Spider-silk inspired polymeric networks by harnessing the mechanical potential of β-sheets through network guided assembly

Nicholas Jun-An Chan, Dunyin Gu, Shereen Tan, Qiang Fu, Thomas Geoffrey Pattison, Andrea J. O’Connor and Greg G. Qiao ()
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Nicholas Jun-An Chan: University of Melbourne, Parkville
Dunyin Gu: University of Melbourne, Parkville
Shereen Tan: University of Melbourne, Parkville
Qiang Fu: University of Melbourne, Parkville
Thomas Geoffrey Pattison: University of Melbourne, Parkville
Andrea J. O’Connor: University of Melbourne, Parkville
Greg G. Qiao: University of Melbourne, Parkville

Nature Communications, 2020, vol. 11, issue 1, 1-14

Abstract: Abstract The high toughness of natural spider-silk is attributed to their unique β-sheet secondary structures. However, the preparation of mechanically strong β-sheet rich materials remains a significant challenge due to challenges involved in processing the polymers/proteins, and managing the assembly of the hydrophobic residues. Inspired by spider-silk, our approach effectively utilizes the superior mechanical toughness and stability afforded by localised β-sheet domains within an amorphous network. Using a grafting-from polymerisation approach within an amorphous hydrophilic network allows for spatially controlled growth of poly(valine) and poly(valine-r-glycine) as β-sheet forming polypeptides via N-carboxyanhydride ring opening polymerisation. The resulting continuous β-sheet nanocrystal network exhibits improved compressive strength and stiffness over the initial network lacking β-sheets of up to 30 MPa (300 times greater than the initial network) and 6 MPa (100 times greater than the initial network) respectively. The network demonstrates improved resistance to strong acid, base and protein denaturants over 28 days.

Date: 2020
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DOI: 10.1038/s41467-020-15312-x

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