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Computer simulations of entropic cohesion in reversibly crosslinked polymers

Karmakar, R and Venkatareddy, N and Himanshu, N and Valsecchi, M and Maiti, PK and Sastry, S and Kumar, SK and Patra, TK (2024) Computer simulations of entropic cohesion in reversibly crosslinked polymers. In: Soft Matter .

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Official URL: https://doi.org/10.1039/d4sm01161a

Abstract

Reversibly crosslinked polymer networks - polymer networks that can undergo bond association and dissociation reactions - rearrange their structures while maintaining their overall integrity, thus resulting in unique properties such as self-healing, reprocessability, shape memory and adaptability. Here, we show that the introduction of crosslinks, whether reversible or permanent, directly impacts the equilibrium polymer density and hence the material's surface tension. For a limiting case where the bonds are the same size as the polymer chain bonds, simulations, Flory hypotheses and thermodynamic calculations show that the crosslinks induce an increased entropic cohesion in the liquid. These findings implicate density as a key variable in polymers with (dynamic) crosslinkers, one that can be used to facilely tune their properties. © 2025 The Royal Society of Chemistry.

Item Type: Journal Article
Publication: Soft Matter
Publisher: Royal Society of Chemistry
Additional Information: The copyright for this article belongs to Royal Society of Chemistry
Keywords: Dissociation; Shape-memory polymer, Crosslinked polymer networks; Crosslinked polymers; Dissociation reactions; Equilibrium polymers; Network polymers; Polymer networks; Property; Reprocessability; Self-healing; Shape-memory, Crosslinking
Department/Centre: Division of Physical & Mathematical Sciences > Physics
Date Deposited: 29 Jan 2025 12:24
Last Modified: 29 Jan 2025 12:24
URI: http://eprints.iisc.ac.in/id/eprint/87327

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