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revised on 12.07.2019 and posted on 12.07.2019by Pezhman Mohammadi, A. Sesilja Aranko, Christopher P. Landowski, Olli Ikkala, Wolfgang Wagermaier, Markus Linder
Silk and cellulose are biopolymers that show a high potential as future
sustainable materials.They also have complementary properties, suitable
for combination in composite materials where cellulose would form the
reinforcing component and silk the tough matrix. Therein, a major
challenge concerns balancing structure and properties in the assembly
process. We used recombinant proteins with triblock architecture
combining structurally modified spider silk with terminal cellulose
affinity modules. Flow-alignment of cellulose nanofibrils and triblock
protein allowed a continuous fiber production.The protein assembly
involved phase separation into concentrated coacervates, with subsequent
conformational switching from disordered structures to beta sheets.
This gave the matrix a tough adhesiveness, forming a new composite
material with high strength and stiffness combined with increased
toughness. We show that versatile design possibilities in protein
engineering enable new fully biological materials, and emphasize the key
role of controlled assembly at multiple length scales for realization.