Fabrication of Transparent PEGylated Antifouling Coatings via One-Step Pyrogallol Deposition.

Antifouling coatings are critical for many biomedical devices. A simple and universal technique used to anchor antifouling polymers is important in order to expand its applications. In this study, we introduced the pyrogallol (PG)-assisted immobilization of poly(ethylene glycol) (PEG) to deposit a thin antifouling layer on biomaterials. Briefly, biomaterials were soaked in a PG/PEG solution and PEG was immobilized onto the biomaterial surfaces via PG polymerization and deposition. The kinetics of PG/PEG deposition started with the deposition of PG on the substrates, followed by the addition of a PEG-rich adlayer. However, prolonged coating added a top-most PG-rich layer, which deteriorated the antifouling efficacy. By controlling the amounts of PG and PEG and the coating time, the PG/PEG coating was able to reduce more than 99% of the adhesion of L929 cells and the adsorption of fibrinogen. The ultrathin (tens of nanometers) and smooth PG/PEG coating was easily deposited onto a wide variety of biomaterials, and the deposition was robust enough to survive harsh sterilization conditions. Furthermore, the coating was highly transparent and allowed most of the UV and Vis light to pass through. The technique has great potential to be applied to biomedical devices that need a transparent antifouling coating, such as intraocular lenses and biosensors.

Fabrication of Polysulfobetaine Gradient Coating via Oxidation Polymerization of Pyrogallol To Modulate Biointerfaces.

A surface with a gradient physical or chemical feature, such as roughness, hardness, wettability, and chemistry, serves as a powerful platform for high-throughput investigation of cell responses to a biointerface. In this work, we developed a continuous antifouling gradient surface using pyrogallol (PG) chemistry. A copolymer of a zwitterionic monomer, sulfobetaine methacrylate, and an amino monomer, aminoethyl methacrylate, were synthesized (pSBAE) and deposited on glass slides via the deposition of self-polymerized PG. A gradient of pSBAE was fabricated on glass slides in 7 min in the presence of an oxidant, ammonium persulfate, by withdrawing the reaction solution. The modified glass slide showed a wettability gradient, determined by measuring the water contact angle. Cell adhesion and protein adsorption were well correlated with surface wettability. We expect that this simple and faster method for the fabrication of a continuous chemical gradient is applicable for high-throughput screening of surface properties to modulate biointerfaces.

One-step electrochemical deposition of antifouling polymers with pyrogallol for biosensing applications.

Electrochemical techniques are highly sensitive and label-free sensing methods for the detection of various biomarkers, toxins, or pathogens. An ideal sensing element should be electroconductive, nonfouling, and readily available for conjugation of ligands. In this work, we have developed a facile, one-step electrodeposition method based on pyrogallol polymerization for preparation of a nonfouling and biotinylated surface on indium tin oxide (ITO). A copolymer of sulfobetaine methacrylate and aminoethyl methacrylate (pSBAE) was synthesized and deposited on ITO in the presence of pyrogallol via cyclic voltammetry. The deposition took less than 15 minutes to sufficiently inhibit cell adhesion. Using biotinylated pSBAE, the modified surface resisted nonspecific protein adsorption from the fetal bovine serum solution and detected added avidin concentrations. The results show an efficient platform to fabricate an electrochemical biosensor for the detection of biomarkers. We expect that this facile one-step technology could be applied to conjugate various biosensing elements for nonfouling biosensors.