Reversible Temperature-Switching of Hydrogel Stiffness of Coassembled, Silk-Collagen-Like
Hydrogels
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Abstract
Recombinant protein polymers, which
can combine different bioinspired
self-assembly motifs in a well-defined block sequence, have large
potential as building blocks for making complex, hierarchically structured
materials. In this paper we demonstrate the stepwise formation of
thermosensitive hydrogels by combination of two distinct, orthogonal
self-assembly mechanisms. In the first step, fibers are coassembled
from two recombinant protein polymers: (a) a symmetric silk-like block
copolymer consisting of a central silk-like block flanked by two soluble
random coil blocks and (b) an asymmetric silk-collagen-like block
copolymer consisting of a central random-coil block flanked on one
side by a silk-like block and on the other side a collagen-like block.
In the second step, induced by cooling, the collagen-like blocks form
triple helices and thereby cross-link the fibers, leading to hydrogels
with a thermo-reversibly switchable stiffness. Our work demonstrates
how complex self-assembled materials can be formed through careful
control of the self-assembly pathway