Bioinspired Mechanically Robust Organic–Inorganic Hybridized Bio‐Adhesives With up to 50% Inorganic Components by Bi‐Continuous Phase Engineering

Conventional methods for making organic-inorganic hybrid materials tend to hinder the capability to reinforce or toughen the materials owing to the limited incorporation of inorganic fillers, which serve only as filler components in the structure. This project aims to tackle these challenges using an innovative bio-inspired method based on the repair of a tooth's natural mineralization-bridging mechanism. The method involves using inorganic oligomers as cross-linkers by means of hydroxyapatite cross-linking to construct a continuous inorganic network and its subsequent seamless integration with an organic network from plant proteins. The result is a novel bi-continuous organic-inorganic hybrid structure created through this process. The approach taken here is novel in that for

the first time, it is possible to achieve a significant increase in the inorganic phase content of the bio-adhesive, at 50%, compared to the 0.2%–3.0% values typically observed in conventional hybrid methods. The bio-adhesive has exceptional mechanical properties, with a significant improvement in the strength increasing 6-fold and toughness increasing 121-fold over the traditional hybrid adhesives with the same inorganic content. Additionally, the bi-continuous hybrid adhesive based on plant protein is low cost and has lower carbon emissions, which is a promising alternative to conventional resins such as urea-formaldehyde. This line of research offers a good perspective to design composites that are high performing, low cost and eco-friendly.

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