Underwater Adhesives from Redox‐Responsive Polyplexes of Thiolated Polyamide Polyelectrolytes

We report the fabrication of optically clear underwater adhesives using polyplexes of oppositely charged partially‐thiolated polyamide polyelectrolytes (TPEs). The thiol content of the constituent PEs was varied to assess its influence on the adhesive properties of the resulting glues. These catechol‐free, redox‐responsive TPE‐adhesives were formulated in aquo and exhibited high optical transparency and strong adhesion even on submerged or moist surfaces of diverse polar substrates such as glass, aluminium, wood, and bone pieces. The adhesives could be cured under water through oxidative disulphide crosslinking of the constituent TPEs. The polyamide backbone provided multi‐site H‐bonding interactions with the substrates while the disulphide crosslinking provided the cohesive strength to the glue. Strong adhesion of mammalian bones (load bearing capacity upto 7 kg/cm2) was achieved using the adhesive containing 30 mol % thiol residues. Higher pH and use of oxidants such as povidone‐iodine solution enhanced the curing rate of the adhesives, and so did the use of Tris buffer instead of Phosphate buffer. The porous architecture of the adhesive and its progressive degradation in aqueous medium over the course of three weeks bode well for diverse biomedical applications where temporary adhesion of tissues is required. Redox‐responsive underwater adhesives exhibiting high optical transparency, biodegradability and strong adhesion of biological substrates were prepared from polyplexes of oppositely charged partially‐thiolated polyamide polyelectrolytes (TPEs).