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Evidence of a two-step process and pathway dependency in the thermodynamics of poly(diallyldimethylammonium chloride)/poly(sodium acrylate) complexation

机译:证据表明两步过程和途径依赖   聚(二烯丙基二甲基氯化铵)/聚(钠)的热力学   丙烯酸酯)络合

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摘要

Recent studies have pointed the importance of polyelectrolyte assembly in theelaboration of innovative nanomaterials. Beyond their structures, manyimportant questions on the thermodynamics of association remain to be answered.Here, we investigate the complexation between poly(diallyldimethylammoniumchloride) (PDADMAC) and poly(sodium acrylate) (PANa) chains using a combinationof three techniques: isothermal titration calorimetry (ITC), static and dynamiclight scattering and electrophoresis. Upon addition of PDADMAC to PANa orvice-versa, the results obtained by the different techniques agree well witheach other, and reveal a two-step process. The primary process is the formationof highly charged polyelectrolyte complexes of sizes 100 nm. The secondaryprocess is the transition towards a coacervate phase made of rich and poorpolymer droplets. The binding isotherms measured are accounted for using aphenomenological model that provides the thermodynamic parameters for eachreaction. Small positive enthalpies and large positive entropies consistentwith a counterion release scenario are found throughout this study. Beyond,this work stresses the importance of the underestimated formulation pathway ormixing order in polyelectrolyte complexation.
机译:最近的研究指出聚电解质组装在创新纳米材料的制造中的重要性。除了它们的结构外,关于缔合热力学的许多重要问题仍有待回答。在这里,我们使用三种技术的组合研究聚二烯丙基二甲基氯化铵(PDADMAC)和聚丙烯酸钠(PANa)链之间的络合作用: ITC),静态和动态光散射和电泳。反之,将PDADMAC添加到PANa时,通过不同技术获得的结果彼此非常吻合,并揭示了一个两步过程。主要过程是形成大小为100 nm的高电荷聚电解质复合物。次级过程是向由富和弱聚合物小滴组成的凝聚相过渡。使用现象学模型解释所测量的结合等温线,该现象学模型为每种反应提供热力学参数。在整个研究过程中,发现与反离子释放情形一致的小正焓和大正熵。除此之外,这项工作强调了低估配方途径或混合顺序在聚电解质络合中的重要性。

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