A Comprehensive Landscape for Fibril Association Behaviors Encoded Synergistically by Saccharides and Peptides

A Comprehensive Landscape for Fibril Association Behaviors Encoded Synergistically by Saccharides and Peptides
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DOI:
10.1021/jacs.1c01951
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发表时间:
2021-04-26
影响因子:
15
通讯作者:
Chen, Guosong
Chen, Guosong
中科院分区:
化学1区
文献类型:
--
作者:
Liu, Rongying;Zhang, Ran;Chen, Guosong

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自然界为我们提供了一幅具有巨大结构多态的纤维全景图,从分子构建块到层级缔合行为。尽管最近在通过自组装创建具有单个构建块的人工系统方面取得了成就,但通过分子编码从模型构建块到纤维关联的关系,导致可控的宏观特性,仍然是一个难以实现的目标。在这篇文章中,通过使用一套设计的糖肽构建块并结合实验和计算工具,我们报道了一个控制纤维多态的文库,从分子堆积到纤维结合及其相关的宏观性质都得到了阐明。用右手或左手加捻时,原纤维的轴向或径向生长是由寡糖和寡肽成分的微妙权衡决定的。同时,从实验和理论上对双链纤维的缔合过程提出了明显的证据。最后,纤维多晶型在水凝胶形成和细胞迁移控制方面表现出显着不同的宏观性质。
Nature provides us a panorama of fibrils with tremendous structural polymorphism from molecular building blocks to hierarchical association behaviors. Despite recent achievements in creating artificial systems with individual building blocks through self-assembly, molecularly encoding the relationship from model building blocks to fibril association, resulting in controlled macroscopic properties, has remained an elusive goal. In this paper, by employing a designed set of glycopeptide building blocks and combining experimental and computational tools, we report a library of controlled fibril polymorphism with elucidation from molecular packing to fibril association and the related macroscopic properties. The growth of the fibril either axially or radially with right- or left-handed twisting is determined by the subtle trade-off of oligosaccharide and oligopeptide components. Meanwhile, visible evidence for the association process of double-strand fibrils has been experimentally and theoretically proposed. Finally the fibril polymorphs demonstrated significant different macroscopic properties on hydrogel formation and cellular migration control.