Construction of Self-defensive Antibacterial and Osteogenic AgNPs/Gentamicin Coatings with Chitosan as Nanovalves for Controlled release

Abstract

To solve the Ti implants-associated infection and poor osseointegration problems, we have constructed the AgNPs/gentamicin (Gen)-loaded silk fibroin (SF) coating with acceptable antibacterial and osteogenic aptitude. Nevertheless, due to uncontrollably sustained drug release, this bactericidal coating encountered some tricky problems, such as local high Ag concentration, short life-span and potential cytotoxicity. In this work, a chitosan (CS) barrier layer was constructed to prebuilt the SF-based film by two means, dip-coating (DCS) and spin-coating (SCS). Intriguingly, the CS barrier layer constructed by spin-coating highly improved the hydrophilic and protein-absorbed performances. As verified in the release profile, both coatings showed a prolonged and pH-dependent pattern of Ag+ with an accelerated release in acidic condition. Also, the multilayer coating with a SCS barrier layer showed an apparent bacteria-trigged antibacterial and biofilm-inhibited performances, whereas the improvements of antibacterial abilities of DCS coating were limited. The mechanisms could be explained that the pH decrease induced by the attachment and proliferation of bacteria triggered collapse of CS barrier layer, accelerating the release of bactericides. Moreover, benefitted from pH-dependent release behavior of Ag and bioactive SCS layer, functional coatings highly enhanced the initial adhesion, migration and proliferation of preosteoblast MC3T3-E1 cells, and subsequently accelerated osteoblast differentiation (alkaline phosphatase production). A relevant aspect of this work was to demonstrate the essential effect of reasonable construction of self-defensive barrier layer in achieving the balance between the high-efficiency bacterial killing and osteogenic activity, and highlighted its excellent potential in clinical applications.