low self‐healing efficiency and insufficient mechanical strength. Inspired by the heterogeneous structures of spider silk, we introduce a novel dual dynamically crosslinked network hydrogel. This hydrogel comprises an acylhydrazone‐crosslinked network, utilizing aldehyde hyaluronic acid (AHA) and 3,3′‐dithiobis (propionohydrazide) (DTP) as a first network, and a secondary network formed by hydrogen bonds‐crosslinked network between tannic acid (TA) and silk fibroin (SF) with β‐sheet formation. The hydrogel exhibits exceptional self‐healing ability due to the dynamic and reversible nature of Schiff base bonds, disulfide bonds, and hydrogen bonds, achieving complete healing within 5 minutes. Additionally, the spider silk‐inspired heterogeneous structures enhance mechanical properties. Furthermore, the incorporation of TA provides enhances adhesion, as well as remarkable antibacterial and antioxidant properties. This innovative hyaluronic acid‐based hydrogel, inspired by spider silk, offers a promising avenue to fortify both the mechanical strength and self‐healing capabilities of hydrogels, thus expanding opportunities for applications in tissue engineering and biomedicine.
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