Valence can control the nonexponential viscoelastic relaxation of multivalent reversible gels
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sciadv.adl5056.pdf
Description
Published version
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811.47 KB
Format
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Checksum (MD5)
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Author(s)
Le Roy, Hugo
Song, Jake
Lundberg, David
Zhukhovitskiy, Aleksandr V
Johnson, Jeremiah A
McKinley, Gareth H
Holten-Andersen, Niels
Lenz, Martin
Date Issued
May 15, 2024
Journal
Science Advances
Publisher
American Association for the Advancement of Science
Citation
Hugo Le Roy et al., Valence can control the nonexponential viscoelastic relaxation of multivalent reversible gels. Sci. Adv.10, eadl5056 (2024).
Version
Final published version
Abstract
Gels made of telechelic polymers connected by reversible cross-linkers are a versatile design platform for biocompatible viscoelastic materials. Their linear response to a step strain displays a fast, near-exponential relaxation when using low-valence cross-linkers, while larger supramolecular cross-linkers bring about much slower dynamics involving a wide distribution of timescales whose physical origin is still debated. Here, we propose a model where the relaxation of polymer gels in the dilute regime originates from elementary events in which the bonds connecting two neighboring cross-linkers all disconnect. Larger cross-linkers allow for a greater average number of bonds connecting them but also generate more heterogeneity. We characterize the resulting distribution of relaxation timescales analytically and accurately reproduce stress relaxation measurements on metal-coordinated hydrogels with a variety of cross-linker sizes including ions, metal-organic cages, and nanoparticles. Our approach is simple enough to be extended to any cross-linker size and could thus be harnessed for the rational design of complex viscoelastic materials.
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DOI of Published Version
https://doi.org/10.1126/sciadv.adl5056
