Future directions in physiochemical modeling of the thermodynamics of polyelectrolyte coacervates
Future directions in physiochemical modeling of the thermodynamics of polyelectrolyte coacervates
复制标题
聚电解质凝聚层热力学物理化学建模的未来方向
DOI：
10.1002/aic.17646
复制
发表时间：
2022
期刊：
影响因子：
3.7
通讯作者：
Larson, Ronald G.
中科院分区：
文献类型：
--
作者：
Ghasemi, Mohsen;Larson, Ronald G.
我们回顾了聚电解质（PE）凝聚的理论，它是带相反电荷的 PE 单元的自发缔合，并在水溶液中相分离成聚合物致密相。最简单的理论可以分为“基于物理”和“基于化学”的方法。在前者中，PE 被视为带电荷的长链分子，由电荷水平、链长度和链柔韧性定义，但缺乏化学特性，静电相互作用驱动凝聚。 “基于化学”的方法侧重于化学特性至关重要的物种之间的局部相互作用，并将凝聚描述为单体和盐的竞争性局部结合相互作用的结果。在本文中，我们通过介绍考虑物理和化学效应的最新方法来展示这些方法如何相互补充。最后，我们提出了通过考虑长程静电和局部化学特异性相互作用来定量预测理论的未来方向。
We review theories of polyelectrolyte (PE) coacervation, which is the spontaneous association of oppositely charged units of PEs and phase separation into a polymer‐dense phase in aqueous solution. The simplest theories can be divided into “physics‐based” and “chemistry‐based” approaches. In the former, PEs are treated as charged, long‐chain, molecules, defined by charge level, chain length, and chain flexibility, but otherwise lacking chemical identity, with electrostatic interactions driving coacervation. The “chemistry‐based” approaches focus on the local interactions between the species for which chemical identity is critical, and describe coacervation as the result of competitive local binding interactions of monomers and salts. In this article, we show how these approaches complement each other by presenting recent approaches that take both physical and chemical effects into account. Finally, we suggest future directions toward producing theories that are made quantitatively predictive by accounting for both long range electrostatic and local chemically specific interactions.