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Int. J. Mol. Sci. 2016, 17(9), 1573;

Spider Silk-CBD-Cellulose Nanocrystal Composites: Mechanism of Assembly

The Robert H. Smith Institute of Plant Sciences and Genetics in Agriculture, Robert H. Smith Faculty of Agriculture, Food and Environment, The Hebrew University of Jerusalem, P.O. Box 12, Rehovot 76100, Israel
The Institute of Chemistry, The Hebrew University of Jerusalem, Edmond J. Safra Campus, Givat Ram, Jerusalem 91904, Israel
Department of Biomedical Engineering, 4 Colby Street, Tufts University, Medford, MA 02155, USA
Department of Physics and Astronomy, Rowan University, Glassboro, NJ 08028, USA
Author to whom correspondence should be addressed.
Academic Editors: John G. Hardy and Chris Holland
Received: 30 June 2016 / Revised: 22 August 2016 / Accepted: 8 September 2016 / Published: 18 September 2016
(This article belongs to the Special Issue Silk-Based Materials: From Production to Characterization)
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The fabrication of cellulose-spider silk bio-nanocomposites comprised of cellulose nanocrystals (CNCs) and recombinant spider silk protein fused to a cellulose binding domain (CBD) is described. Silk-CBD successfully binds cellulose, and unlike recombinant silk alone, silk-CBD self-assembles into microfibrils even in the absence of CNCs. Silk-CBD-CNC composite sponges and films show changes in internal structure and CNC alignment related to the addition of silk-CBD. The silk-CBD sponges exhibit improved thermal and structural characteristics in comparison to control recombinant spider silk sponges. The glass transition temperature (Tg) of the silk-CBD sponge was higher than the control silk sponge and similar to native dragline spider silk fibers. Gel filtration analysis, dynamic light scattering (DLS), small angle X-ray scattering (SAXS) and cryo-transmission electron microscopy (TEM) indicated that silk-CBD, but not the recombinant silk control, formed a nematic liquid crystalline phase similar to that observed in native spider silk during the silk spinning process. Silk-CBD microfibrils spontaneously formed in solution upon ultrasonication. We suggest a model for silk-CBD assembly that implicates CBD in the central role of driving the dimerization of spider silk monomers, a process essential to the molecular assembly of spider-silk nanofibers and silk-CNC composites. View Full-Text
Keywords: spider silk; cellulose nanocrystals; cellulose binding domain; nanocomposite; biomaterials spider silk; cellulose nanocrystals; cellulose binding domain; nanocomposite; biomaterials

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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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Meirovitch, S.; Shtein, Z.; Ben-Shalom, T.; Lapidot, S.; Tamburu, C.; Hu, X.; Kluge, J.A.; Raviv, U.; Kaplan, D.L.; Shoseyov, O. Spider Silk-CBD-Cellulose Nanocrystal Composites: Mechanism of Assembly. Int. J. Mol. Sci. 2016, 17, 1573.

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