Polyphenolic compounds present in tea, red wine, and chocolate form thin adherent polyphenol films on substrates through spontaneous adsorption from solution. From this observation emerged a versatile and comprehensive approach to surface modification of a variety of solid, porous, and nanoparticulate substrates composed of metals, ceramics, and polymers (see picture; ROS=reactive oxygen species).

A growing number of device-related nosocomial infections, elevated hospitalization costs, and patient morbidity necessitate the development of novel antibacterial strategies for clinical devices. We have previously demonstrated a simple, aqueous polydopamine dip-coating method to functionalize surfaces for a wide variety of uses. Here, we extend this strategy with the goal of imparting antifouling and antimicrobial properties to substrates, exploiting the ability of polydopamine to immobilize polymers and induce metal nanoparticle formation. Polydopamine was deposited as a thin adherent film of 4 nm thickness from alkaline aqueous solution onto polycarbonate substrates, followed by grafting of antifouling polymer polyethylene glycol and in situ deposition of silver nanoparticles onto the polydopamine coated polycarbonate substrates. Elemental and morphological surface analyses confirmed successful grafting of polyethylene glycol brushes onto polydopamine-coated substrates, as well as spontaneous silver nanoparticle formation for polydopamine-coated substrates incubated in silver-nitrate solutions. Sustained silver release was observed over at least 7 days from silver-coated substrates, and the release kinetics could be modulated via additional polydopamine overlayers. In vitro functional assays employing gram negative and positive strains demonstrated dual fouling resistance and antibacterial properties of the coatings due to the fouling resistance of grafted polyethylene glycol and antibacterial effect of silver, respectively. Polycarbonate substrates coated only with silver using a method similar to existing commercial coatings provided an antibacterial effect but failed to inhibit bacterial attachment. Taking into account the previously demonstrated substrate versatility of polydopamine coatings, our findings suggest that this strategy could be implemented on a variety of substrate materials to simultaneously improve antifouling and antimicrobial performance.

The strong interfacial properties of selected plant polyphenols were recently exploited in forming functionally versatile nanocoatings via dip-coating. Here, we screened a library of ~20 natural and synthetic phenols and polyphenols, identifying eight catechol-, gallol- and resorcinol-rich precursors capable of forming coatings. Several newly identified compounds expand the molecular diversity of tannin-inspired coatings.

Poly(N-substituted glycine) “peptoids” are a class of peptidomimetic molecules receiving significant interest as engineered biomolecules. Sarcosine (i.e. poly(N-methyl glycine)) has the simplest sidechain chemical structure of this family. In this contribution, we demonstrate that surface-grafted polysarcosine (PSAR) brushes exhibit excellent resistance to non-specific protein adsorption and cell attachment. Polysarcosine was coupled to a mussel adhesive protein inspired DOPA-Lys pentapeptide, which enabled solution grafting and control of the surface chain density of the PSAR brushes. Protein adsorption was found to decrease monotonically with increasing grafted chain densities, and protein adsorption could be completely inhibited above certain critical chain densities specific to different polysarcosine chain-lengths. The dependence of protein adsorption on chain length and density was also investigated by a molecular theory. PSAR brushes at high chain length and density were shown to resist fibroblast cell attachment over a 7 wk period, as well as resist the attachment of some clinically relevant bacteria strains. The excellent antifouling performance of PSAR may be related to the highly hydrophilic character of polysarcosine, which was evident from high-pressure liquid chromatography measurements of polysarcosine and water contact angle measurements of the PSAR brushes. Peptoids have been shown to resist proteolytic degradation and polysarcosine could be produced in large quantities by N-carboxy anhydride polymerization. In summary, surface grafted polysarcosine peptoid brushes hold great promise for antifouling applications.

Polyphenolverbindungen, die in Tee, Rotwein und Schokolade vorkommen, bilden auf Trägermaterialien dünne haftende Polyphenolfilme durch spontane Adsorption aus einer Lösung. Auf der Grundlage dieser Beobachtung wurde ein allgemein anwendbarer Prozess zur Oberflächenmodifizierung von festen, porösen und nanopartikulären Metall‐, Keramik‐ und Polymermaterialien entwickelt (siehe Bild; ROS=reaktive Sauerstoffspezies).