Tuning chain interaction entropy in complex coacervation using polymer stiffness, architecture, and salt valency
Tuning chain interaction entropy in complex coacervation using polymer stiffness, architecture, and salt valency
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DOI：
10.1039/c7me00108h
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发表时间：
2018-02
期刊：
影响因子：
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通讯作者：
T. K. Lytle;C. Sing
中科院分区：
文献类型：
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作者：
T. K. Lytle;C. Sing
带相反电荷的聚电解质可以在盐溶液中进行液-液相分离，从而产生聚合物致密的“凝聚”相，该相已被用于从食品科学到自组装材料的广泛应用中。凝聚体可以通过改变参数如盐的作为盐浓度和化合价、盐的长度和盐的特性来调整以用于特定的应用。最近的模拟和理论已经开始阐明分子结构对凝聚相行为的作用，特别是对于表现出高电荷密度的常见合成聚电解质。在这篇手稿中，我们使用转移矩阵理论和蒙特卡罗模拟相结合，以了解在物理水平上如何一系列的分子特征，特别是聚合物的结构和刚度，和盐价可以用来设计这些材料的相图。我们展示了一个物理图片的复杂凝聚的基本熵驱动的过程是如何受到这种广泛的物理属性。
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.