Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 20, Pages 23352-23368Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c01993
Keywords
silicone implants; protein-repellent; antimicrobial; chitosan; lysine; bioactive coatings; adsorption; QCM-D
Funding
- Slovenian Research Agency [P2-0118, J4-1764]
- Spanish Ministry of Economy, Industry and Competitiveness [CTQ2017-88948-P]
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Medical implant-associated infections caused by biofilm formation are a major concern, but bioactive nanocoatings can prevent bacterial attachment and biofilm formation. A novel polyelectrolyte-surfactant complex was developed and successfully deposited on PDMS surfaces, showing strong repulsion towards blood proteins and effective antimicrobial activity against both Gram-negative and Gram-positive bacteria under dynamic conditions. This multifunctional coating has great potential in improving the design of medical devices by combining protein-repellent and antimicrobial properties.
Medical implant-associated infections resulting from biofilm formation triggered by unspecific protein adsorption are the prevailing cause of implant failure. However, implant surfaces rendered with multifunctional bioactive nanocoatings offer a promising alternative to prevent the initial attachment of bacteria and effectively interrupt biofilm formation. The need to research and develop novel and stable bioactive nanocoatings for medical implants and a comprehensive understanding of their properties in contact with the complex biological environment are crucial. In this study, we developed an aqueous stable and crosslinker-free polyelectrolyte-surfactant complex (PESC) composed of a renewable cationic polysaccharide, chitosan, a lysine-based anionic surfactant (77KS), and an amphoteric antibiotic, amoxicillin, which is widely used to treat a number of infections caused by bacteria. We successfully introduced the PESC as bioactive functional nanolayers on the model and real polydimethylsiloxane (PDMS) surfaces under dynamic and ambient conditions. Besides their high stability and improved wettability, these uniformly deposited nanolayers (thickness: 44-61 nm) with mixed charges exhibited strong repulsion toward three model blood proteins (serum albumin, fibrinogen, and gamma-globulin) and their competitive interactions in the mixture in real-time, as demonstrated using a quartz crystal microbalance with dissipation (QCM-D). The functional nanolayers with a maximum negative zeta potential (sigma: -19 to -30 mV at pH 7.4), water content (1628-1810 ng cm(-2)), and hydration (low viscosity and elastic shear modulus) correlated with the mass, conformation, and interaction nature of proteins. In vitro antimicrobial activity testing under dynamic conditions showed that the charged nanolayers actively inhibited the growth of both Gram-negative (Escherichia coli) and Gram-positive (Staphylococcus aureus) bacteria compared to unmodified PDMS. Given the ease of fabrication of multifunctional and charged biobased coatings with simultaneous protein-repellent and antimicrobial activities, the limitations of individual approaches could be overcome leading to a better and advanced design of various medical devices (e.g., catheters, prosthetics, and stents).
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