Diffusive Trends in Concentrated Oppositely-Charged Polyelectrolyte Solutions and Onset of Glassy Dynamics,ACS Macro Letters

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Diffusive Trends in Concentrated Oppositely-Charged Polyelectrolyte Solutions and Onset of Glassy Dynamics
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-08-19 , DOI: 10.1021/acsmacrolett.4c00378
Harrison Landfield ₁ , Muzhou Wang ₁

Affiliation

We utilize single particle tracking studies to investigate the diffusion of polylysine through concentrated matrices of cationic polylysine and anionic polyglutamic acid with no added salts. These studies show that diffusivity has a strong apparently exponential dependence on concentration in crowded systems that does not appear to be a function of the charge sign. These trends are consistent in both single-phase systems prepared at concentrated conditions and polymer-rich coacervate phases formed from dilute phase-separating systems. The likely origin of this behavior is the onset of glassy dynamics spurred by a decrease in plasticization by water and the large excluded volume associated with charge-bearing species. This effect can be contextualized through free volume-based theories such as the Vrentas–Duda model. Overall, we obtain dynamic behavior that is distinctly different from behavior observed in more dilute systems and warrants further investigation.

中文翻译：

浓带相反电荷的聚电解质溶液的扩散趋势和玻璃态动力学的开始

我们利用单粒子跟踪研究来研究聚赖氨酸在不添加盐的情况下通过阳离子聚赖氨酸和阴离子聚谷氨酸的浓缩基质的扩散。这些研究表明，在拥挤的系统中，扩散率对浓度具有明显的指数依赖性，而这似乎不是电荷符号的函数。这些趋势在浓缩条件下制备的单相体系和由稀相分离体系形成的富含聚合物的凝聚相中是一致的。这种行为的可能起源是由于水塑化作用的减少以及与带电荷物质相关的大量排除体积而引起的玻璃态动力学的开始。这种效应可以通过基于自由体积的理论（例如 Vrentas-Duda 模型）来具体化。总的来说，我们获得的动态行为与在更稀的系统中观察到的行为明显不同，值得进一步研究。

更新日期：2024-08-19

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