Tuning the underwater adhesiveness of antibacterial polysaccharides complex coacervates

HYPOTHESIS: Adjusting the water content and mechanical properties of polyelectrolyte coacervates for optimal underwater adhesion requires simultaneous control of the macromolecular design and the type and concentration of the salt used. Using synthetic or bio-inspired polymers to make coacervates often involves complicated chemistries and large variations in salt concentration. The underwater adhesiveness of simple, bio-sourced coacervates can be tuned with relatively small variations in salt concentration. Bio-sourced polymers can also impart beneficial biological activities to the final material. EXPERIMENTS: We made complex coacervates from charged chitosan (CHI) and hyaluronic acid (HA) with NaCl as the salt. Their water content and viscoelastic properties were investigated to identify the formulation with optimal underwater adhesion in physiological conditions. The coacervates were also studied in antibacterial and cytotoxicity experiments. FINDINGS: As predicted by linear rheology, the CHI-HA coacervates at 0.1 and 0.2 M NaCl had the highest pull-off adhesion strengths of 44.4 and 40.3 kPa in their respective supernatants. In-situ physical hardening of the 0.2 M coacervate upon a salt switch in 0.1 M NaCl resulted in a pull-off adhesion strength of 62.9 kPa. This material maintained its adhesive properties in physiological conditions. Finally, the optimal adhesive was found to be non-cytotoxic and inherently antimicrobial through a chitosan release-killing mechanism.

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