Publications by Author: Ariana Annie Chen

Fouling-resistant coating materials have important applications in marine industry and biomedicine. Zwitterionic carboxybetaine polymers have demonstrated robust antibiofouling functionalities in experiments. In this work, we performed atomistic molecular dynamics simulations to study the molecular mechanism of hydration and antibiofouling of poly(carboxybetaine acrylamide) (polyCBAA) brush surfaces. We focused on the zwitterionic carboxybetaine, which has only a short methylene spacer between the positive quaternary ammonium and the negative carboxylate groups. Our study shows that a large amount of water is present within the polyCBAA surface, and a condensed water layer of single-molecular thickness covers the top of the polymer surface. Moreover, the clustering of the zwitterionic chains results in an amorphous structure of the polymer surface, a reduced degree of order in the interfacial water molecules, and weak protein attachment. The low protein desorption free energy demonstrates that the polyCBAA surface exhibits strong fouling resistance due to its significant interfacial hydration and the small dipole moment of the carboxybetaine group, minimizing protein–surface electrostatic interactions. Our study at the molecular level will be important to the future development of zwitterionic materials.

Developing fouling-resistant materials is of paramount interest in marine industries and biomedical applications. In this work, we studied the interfacial hydration and surface–protein interactions of the amphiphilic brush surface functionalized with hybrid hydrophilic trimethylamine N-oxide (TMAO) and hydrophobic pentafluoroethyl groups using a combination of atomistic molecular dynamics simulations and free-energy computations. Our results show that while the interfacial hydration density of the amphiphilic surface slightly decreases with the introduction of small fluorocarbons compared to that of the pure TMAO-functionalized surface, the amphiphilic surface remains relatively strong in resisting protein adsorption. The nanosized clustering of hydrophobic fluorine atoms on the top of the amphiphilic brush surface introduces weak protein adsorption; however, due to the strong interfacial hydration and weak hydrophobic interaction, the amphiphilic surface exhibits sufficient antibiofouling activities. Our fundamental studies will be critical for the discovery of marine fouling-resistant coating surfaces.