School of Interdisciplinary Bioscience and Bioengineering, ‡Ocean Science and Technology Institute, §School of Environmental Science and Engineering, ∥Department of Chemical Engineering, and ⊥Integrative Biosciences and Biotechnology, Pohang University of Science and Technology , Pohang 790-784, Korea.
Biomacromolecules. 2014 May 12;15(5):1579-85. doi: 10.1021/bm4017308. Epub 2014 Apr 8.
Hydrogel systems based on cross-linked polymeric materials which could provide both adhesion and cohesion in wet environment have been considered as a promising formulation of tissue adhesives. Inspired by marine mussel adhesion, many researchers have tried to exploit the 3,4-dihydroxyphenylalanine (DOPA) molecule as a cross-linking mediator of synthetic polymer-based hydrogels which is known to be able to achieve cohesive hardening as well as adhesive bonding with diverse surfaces. Beside DOPA residue, composition of other amino acid residues and structure of mussel adhesive proteins (MAPs) have also been considered important elements for mussel adhesion. Herein, we represent a novel protein-based hydrogel system using DOPA-containing recombinant MAP. Gelation can be achieved using both oxdiation-induced DOPA quinone-mediated covalent and Fe(3+)-mediated coordinative noncovalent cross-linking. Fe(3+)-mediated hydrogels show deformable and self-healing viscoelastic behavior in rheological analysis, which is also well-reflected in bulk adhesion strength measurement. Quinone-mediated hydrogel has higher cohesive strength and can provide sufficient gelation time for easier handling. Collectively, our newly developed MAP hydrogel can potentially be used as tissue adhesive and sealant for future applications.
基于交联聚合物材料的水凝胶系统可以在湿环境中提供附着力和内聚力，因此被认为是一种有前途的组织粘合剂配方。受海洋贻贝黏附的启发，许多研究人员试图利用 3,4-二羟基苯丙氨酸（DOPA）分子作为合成聚合物基水凝胶的交联介质，众所周知，它能够实现内聚硬化以及与各种表面的黏附结合。除了 DOPA 残基外，贻贝黏附蛋白（MAPs）的其他氨基酸残基组成和结构也被认为是贻贝黏附的重要因素。在此，我们使用含有 DOPA 的重组 MAP 代表一种新型蛋白质基水凝胶系统。氧化诱导的 DOPA 醌介导的共价交联和 Fe(3+)介导的配位非共价交联都可以实现凝胶化。Fe(3+)介导的水凝胶在流变分析中表现出可变形和自修复的黏弹性行为，这在体黏附强度测量中也得到了很好的反映。醌介导的水凝胶具有更高的内聚强度，并为更轻松的处理提供足够的凝胶化时间。总的来说，我们新开发的 MAP 水凝胶可能有潜力作为未来应用的组织粘合剂和密封剂。
