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Modular Surface Functionalization of Polyisobutylene-based Biomaterials

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2014, Doctor of Philosophy, University of Akron, Polymer Science.

Polyisobutylene (PIB) has a unique combination of properties including chemical/oxidative resistance, low Tg (~70 °C) and hydrophobicity.1 PIB-based materials have also been found to have excellent biocompatibility and biostability: a PIB-based triblock copolymer thermoplastic elastomer (TPE) [poly(styrene-b-isobutylene-b-styrene)] (SIBS) is FDA-approved as a drug eluting coating for coronary stents.2 A new generation of PIB-based TPEs, with an arborescent or tree-like core (arbPIB) and plastic phases composed of blocks of polystyrene or poly(p-methyl styrene) (MS) has been developed in Professor Puskas group. These materials display unique TPE properties to make them very attractive for biomedical applications.3 The biocompatibility of these novel block copolymers has already been demonstrated in vitro and in vivo in rabbits.4

The Puskas group proposed to modify the surface properties of PIB-based TPEs using a modular approach. Using this approach it is possible to modify the surface chemistry and topology independently. The surface chemistry can be modified by “gluing” low molecular weight functionalized PIBs (PIB-X) to the surface of the TPEs. This “modular” approach will give unprecedented control over surface chemistry and topology and will contribute to new fundamental understanding of the effects of surface properties on the biocompatibility of polymeric materials. In this work PIB with a primary hydroxy head group (HO-PIB) was made in situ by living carbocationic polymerization using propylene oxide as initiator and titanium tetrachloride (TiCl4) as coinitiator. PIB functionalized with non-fouling moieties (PIB-X) was then synthesized from HO-PIB using Candida antarctica Lipase B (CALB) as enzymatic catalyst and spin coated onto the surface of the TPE. Protein adsorption studies using Surface Plasmon Resonance (SPR) demonstrated decreased fibrinogen (Fg) adsorption to the modified surface. XPS analyses provided clear evidence of the effectiveness of the modular approach in modifying the surface chemistry of the TPE revealing that the polar groups of PIB-X migrated to the surface of the film. This modular approach is much simpler than attaching functional groups covalently to surfaces; therefore it holds great promise in practical applications to improve the tissue-implant interaction.

Judit E. Puskas, Dr. (Advisor)
William Landis, Dr. (Committee Chair)
Gary R. Hamed, Dr. (Committee Member)
Chrys Wesdemiotis, Dr. (Committee Member)
Nic D. Leipzig, Dr. (Committee Member)
262 p.

Recommended Citations

Citations

  • Alvarez Albarran, A. (2014). Modular Surface Functionalization of Polyisobutylene-based Biomaterials [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron1405173637

    APA Style (7th edition)

  • Alvarez Albarran, Alejandra. Modular Surface Functionalization of Polyisobutylene-based Biomaterials. 2014. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron1405173637.

    MLA Style (8th edition)

  • Alvarez Albarran, Alejandra. "Modular Surface Functionalization of Polyisobutylene-based Biomaterials." Doctoral dissertation, University of Akron, 2014. http://rave.ohiolink.edu/etdc/view?acc_num=akron1405173637

    Chicago Manual of Style (17th edition)