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  Influence of network topology on the viscoelastic properties of dynamically crosslinked hydrogels

Grad, E. M., Tunn, I., Voerman, D., Sanz de León, A., Hammink, R., & Blank, K. G. (2020). Influence of network topology on the viscoelastic properties of dynamically crosslinked hydrogels. Frontiers in Chemistry, 8: 536. doi:10.3389/fchem.2020.00536.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-AE6B-F Version Permalink: http://hdl.handle.net/21.11116/0000-0006-C4E9-6
Genre: Journal Article

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 Creators:
Grad, Emilia M.1, Author
Tunn, Isabell1, Author              
Voerman, Dion, Author
Sanz de León, Alberto1, Author              
Hammink, Roel, Author
Blank, Kerstin G.1, Author              
Affiliations:
1Kerstin Blank, Mechano(bio)chemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2301698              

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Free keywords: hydrogel, rheology, coiled coil, polyisocyanopeptide, polyethylene glycol, relaxation time, network topology, multivalency
 Abstract: Biological materials combine stress relaxation and self-healing with non-linear stress-strain responses. These characteristic features are a direct result of hierarchical self-assembly, which often results in fiber-like architectures. Even though structural knowledge is rapidly increasing, it has remained a challenge to establish relationships between microscopic and macroscopic structure and function. Here, we focus on understanding how network topology determines the viscoelastic properties, i.e., stress relaxation, of biomimetic hydrogels. We have dynamically crosslinked two different synthetic polymers with one and the same crosslink. The first polymer, a polyisocyanopeptide (PIC), self-assembles into semi-flexible, fiber-like bundles, and thus displays stress-stiffening, similar to many biopolymer networks. The second polymer, 4-arm poly(ethylene glycol) (starPEG), serves as a reference network with well-characterized structural and viscoelastic properties. Using one and the same coiled coil crosslink allows us to decouple the effects of crosslink kinetics and network topology on the stress relaxation behavior of the resulting hydrogel networks. We show that the fiber-containing PIC network displays a relaxation time approximately two orders of magnitude slower than the starPEG network. This reveals that crosslink kinetics is not the only determinant for stress relaxation. Instead, we propose that the different network topologies determine the ability of elastically active network chains to relax stress. In the starPEG network, each elastically active chain contains exactly one crosslink. In the absence of entanglements, crosslink dissociation thus relaxes the entire chain. In contrast, each polymer is crosslinked to the fiber bundle in multiple positions in the PIC hydrogel. The dissociation of a single crosslink is thus not sufficient for chain relaxation. This suggests that tuning the number of crosslinks per elastically active chain in combination with crosslink kinetics is a powerful design principle for tuning stress relaxation in polymeric materials. The presence of a higher number of crosslinks per elastically active chain thus yields materials with a slow macroscopic relaxation time but fast dynamics at the microscopic level. Using this principle for the design of synthetic cell culture matrices will yield materials with excellent long-term stability combined with the ability to locally reorganize, thus facilitating cell motility, spreading, and growth.

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Language(s): eng - English
 Dates: 2020-06-302020
 Publication Status: Published in print
 Pages: -
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 Table of Contents: -
 Rev. Method: -
 Identifiers: DOI: 10.3389/fchem.2020.00536
BibTex Citekey: 10.3389/fchem.2020.00536
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Title: Frontiers in Chemistry
  Abbreviation : Front. Chem.
Source Genre: Journal
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Publ. Info: Lausanne, Switzerland : Frontiers Media
Pages: - Volume / Issue: 8 Sequence Number: 536 Start / End Page: - Identifier: ISSN: 2296-2646