Dynamic Antimicrobial Poly(disulfide) Coatings Exfoliate Biofilms On Demand Via Triggered Depolymerization

Abstract Bacterial biofilms are notoriously problematic in applications ranging from biomedical implants to ship hulls. Cationic, amphiphilic antibacterial surface coatings delay the onset of biofilm formation by killing microbes on contact, but they lose effectiveness over time due to non‐specific binding of biomass and biofilm formation. Harsh treatment methods are required to forcibly expel the biomass and regenerate a clean surface. Here, a simple, dynamically reversible method of polymer surface coating that enables both chemical killing on contact, and on‐demand mechanical delamination of surface‐bound biofilms, by triggered depolymerization of the underlying antimicrobial coating layer, is developed. Antimicrobial polymer derivatives based on α‐lipoic acid (LA) undergo dynamic and reversible polymerization into polydisulfides functionalized with biocidal quaternary ammonium salt groups. These coatings kill >99.9% of Staphylococcus aureus cells, repeatedly for 15 cycles without loss of activity, for moderate microbial challenges (≈10 ⁵ colony‐forming units (CFU) mL ⁻¹ , 1 h), but they ultimately foul under intense challenges (≈10 ⁷ CFU mL ⁻¹ , 5 days). The attached biofilms are then exfoliated from the polymer surface by UV‐triggered degradation in an aqueous solution at neutral pH. This work provides a simple strategy for antimicrobial coatings that can kill bacteria on contact for extended timescales, followed by triggered biofilm removal under mild conditions.