Entropy maximization underlies topology and mechanical properties in dynamic covalent hydrogels

Fuente: arXiv
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Main Authors: Cousin, Lucien, Miotti, Pietro, Marco-Dufort, Bruno, Pivkin, Igor V., Tibbitt, Mark W.
Format: Preprint
Published: 2026
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author Cousin, Lucien
Miotti, Pietro
Marco-Dufort, Bruno
Pivkin, Igor V.
Tibbitt, Mark W.
author_facet Cousin, Lucien
Miotti, Pietro
Marco-Dufort, Bruno
Pivkin, Igor V.
Tibbitt, Mark W.
contents Adding dynamic bonds in polymer networks enables reprocessing and recycling; however the full impact of reversible bonds on dynamic network mechanics remains unclear. We build model dynamic networks and observe substantial deviations from classic theory. We rationalize these findings by considering that bond exchange enables the networks to rearrange and adopt a topology with a higher entropy. This allows us to accurately predict the gel point and elasticity of the dynamic networks. Further, we show by controlling bond exchange that network rearrangement can dramatically alter the mechanical properties, even without loss of bonds.
format Preprint
id arxiv_https___arxiv_org_abs_2603_17871
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Entropy maximization underlies topology and mechanical properties in dynamic covalent hydrogels
Cousin, Lucien
Miotti, Pietro
Marco-Dufort, Bruno
Pivkin, Igor V.
Tibbitt, Mark W.
Soft Condensed Matter
Adding dynamic bonds in polymer networks enables reprocessing and recycling; however the full impact of reversible bonds on dynamic network mechanics remains unclear. We build model dynamic networks and observe substantial deviations from classic theory. We rationalize these findings by considering that bond exchange enables the networks to rearrange and adopt a topology with a higher entropy. This allows us to accurately predict the gel point and elasticity of the dynamic networks. Further, we show by controlling bond exchange that network rearrangement can dramatically alter the mechanical properties, even without loss of bonds.
title Entropy maximization underlies topology and mechanical properties in dynamic covalent hydrogels
topic Soft Condensed Matter
url https://arxiv.org/abs/2603.17871