Hydration and antibiofouling of TMAO-derived zwitterionic polymers surfaces studied with atomistic molecular dynamics simulations

Hidden hydrophobicity impacts polymer immunogenicity

“…2). 22,23 We also normalized DG with the solvent-accessible surface area (SASA) to provide an additional evaluation. As one -OH group could signicantly change water binding to one EG monomer, we did not calculate the monomer of OH-terminated PEG here.…”

Hydration behaviors of nonfouling zwitterionic materials

“…11,12 The presence of a strong surface hydration layer creates a signicant energy barrier at ∼3 Å above the top of pTMAO brush surfaces, 11,12 resisting adsorption of proteins of different charges, such as the positively charged lysozyme protein and the negatively charged barnacle cement protein. 12 The desorption free energy of a lysozyme protein on pTMAO brush surfaces in pure water is only ∼4.0 kT, 12 which is one order of magnitude lower than that on a trans-azobenzene-terminated fouling surface (∼60 kT). 67 Even for a large-sized barnacle cement protein, its desorption free energy on pTMAO brush surfaces in pure water is only ∼18.5 kT.…”

“…9,10 Effective foulingresistant coatings can prevent protein attachment and biofouling propagation. 9,11,12 Strong surface hydration was found to act as a barrier against biomolecules, preventing them from being adsorbed on submerged surfaces. 11,12 Hence, strong surface hydration is generally regarded as a crucial factor in the design of effective fouling-resistant coating materials.…”

“…9,11,12 Strong surface hydration was found to act as a barrier against biomolecules, preventing them from being adsorbed on submerged surfaces. 11,12 Hence, strong surface hydration is generally regarded as a crucial factor in the design of effective fouling-resistant coating materials. 4,11,13 Zwitterionic materials, which contain equally charged positive and negative moieties, have emerged as highly effective ultralow fouling materials for biomedical and engineering applications.…”

“…To overcome this issue, trimethylamine-N-oxide (TMAO) containing polymer, which exhibits excellent fouling-resistant activity in high-salt solutions, has been recently developed. 11,12 The direct connection between the positive and negative moieties, i.e., a short distance with no atom in between, in TMAO is believed to be the critical factor for its outstanding fouling-resistant property. Experimental observations 14,20 rationalized that the fouling-resistant property of zwitterionic materials increases as the length of the zwitterionic spacing (i.e., the separation between positively and negatively charged moieties) decreases.…”