Liu, R.; Zhang, R.; Li, L.; Kochovski, Z.; Yao, L.; Nieh, M.P.; Lu, Y.; Shi, T.; Chen, G.: A Comprehensive Landscape for Fibril Association Behaviors Encoded Synergistically by Saccharides and Peptides. Journal of the American Chemical Society 143 (2021), p. 6622-6633
10.1021/jacs.1c01951
Abstract:
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.