A simultaneously antimicrobial, protein-repellent, and cell-compatible surface-attached polymer network is reported, which reduces the growth of bacterial biofilms on surfaces through its multifunctionality. The coating was made from a poly(oxonorbornene)-based zwitterion (PZI), which was surface-attached and cross-linked in one step by simultaneous UV-activated CH insertion and thiol-ene reaction. The process was applicable to both laboratory surfaces like silicon, glass, and gold and real-life surfaces like polyurethane foam wound dressings. The chemical structure and physical properties of the PZI surface and the two reference surfaces SMAMP ("synthetic mimic of an antimicrobial peptide"), an antimicrobial but protein-adhesive polymer coating, and PSB (poly(sulfobetaine)), a protein-repellent but not antimicrobial polyzwitterion coating were characterized by Fourier transform infrared spectroscopy, ellipsometry, contact angle measurements, photoelectron spectroscopy, swellability measurements (using surface plasmon resonance spectroscopy, SPR), zeta potential measurements, and atomic force microscopy. The time-dependent antimicrobial activity assay (time-kill assay) confirmed the high antimicrobial activity of the PZI; SPR was used to demonstrate that it was also highly protein-repellent. Biofilm formation studies showed that the material effectively reduced the growth of Escherichia coli and Staphylococcus aureus biofilms. Additionally, it was shown that the PZI was highly compatible with immortalized human mucosal gingiva keratinocytes and human red blood cells using the Alamar Blue assay, the live-dead stain, and the hemolysis assay. PZI thus may be an attractive coating for biomedical applications, particularly for the fight against bacterial biofilms on medical devices and in other applications.

Contact-active antimicrobial polymer surfaces bear cationic charges and kill or deactivate bacteria by interaction with the negatively charged parts of their cell envelope (lipopolysaccharides, peptidoglycan, and membrane lipids). The exact mechanism of this interaction is still under debate. While cationic antimicrobial polymer surfaces can be very useful for short-term applications, they lose their activity once they are contaminated by a sufficiently thick layer of adhering biomolecules or bacterial cell debris. This layer shields incoming bacteria from the antimicrobially active cationic surface moieties. Besides discussing antimicrobial surfaces, this feature article focuses on recent strategies that were developed to overcome the contamination problem. This includes bifunctional materials with simultaneously presented antimicrobial and protein-repellent moieties; polymer surfaces that can be switched from an antimicrobial, cell-attractive to a cell-repellent state; polymer surfaces that can be regenerated by enzyme action; degradable antimicrobial polymers; and antimicrobial polymer surfaces with removable top layers.

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Biofilm-associated infections of medical devices are a global problem. For the prevention of such infections, biomaterial surfaces are chemically or topographically modified to slow down the initial stages of biofilm formation. In the bifunctional material here presented, chemical and topographical cues are combined, so that protein and bacterial adhesion as well as bacterial proliferation are effectively inhibited. Upon changes in the surface topography parameters and investigation of the effect of these changes on bioactivity, structure−property relationships are obtained. The target material is obtained by microcontact printing (μCP), a soft lithography method. The antimicrobial component, poly(oxanorbornene)-based synthetic mimics of an antimicrobial peptide (SMAMP), was printed onto a protein-repellent polysulfobetaine hydrogel, so that bifunctional 3D structured polymer surfaces with 1, 2, and 8.5 μm spacing are obtained. These surfaces are characterized with fluorescence microscopy, surface plasmon resonance spectroscopy, atomic force microscopy, and contact angle measurements. Biological studies show that the bifunctional surfaces with 1 and 2 μm spacing are 100% antimicrobially active against Escherichia coli and Staphylococcus aureus, 100% fibrinogen-repellent, and nontoxic to human gingival mucosal keratinocytes. At 8.5 μm spacing, the broad-band antimicrobial activity and the protein repellency are compromised, which indicates that this spacing is above the upper limit for effective simultaneous antimicrobial activity and protein repellency of polyzwitterionic−polycationic materials.