Enzymatic Crosslinking of Polyelectrolyte Complexes Produces Strong, Reconstitutable Biomedical Adhesives

Tissue adhesives that offer rapid wound sealing, reduce blood loss, enhance aesthetic outcomes, and lower biomedical issues can significantly augment the wound treatment regimen. Taking inspiration from proteinaceous adhesives secreted by marine organisms, herein we designed anionic and cationic polyamide polyelectrolytes (PEs) containing Horseradish Peroxidase (HRP)-responsive phenolic pendants. These PEs underwent facile polyelectrolyte complex (PEC) formation in aqueous medium. The PEC-rich phase was employed to formulate water-based biomedical adhesives that demonstrated robust adhesion to diverse surfaces - from biological tissues like bone to materials such as wood, glass, and metal. The PEC adhesive worked on both dry and wet substrates and its adhesive strength increased with environmental humidity. The strongest adhesion was found for wood with adhesive strength up to 10 MPa. The adhesive could be kept in a lyophilized powder form and reconstituted prior to use without significant impact on the adhesive performance. Furthermore, the PEC adhesive exhibited strong hemostatic and wound-healing capabilities in vivo in mice, significantly surpassing the commercial cyanoacrylate-based tissue adhesives in performance. These findings, coupled with the adhesive's biocompatibility and hemocompatibility, position these enzyme-cured PEC adhesives as promising contender in wound healing applications.