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Surface-Initiated Atom Transfer Radical Polymerization of Oligo(ethylene glycol) Methyl Methacrylate from a Mixed Self-Assembled Monolayer on Gold†

  1. H. Ma1,4,
  2. M. Wells2,3,
  3. T. P. Beebe Jr.2,
  4. A. Chilkoti1

Article first published online: 16 FEB 2006

DOI: 10.1002/adfm.200500426

Issue

Advanced Functional Materials

Advanced Functional Materials

Volume 16, Issue 5, pages 640–648, March, 2006

Additional Information

How to Cite

Ma, H., Wells, M., Beebe, T. and Chilkoti, A. (2006), Surface-Initiated Atom Transfer Radical Polymerization of Oligo(ethylene glycol) Methyl Methacrylate from a Mixed Self-Assembled Monolayer on Gold. Advanced Functional Materials, 16: 640–648. doi: 10.1002/adfm.200500426

Author Information

  1. 1

    Department of Biomedical Engineering, Duke University, Box 90281, Durham, NC 27708-0281, USA

  2. 2

    Department of Chemistry & Biochemistry, University of Delaware, Newark, DE 19716, USA

  3. 3

    IonTof USA, Inc., Chestnut Ridge, NY 10977, USA

  4. 4

    Present address: Department of Biomedical Engineering, College of Engineering, Peking University, Beijing, 100871, P. R. China

  1. †

    The authors thank Dr. Stephen L. Craig and Dr. Stefan Zauscher for helpful discussions. H. M. was the recipient of a fellowship from the Graduate School at Duke University. This work was supported by the Centers for Disease Control through a grant (NCID R01 CI-00097-01) to A. C. and by the NIH through grants R01-NS43928 and R01-EB0049 to T. P. B.

Publication History

  1. Issue published online: 7 MAR 2006
  2. Article first published online: 16 FEB 2006
  3. Manuscript Accepted: 11 NOV 2005
  4. Manuscript Received: 6 JUN 2005

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Keywords:

  • Biomedical applications;
  • Coatings;
  • Polymer brushes;
  • Polymer films;
  • Polymerization

Graphical Abstract

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The in-situ synthesis of protein-resistant polymer films by surface-initiated ATRP of oligo(ethylene glycol) methyl methacrylate from mixed SAMs of initiator-functionalized alkanethiol/ diluent thiol is described (see Figure). Above a threshold solution molar ratio of the initiator thiol to diluent thiol of 0.2, and a dry-film thickness of ∼4 nm, fibronectin adsorption on the polymer coatings was below 1 ng cm–2.

Abstract

This paper describes the in-situ synthesis of an oligo(ethylene glycol)-functionalized polymer brush in which the oligo(ethylene glycol) chains are presented as side-chains from a methacrylate backbone that is anchored to the surface. These polymer “bottlebrushes” have been synthesized by surface-initiated atom transfer radical polymerization (SI-ATRP) of oligo(ethylene glycol) methyl methacrylate (OEGMA) from a mixed self-assembled monolayer (SAM) of an ATRP initiator-functionalized alkanethiol and a diluent, methyl-terminated thiol. The systematic control of the ATRP initiator surface density afforded by the mixed SAM on gold and the polymerization time enables the polymer chain length and surface density to be independently controlled. Surface plasmon resonance (SPR) spectroscopy of fibronectin (Fn) adsorption on poly(OEGMA) grown from the surface of the mixed SAMs on gold shows that above a threshold solution molar ratio of the ATRP-initiator thiol to methyl-terminated thiol of 0.2, and a dry film thickness of ∼ 4 nm, Fn adsorption on the surface-initiated poly(OEGMA) coatings was below the detection limit of SPR. The relatively low surface density of the ATRP initiator required to confer protein resistance to the surface suggests that SI-ATRP may be a viable strategy to create protein resistant polymer brushes on real-world materials.

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