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Tuning chain interaction entropy in complex coacervation using polymer stiffness, architecture, and salt valency

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Abstract

Oppositely-charged polyelectrolytes can undergo a liquid–liquid phase separation in a salt solution, resulting in a polymer-dense ‘coacervate’ phase that has found use in a wide range of applications from food science to self-assembled materials. Coacervates can be tuned for specific applications by varying parameters such as salt concentration and valency, polyelectrolyte length, and polyelectrolyte identity. Recent simulation and theory has begun to clarify the role of molecular structure on coacervation phase behavior, especially for common synthetic polyelectrolytes that exhibit high charge densities. In this manuscript, we use a combination of transfer matrix theory and Monte Carlo simulation to understand at a physical level how a range of molecular features, in particular polymer architecture and stiffness, and salt valency can be used to design the phase diagrams of these materials. We demonstrate a physical picture of how the underlying entropy-driven process of complex coacervation is affected by this wide range of physical attributes.

Graphical abstract: Tuning chain interaction entropy in complex coacervation using polymer stiffness, architecture, and salt valency

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Publication details

The article was received on 30 Sep 2017, accepted on 06 Nov 2017 and first published on 06 Nov 2017


Article type: Paper
DOI: 10.1039/C7ME00108H
Citation: Mol. Syst. Des. Eng., 2018, Advance Article
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    Tuning chain interaction entropy in complex coacervation using polymer stiffness, architecture, and salt valency

    T. K. Lytle and C. E. Sing, Mol. Syst. Des. Eng., 2018, Advance Article , DOI: 10.1039/C7ME00108H

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