Polyelectrolyte Complex Coacervation across a Broad Range of Charge Densities.
Polyelectrolyte Complex Coacervation across a Broad Range of Charge Densities.
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DOI：
10.1021/acs.macromol.1c00703
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发表时间：
2021-07-27
期刊：
影响因子：
5.5
通讯作者：
Tirrell MV
中科院分区：
文献类型：
--
作者：
Neitzel AE;Fang YN;Yu B;Rumyantsev AM;de Pablo JJ;Tirrell MV
合成了具有近理想随机分布的带电和中性环氧乙烷共聚单体的同源（共）聚电解质的聚电解质复合凝聚体。这些构建块提供的独特平台使得能够研究电荷分数0.10 ≤ f ≤ 1.0的相行为。实验相图为f = 0.30-1.0的复杂和上层清液相的热重分析，并与分子动力学模拟和理论标度律进行对比。在中至高f下，提取了无盐凝聚层相中聚合物重量分数（wP，c）的依赖性wP，c = f0.37±0.01;该趋势与伴随的模拟预测非常一致。在f = 0.50以下，发现wP，c更显著地降低，定性地与理论和模拟预测在f ≤ 0.25时指数为2/3一致。优先盐分配到凝聚层或上清液被发现是由化学成分（共）聚电解质。
Polyelectrolyte complex coacervates of homologous (co)polyelectrolytes with a near-ideally random distribution of a charged and neutral ethylene oxide comonomer were synthesized. The unique platform provided by these building blocks enabled an investigation of the phase behavior across charge fractions 0.10 ≤ f ≤ 1.0. Experimental phase diagrams for f = 0.30–1.0 were obtained from thermogravimetric analysis of complex and supernatant phases and contrasted with molecular dynamics simulations and theoretical scaling laws. At intermediate to high f, a dependence of polymer weight fraction in the salt-free coacervate phase (wP,c) of wP,c ∼ f0.37±0.01 was extracted; this trend was in good agreement with accompanying simulation predictions. Below f = 0.50, wP,c was found to decrease more dramatically, qualitatively in line with theory and simulations predicting an exponent of 2/3 at f ≤ 0.25. Preferential salt partitioning to either coacervate or supernatant was found to be dictated by the chemistry of the constituent (co)polyelectrolytes.
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