Conformal Electrodeposition of Antimicrobial Hydrogels Formed by Self-Assembled Peptide Amphiphiles

The colonization of biomedical surfaces by bacterial biofilms is concerning because these microorganisms display higher antimicrobial resistance in biofilms than in liquid cultures. Developing antimicrobial coatings that can be easily applied to medically-relevant complex-shaped objects, such as implants and surgical instruments, is an important and challenging research direction. This work reports the preparation of antibacterial surfaces via the electrodeposition of a conformal hydrogel of self-assembling cationic peptide-amphiphiles (PAs). Hydrogels of three PAs are electrodeposited: C₁₆K₂, C₁₆K₃, and C₁₈K₂, where C_n is an alkyl chain of n methylene groups and K_m is an oligopeptide of m lysines. The processing variables (electrodeposition time, potential, pH, salt concentration, agitation) enable fine control of film thickness, demonstrating the flexibility of the method and allowing to unravel the mechanisms underlying electrodeposition. The electrochemically prepared hydrogels inhibit the growth of Staphylococcus aureus, Escherichia coli, and Pseudomonas aeruginosa in agar plates, and prevent the formation of biofilms of Acinetobacter baumannii and P. aeruginosa and the formation of A. baumannii colonies in solid media. C₁₆K₂ and C₁₆K₃ hydrogels outperform the antimicrobial activity of those of C₁₈K₂ while maintaining good compatibility with human cells.