Protein metal complexes as reversible sacrificial bonds in self-healing biopolymers

深海丝是由海洋贻贝分泌的生物聚合物纤维，具有自主和内在的自我修复行为。由于线程是基于蛋白质和非细胞，他们提出了一个有吸引力的仿生模型系统，启发自我修复聚合物的发展。以往的研究表明，愈合行为的结果从可逆的蛋白质-金属交联，然而，目前还不清楚如何因素，如交联密度和分布，配体-金属组合的选择，或蛋白质亚基的层次组织影响的自我愈合行为。我们提出了一个跨学科的研究项目，旨在更好地了解金属蛋白质复合物的作用，作为可逆的交联作用的纤维核心和保护角质层的深海线程的自愈行为。此外，我们的目标是阐明自我修复的行为是如何修改和增强，通过更高层次的组织这样的交联。因此，一个比较生物学的方法，使用线程从几个相关的物种将平行进行，以检查如何愈合行为已适应和优化不同的物理条件的进化。通过在分子水平上研究深渊线的愈合行为，通过更高层次的层次结构，我们希望提取材料独立的结构和化学设计原则，以激发自主和内在自我修复聚合物的生产。

Byssal threads are biopolymeric fibers secreted by marine mussels that exhibit autonomic and intrinsic self-healing behavior . Because threads are protein-based and acellular, they present an appealing biomimetic model system for inspiring the development of self-healing polymers. Previous studies indicate that healing behavior results from reversible protein-metal cross-links; however, it is still unclear how factors such as cross-link density and distribution, choice of ligand-metal combination, or the hierarchical organization of the protein subunits influence the self-healing behavior. We propose a cross-disciplinary research project directed at better understanding the role metal-protein complexes play as reversible cross-links in the selfhealing behavior of the fibrous core and protective cuticle of byssal threads. Furthermore, we aim to elucidate how self-healing behavior is modified and enhanced through higher order organization of such cross-links. Accordingly, a comparative biological approach using threads from several related species will be undertaken in parallel to examine how healing behavior has been adapted and optimized to different physical conditions by evolution. By investigating the healing behavior of byssal threads at the molecular level up through higher levels of hierarchy, we expect to extract material-independent structural and chemical design principles to inspire the production of autonomic and intrinsic self-healing polymers.