Multibody Interactions, Phase Behavior, and Clustering in Nanoparticle-Polyelectrolyte Mixtures.
Multibody Interactions, Phase Behavior, and Clustering in Nanoparticle-Polyelectrolyte Mixtures.
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纳米粒子-聚电解质混合物中的多体相互作用、相行为和聚集。
DOI：
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发表时间：
2015
影响因子：
3.3
通讯作者：
V. Ganesan
中科院分区：
文献类型：
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作者：
Gunja Pandav;V. Pryamitsyn;J. Errington;V. Ganesan
我们提出了悬浮在带相反电荷的聚电解质（PE）溶液中的带电纳米颗粒（CNP）的相互作用、相行为和聚集特性的计算研究结果。我们使用了早期工作中提出的平均场聚合物自洽场论 (SCFT) 模型的扩展 (Macromolecules, 2014, 47, 6095 - 6112) 来明确表征此类系统中的多体相互作用。对于稀-中等粒子体积分数，三个和更高的多体相互作用的大小相对于对相互作用的贡献较弱。基于这些结果，我们将配对相互作用势嵌入热力学微扰理论方法中，以识别此类系统的相行为。这种框架的结果表明，气体和 FCC 晶相是热力学稳定的，而流体相在此类系统中是亚稳态的。为了补充使用 SCFT 研究的参数，我们使用最近开发的多体模拟方法来研究 CNP-PE 混合物中的聚集和簇形态。对于低粒子电荷，此类系统主要表现出由 CNP 之间直接接触聚集产生的簇。然而，对于较高的颗粒和 PE 电荷以及较低的 PE 浓度，可以看到形成大面积的 PE 桥接簇。我们提出了总结这些结果的形态相图。
We present the results of a computational study of the interactions, phase-behavior and aggregation characteristics of charged nanoparticles (CNPs) suspended in solution of oppositely charged polyelectrolytes (PEs). We used an extension of the mean-field polymer self-consistent field theory (SCFT) model presented in our earlier work ( Macromolecules , 2014 , 47 , 6095 - 6112 ) to explicitly characterize the multibody interactions in such systems. For dilute-moderate particle volume fractions, the magnitudes of three and higher multibody interactions were seen to be weak relative to the contributions from pair interactions. On the basis of such results, we embeded the pair-interaction potentials within a thermodynamic perturbation theory approach to identify the phase behavior of such systems. The results of such a framework suggested that the gas and FCC crystal phases were thermodynamically stable, whereas the fluidlike phase was metastable in such systems. To complement the parameters studied using SCFT, we used a recently developed multibody simulation approach to study the aggregation and cluster morphologies in CNP-PE mixtures. For low particle charges, such systems mainly exhibited clusters arising from direct contact aggregation between CNPs. However, for higher particle and PE charges and low PE concentrations, large regions of PE-bridged clusters were seen to form. We present a morphological phase diagram summarizing such results.
影响因子：
17.1
作者：
Murthy, Avinash K.;Stover, Robert J.;Borwankar, Ameya U.;Nie, Golay D.;Gourisankar, Sai;Truskett, Thomas M.;Sokolov, Konstantin V.;Johnston, Keith P.
通讯作者：
Johnston, Keith P.