pH-induced metal-ligand cross-links inspired by mussel yield self-healing polymer networks with near-covalent elastic moduli

DOI Web Site 40 Citations
  • Niels Holten-Andersen
    Department of Chemistry, Institute for Biophysical Dynamics, and the James Franck Institute, University of Chicago, Chicago, IL 60637;
  • Matthew J. Harrington
    Department of Biomaterials, Max Planck Institute for Colloids and Interfaces, Potsdam 14424, Germany;
  • Henrik Birkedal
    Department of Chemistry and Interdisciplinary Nanoscience Center (iNANO), Aarhus University, Aarhus 8000, Denmark;
  • Bruce P. Lee
    Department of Biomedical Engineering and Chemistry of Life Processes Institute, Northwestern University, Evanston, IL 60208; and
  • Phillip B. Messersmith
    Department of Biomedical Engineering and Chemistry of Life Processes Institute, Northwestern University, Evanston, IL 60208; and
  • Ka Yee C. Lee
    Department of Chemistry, Institute for Biophysical Dynamics, and the James Franck Institute, University of Chicago, Chicago, IL 60637;
  • J. Herbert Waite
    Biomolecular Science and Engineering, University of California, Santa Barbara, CA 93106

Description

<jats:p> Growing evidence supports a critical role of metal-ligand coordination in many attributes of biological materials including adhesion, self-assembly, toughness, and hardness without mineralization [Rubin DJ, Miserez A, Waite JH (2010) <jats:italic>Advances in Insect Physiology: Insect Integument and Color</jats:italic> , eds Jérôme C, Stephen JS (Academic Press, London), pp 75–133]. Coordination between Fe and catechol ligands has recently been correlated to the hardness and high extensibility of the cuticle of mussel byssal threads and proposed to endow self-healing properties [Harrington MJ, Masic A, Holten-Andersen N, Waite JH, Fratzl P (2010) <jats:italic>Science</jats:italic> 328:216–220]. Inspired by the pH jump experienced by proteins during maturation of a mussel byssus secretion, we have developed a simple method to control catechol-Fe <jats:sup>3+</jats:sup> interpolymer cross-linking via pH. The resonance Raman signature of catechol-Fe <jats:sup>3+</jats:sup> cross-linked polymer gels at high pH was similar to that from native mussel thread cuticle and the gels displayed elastic moduli (G′) that approach covalently cross-linked gels as well as self-healing properties. </jats:p>

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