Fouling-Resistant Hydrogels Prepared by the Swelling-Assisted Infusion and Polymerization of Dopamine

Biofilm-associated infections stemming from medical devices are increasingly challenging to treat due to the spread of antibiotic resistance. In this study, we present a simple strategy that significantly enhances the antifouling performance of covalently cross-linked poly(ethylene glycol) (PEG) and physically cross-linked agar hydrogels by incorporation of the fouling-resistant polymer zwitterion, poly(2-methacryloyloxyethyl phosphorylcholine) (pMPC). Dopamine polymerization was initiated during swelling of the hydrogels, which provided dopamine and pMPC, an osmotic driving force into the hydrogel interior. Both PEG and agar hydrogels were synthesized over a broad range of storage moduli (1.7-1300 kPa), which remained statistically equivalent after being functionalized with pMPC and polydopamine (PDA). When challenged with fibrinogen, a model blood-clotting protein, the pMPC/PDA-functionalized PEG and agar hydrogels displayed a >90% reduction in protein adsorption compared to hydrogel controls. Further, greater than an order-of-magnitude reduction in Escherichia coli and Staphylococcus aureus adherence was observed. This study demonstrates a versatile material platform to enhance the fouling resistance of hydrogels through a pMPC/PDA incorporation strategy that is independent of the chemical composition and network structure of the original hydrogel.