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

被引:1328
作者
Holten-Andersen, Niels [1 ,2 ]
Harrington, Matthew J. [3 ]
Birkedal, Henrik [4 ,5 ]
Lee, Bruce P. [6 ,7 ]
Messersmith, Phillip B. [6 ,7 ]
Lee, Ka Yee C. [1 ,2 ]
Waite, J. Herbert [8 ]
机构
[1] Univ Chicago, Dept Chem, Inst Biophys Dynam, Chicago, IL 60637 USA
[2] Univ Chicago, James Franck Inst, Chicago, IL 60637 USA
[3] Max Planck Inst Colloids & Interfaces, Dept Biomat, D-14424 Potsdam, Germany
[4] Aarhus Univ, Dept Chem, DK-8000 Aarhus, Denmark
[5] Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus, Denmark
[6] Northwestern Univ, Dept Biomed Engn, Evanston, IL 60208 USA
[7] Northwestern Univ, Chem Life Proc Inst, Evanston, IL 60208 USA
[8] Univ Calif Santa Barbara, Santa Barbara, CA 93106 USA
基金
美国国家卫生研究院; 美国国家科学基金会;
关键词
biomaterials; catecholate polymer; metal coordination; reversible cross-links; physical gels; TYROSINE-HYDROXYLASE; RESONANCE RAMAN; ADHESIVE; PROTEIN; COMPLEXATION; CHEMISTRY; COATINGS; CUTICLE; GEL;
D O I
10.1073/pnas.1015862108
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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 Jerome 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-Fe3+ interpolymer cross-linking via pH. The resonance Raman signature of catechol-Fe3+ 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.
引用
收藏
页码:2651 / 2655
页数:5
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