Journal
NATURE COMMUNICATIONS
Volume 6, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms7892
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Funding
- NIH [U01 EB014967]
- NSF
- ONR-PECASE
- National Science Foundation (NSF) [ECS-0335765]
- Energy & Materials Initiative at the Florida State University
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Science, ICT & Future Planning [2013R1A1A010091]
- European Research Council [279985, 619448, 632277]
- European Commission under the Graphene Flagship (WP10 'Nanocomposites') [604391]
- Provincia Autonoma di Trento ('Graphene Nanocomposites') [S116/2012-242637, 2266]
- European Research Council (ERC) [619448] Funding Source: European Research Council (ERC)
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Scalable computational modelling tools are required to guide the rational design of complex hierarchical materials with predictable functions. Here, we utilize mesoscopic modelling, integrated with genetic block copolymer synthesis and bioinspired spinning process, to demonstrate de novo materials design that incorporates chemistry, processing and material characterization. We find that intermediate hydrophobic/hydrophilic block ratios observed in natural spider silks and longer chain lengths lead to outstanding silk fibre formation. This design by nature is based on the optimal combination of protein solubility, self-assembled aggregate size and polymer network topology. The original homogeneous network structure becomes heterogeneous after spinning, enhancing the anisotropic network connectivity along the shear flow direction. Extending beyond the classical polymer theory, with insights from the percolation network model, we illustrate the direct proportionality between network conductance and fibre Young's modulus. This integrated approach provides a general path towards de novo functional network materials with enhanced mechanical properties and beyond (optical, electrical or thermal) as we have experimentally verified.
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