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

2011; National Academy of Sciences; Volume: 108; Issue: 7 Linguagem: Inglês

10.1073/pnas.1015862108

1091-6490

Niels Holten‐Andersen, Matthew J. Harrington, Henrik Birkedal, Bruce P. Lee, Phillip B. Messersmith, Ka Yee C. Lee, J. Herbert Waite,

Force Microscopy Techniques and Applications

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) Advances in Insect Physiology: Insect Integument and Color , 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) Science 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 3+ interpolymer cross-linking via pH. The resonance Raman signature of catechol-Fe 3+ 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.