title: Reversible Temperature-Switching of Hydrogel Stiffness of Coassembled, Silk-Collagen-Like Hydrogels.
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.
authors.affiliation: †Physical Chemistry and Soft Matter, Wageningen University, Dreijenplein 6, NL-6703 HB Wageningen, The Netherlands.
authors.forename: Wolf H
authors.initials: WH
authors.lastname: Rombouts
authors.affiliation: ⊥TI-COAST, Science Park 904, NL-1098 XH Amsterdam, The Netherlands.
authors.forename: Daan W
authors.initials: DW
authors.lastname: de Kort
authors.affiliation: †Physical Chemistry and Soft Matter, Wageningen University, Dreijenplein 6, NL-6703 HB Wageningen, The Netherlands.
authors.forename: Thao T H
authors.initials: TT
authors.lastname: Pham
authors.forename: Carlo P M
authors.initials: CP
authors.lastname: van Mierlo
authors.affiliation: §Wageningen UR Food and Biobased Research, Bornse Weilanden 9, NL-6708 WG Wageningen, The Netherlands.
authors.forename: Marc W T
authors.initials: MW
authors.lastname: Werten
authors.affiliation: §Wageningen UR Food and Biobased Research, Bornse Weilanden 9, NL-6708 WG Wageningen, The Netherlands.
authors.forename: Frits A
authors.initials: FA
authors.lastname: de Wolf
authors.affiliation: †Physical Chemistry and Soft Matter, Wageningen University, Dreijenplein 6, NL-6703 HB Wageningen, The Netherlands.
authors.forename: Jasper
authors.initials: J
authors.lastname: van der Gucht
mesh_terms: D000595:Amino Acid Sequence; D003094:Collagen / Q000138:chemical synthesis / Q000737:chemistry*; D020136:Hydrogel, Polyethylene Glycol Dimethacrylate / Q000138:chemical synthesis / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D057927:Hydrophobic and Hydrophilic Interactions; D011108:Polymers / Q000138:chemical synthesis / Q000737:chemistry; D011994:Recombinant Proteins / Q000138:chemical synthesis* / Q000737:chemistry; D047011:Silk / Q000138:chemical synthesis / Q000737:chemistry*; D013696:Temperature
chemical_list: D011108:Polymers; D011994:Recombinant Proteins; D047011:Silk; D020136:Hydrogel, Polyethylene Glycol Dimethacrylate; D003094:Collagen