Laccase-catalyzed surface oxidation of poly(2-hydroxyethyl methacrylate) contact lens hydrogel using polyvinylamine-graft-TEMPO as mediator

Surface oxidation is a commonly used surface modification method for macromolecular biomaterials, which can increase the surface hydrophilicity and biocompatibility, and provide active sites for subsequent functional modifications. The nitroxyl radical, as represented by TEMPO, could act as an electron transfer mediator in the catalytic oxidation reaction in aqueous phase. By immobilizing TEMPO on a water-soluble polymer carrier polyvinylamine (PVAm) and using laccase as a catalyst, the surface of poly(2-hydroxyethyl methacrylate) (pHEMA) contact lens hydrogel can be selectively oxidized. Herein, polyvinylamine-graft-TEMPO was used as a polymeric electron transfer mediator to confine the oxidation reaction within the surface of the pHEMA hydrogel. The oxidized hydrogel with surface aldehydes was subsequently coated with hyaluronic acid, which gained low rate of water loss and low protein adsorption. This surface oxidation method can provide new ways for the activation, modification, and function expansion for the surface of polymeric biomaterials especially contact lens hydrogels.