The adherence of bacteria and the formation of biofilm on implants is a serious problem that often leads to implant failure. A series of antimicrobial coatings have been constructed to resist bacterial adherence or to kill bacteria through contact with or release of antibacterial agents. The accumulation of dead bacteria facilitates further bacterial contamination and biofilm development. Herein, we have designed and constructed a novel, reversibly switchable bactericidal and antifouling surface through surface-initiated reversible addition-fragmentation chain transfer (RAFT) polymerization to combine thermally responsive N-isopropylacrylamide (NIPAAm) and bactericidal quaternary ammonium salts (2-(dimethylamino)-ethyl methacrylate (DMAEMA)). Measurements of spectroscopic ellipsometry and water contact angle and X-ray photoelectron spectroscopy were used to examine the process of the surface functionalization. The temperature-responsive P(DMAEMA-co-NIPAAm) copolymer coating can switch by phase transition between a hydrophobic capturing surface at high temperatures and a relatively hydrophilic antifouling surface at lower temperatures. The quaternary ammonium salts of PDMAEMA displayed bactericidal efficiency against both Escherichia coli and Staphylococcus aureus. The functionalized surface could efficiently prevent bovine serum albumin adsorption and had good biocompatibility against human lens epithelial cells.
Bacteria adhesion on the surface of biomaterials and following biofilm formation are important problems in biomedical applications. The charged antibiotics with small molar mass can hardly deposit alternately with polymers into multilayered films to load the drug. Herein, the (poly(acrylic acid)-gentamicin/poly(ethylenimine))n ((PAA-GS/PEI)n) multilayer film was designed and constructed via a layer-by-layer self-assembly method. Low molar mass GS cations were first combined with polyanion PAA and self-assembled with PEI to form multilayer films showing exponential growth behavior. The GS dosage could be adjusted by changing the layer number of films. Furthermore, the thermal cross-linking method was used to control the release rate of GS in PBS buffer. Owing to the diffusion of GS, a zone of inhibition of about 7.0 mm showed the efficient disinfection activity of the multilayer film. It could also be seen from the biofilm inhibition assay that the multilayer film effectively inhibited bacterial adhesion and biofilm formation. As the drug loading dosage was 160 μg/cm(2), the multilayer films showed very low cytotoxicity against human lens epithelial cells. The present work provides an easy way to load GS into multilayer films which can be applied to surface modification of implants and biomedical devices.
Once a biomedical implant is implanted into a human body, proteins and bacteria can easily colonize the implant, and subsequently, a biofilm can grow on the surface. A biofilm can protect the inhabiting bacteria against macrophages and neutrophil cell attack from the host immune system. The most important issue for artificial antibacterial surfaces is the accumulation of the bacteria corpse after they are killed by contact, which promotes further adhesion of bacteria and biofilm formation. Therefore, we constructed a novel multifunctional bactericidal and fouling release antibacterial surface through the combination of temperature-responsive N-vinylcaprolactam (VCL), hydrophilic 2-methacryloyloxyethyl phosphorylcholine (MPC) and a bactericidal quaternary ammonium salt (2-(dimethylamino)-ethyl methacrylate (DMAEMA)). The terpolymer coating was prepared through surface-initiated reversible addition-fragmentation chain-transfer (RAFT) polymerization and characterized using water contact angle measurements, atomic force microscopy and spectroscopic ellipsometry. At a temperature above the lower critical solution temperature (LCST), the P(VCL-co-DMAEMA-co-MPC) terpolymer coating was in a compressed and hydrophobic state with low moisture content, which displayed bactericidal efficiency against Gram-positive Staphylococcus aureus. The coating could be switched into a relatively hydrophilic surface at a temperature below the LCST, which showed self-cleaning properties against both bacteria and bovine serum albumin. The functionalized surface showed good biocompatibility against human lens epithelial cells as evaluated by morphology studies and activity measurements.
Implant-associated bacterial infections pose serious medical and financial issues due to the colonization and proliferation of pathogens on the surface of the implant. The as-prepared traditional antibacterial surfaces can neither resist bacterial adhesion nor inhibit the development of biofilm over the long term. Herein, novel (montmorillonite/poly-l-lysine-gentamicin sulfate) ((MMT/PLL-GS)) organic-inorganic hybrid multilayer films were developed to combine enzymatic degradation PLL for on-demand self-defense antibiotics release. Small molecule GS was loaded into the multilayer films during self-assembly and the multilayer films showed pH-dependent and linear growth behavior. The chymotrypsin- (CMS) and bacterial infections-responsive film degradation led to the peeling of the films and GS release. Enzyme-responsive GS release exhibited CMS concentration dependence as measured by the size of the inhibition zone and SEM images. Notably, the obtained antibacterial films showed highly efficient bactericidal activity which killed more than 99.9% of S. aureus in 12 h. Even after 3 d of incubation in S. aureus, E. coli or S. epidermidis solutions, the multilayer films exhibited inhibition zones of more than 1.5 mm in size. Both in vitro and in vivo antibacterial tests indicated good cell compatibility, and anti-inflammatory, and long-term bacterial anti-adhesion and biofilm inhibition properties.
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