Hydrophilic Polymer-Guided Polycatecholamine Assembly and Surface Deposition

Mussel-inspired surface chemistry based on polycatecholamines and polyphenols has been widely applied as a facile and universal method for modifying surfaces. Specifically, the catecholamine-assisted codeposition as a one-step strategy is a versatile strategy used to impart surface functionalities. Despite successful incorporation of numerous functional agents, very little understanding has emerged over the years regarding the mechanism behind their coassembly and codeposition. Here, we employed six different ultrahigh molecular weight hydrophilic polymers of diverse chemistry and architecture and three catecholamines and a polyphenol for investigating the coassembly and codeposition process. The chemistry of the polymers is found to influence the strength of the interaction between the polycatecholamine and the hydrophilic polymers, thus playing an important role in the aqueous self-assembly in solution to nanoaggregates, its formation kinetics, steric stabilization, and surface deposition. Additionally, the codeposition method was used as a platform for developing antifouling and antibiofilm coatings and evaluating their efficiency. Both the chemistry of hydrophilic polymers and the type of the catecholamine influence the antibiofilm properties of the coating. Our studies demonstrated that significant opportunities exist to further define the surface coating process and polycatecholamine self-assembly process by altering the polycatecholamine–hydrophilic polymer interactions.