title: Probing structure-antifouling activity relationships of polyacrylamides and polyacrylates.
abstract: We have synthesized two different polyacrylamide polymers with amide groups (polySBAA and polyHEAA) and two corresponding polyacrylate polymers without amide groups (polySBMA and polyHEA), with particular attention to the evaluation of the effect of amide group on the hydration and antifouling ability of these systems using both computational and experimental approaches. The influence of polymer architectures of brushes, hydrogels, and nanogels, prepared by different polymerization methods, on antifouling performance is also studied. SPR and ELISA data reveal that all polymers exhibit excellent antifouling ability to repel proteins from undiluted human blood serum/plasma, and such antifouling ability can be further enhanced by presenting amide groups in polySBAA and polyHEAA as compared to polySBMA and polyHEA. The antifouling performance is positively correlated with the hydration properties. Simulations confirm that four polymers indeed have different hydration characteristics, while all presenting a strong hydration overall. Integration of amide group with pendant hydroxyl or sulfobetaine group in polymer backbones is found to increase their surface hydration of polymer chains and thus to improve their antifouling ability. Importantly, we present a proof-of-concept experiment to synthesize polySBAA nanogels, which show a switchable property between antifouling and pH-responsive functions driven by acid-base conditions, while still maintaining high stability in undiluted fetal bovine serum and minimal toxicity to cultured cells. This work provides important structural insights into how very subtle structural changes in polymers can yield great improvement in biological activity, specifically the inclusion of amide group in polymer backbone/sidechain enables to obtain antifouling materials with better performance for biomedical applications.
authors.affiliation: Department of Chemical and Biomolecular Engineering, The University of Akron, Akron, OH 44325, USA.
authors.forename: Chao
authors.initials: C
authors.lastname: Zhao
authors.forename: Jun
authors.initials: J
authors.lastname: Zhao
authors.forename: Xiaosi
authors.initials: X
authors.lastname: Li
authors.forename: Jiang
authors.initials: J
authors.lastname: Wu
authors.forename: Shenfu
authors.initials: S
authors.lastname: Chen
authors.forename: Qiang
authors.initials: Q
authors.lastname: Chen
authors.forename: Qiuming
authors.initials: Q
authors.lastname: Wang
authors.forename: Xiong
authors.initials: X
authors.lastname: Gong
authors.forename: Lingyan
authors.initials: L
authors.lastname: Li
authors.forename: Jie
authors.initials: J
authors.lastname: Zheng
mesh_terms: D000180:Acrylic Resins / Q000737:chemistry* / Q000494:pharmacology*; D000327:Adsorption / Q000187:drug effects; D057219:Biofouling / Q000517:prevention & control*; D016923:Cell Death / Q000187:drug effects; D045744:Cell Line, Tumor; D005340:Fibrinogen / Q000378:metabolism; D006801:Humans; D057446:Hydrodynamics; D020136:Hydrogel, Polyethylene Glycol Dimethacrylate / Q000737:chemistry; D006860:Hydrogen Bonding / Q000187:drug effects; D006863:Hydrogen-Ion Concentration / Q000187:drug effects; D008856:Microscopy, Fluorescence; D000080385:Nanogels; D010316:Particle Size; D011092:Polyethylene Glycols / Q000737:chemistry; D011094:Polyethyleneimine / Q000737:chemistry; D012235:Rhodamines / Q000378:metabolism; D013329:Structure-Activity Relationship; D020349:Surface Plasmon Resonance; D013997:Time Factors; D014867:Water / Q000737:chemistry; D000099166:Polyacrylamides
chemical_list: D000180:Acrylic Resins; D005340:Fibrinogen; D020136:Hydrogel, Polyethylene Glycol Dimethacrylate; D000080385:Nanogels; D011092:Polyethylene Glycols; D011094:Polyethyleneimine; D012235:Rhodamines; D014867:Water; D000099166:Polyacrylamides; C413692:polyethylene glycol polyethyleneimine nanogel; C026188:rhodamine 6G; C006903:carbopol 940