Theory of polyelectrolyte complexation-Complex coacervates are self-coacervates
Theory of polyelectrolyte complexation-Complex coacervates are self-coacervates
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DOI：
10.1063/1.4985568
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发表时间：
2017-06-14
影响因子：
4.4
通讯作者：
Fredrickson, Glenn H.
中科院分区：
文献类型：
--
作者：
Delaney, Kris T.;Fredrickson, Glenn H.
阳离子和阴离子聚合物的混合物的络合以产生络合凝聚相是胶体和聚合物科学以及包括药物递送、传感技术和生物启发粘合剂的应用的基本重要性的主题。不幸的是，复凝聚的理论基础被广泛误解，概念错误在文献中传播。在这里，在没有盐的情况下，一个简单的对称混合物模型被用来讨论相图的显着特征，包括临界点的位置，双节点，和旋节点。有人认为，电荷补偿二聚在稀区呈现的相图带相反电荷的双嵌段混合物定性和定量类似的单组分对称二嵌段聚两性电解质溶液，一个系统能够“自凝聚”。“使用相应的双嵌段和二嵌段聚两性电解质模型的完全波动场理论模拟验证了理论预测。这些代表了第一个全面的，近似免费的凝聚和自凝聚系统的相图出现在文献中。
The complexation of mixtures of cationic and anionic polymers to produce complex-coacervate phases is a subject of fundamental importance to colloid and polymer science as well as to applications including drug delivery, sensing technologies, and bio-inspired adhesives. Unfortunately the theoretical underpinnings of complex coacervation are widely misunderstood and conceptual mistakes have propagated in the literature. Here, a simple symmetric polyelectrolyte mixture model in the absence of salt is used to discuss the salient features of the phase diagram, including the location of the critical point, binodals, and spinodals. It is argued that charge compensation by dimerization in the dilute region renders the phase diagram of an oppositely charged polyelectrolyte mixture qualitatively and quantitatively similar to that of a single-component symmetric diblock polyampholyte solution, a system capable of "self-coacervation." The theoretical predictions are verified using fully fluctuating field-theoretic simulations for corresponding polyelectrolyte and diblock polyampholyte models. These represent the first comprehensive, approximation-free phase diagrams for coacervate and self-coacervate systems to appear in the literature.