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Biological adhesion occurs in various circumstances. Differences of sessile organisms in size, shape, physiology, lifecycle, living environment, and phylogenic relationship would have different design implications in their adhesives, and the structures and mechanisms have yet to be properly unraveled at the molecular level. This chapter focused on the structure and mechanism of underwater adhesion and adhesives of three representative aquatic organisms, barnacle, mussel and tube worm, and the conceptual gap between chemical synthetic adhesives and bio-molecular ones was discussed. Collectively, it was proposed that the combination of unraveling the natural system and the design of analogous protein/peptide-based materials may eventually fill the gap between bio-molecular materials and synthetic chemical polymers.

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