Understanding the electrostatic interactions in ion-containing polymers is crucial to better design shape memory polymers and ion-conducting membranes for multiple energy storage and conversion applications. In molten polymers, the dielectric permittivity is low, generating strong ionic correlations that lead to clustering of the charges. Here, we investigate the influence of electrostatic interactions on the nanostructure of randomly charged polymers (ionomers) using coarse-grained molecular dynamics simulations. Densely packed branched structures rich in charged species are found as the strength of the electrostatic interactions increases. Polydispersity in charge fraction and composition combined with ion correlations leads to percolated nanostructures with long-range fluctuations. We identify the percolation point at which the ionic branched nanostructures percolate and offer a rigorous investigation of the statistics of the shape of the aggregates. The extra degree of freedom introduced by the charge polydispersity leads to bicontinuous structures with a broad range of compositions, similar to neutral A–B random copolymers, as well as to desirable percolated ionic structure in randomly charged-neutral diblock copolymers. These findings provide insight into the design of conducting and robust nanostructures in ion-containing polymers.

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随机离聚物中的离子相关性

了解含离子聚合物中的静电相互作用对于更好地设计形状记忆聚合物和离子传导膜以用于多种能量存储和转换应用至关重要。在熔融聚合物中，介电常数低，会产生强烈的离子相关性，从而导致电荷聚集。在这里，我们使用粗粒度的分子动力学模拟研究静电相互作用对随机带电的聚合物（离聚物）的纳米结构的影响。随着静电相互作用强度的增加，发现了富含电荷物质的密集堆积的分支结构。电荷分数和组成的多分散性以及离子相关性导致渗透的纳米结构发生长期波动。我们确定了离子支化纳米结构的渗透点，并对聚集体的形状统计进行了严格的研究。电荷多分散性带来的额外自由度导致双连续结构具有广泛的组成范围，类似于中性A–B无规共聚物，以及无规中性二嵌段共聚物中所需的渗透离子结构。这些发现提供了对含离子聚合物中导电和坚固纳米结构设计的见解。以及无规中性二嵌段共聚物中所需的渗透离子结构。这些发现提供了对含离子聚合物中导电和坚固纳米结构设计的见解。以及无规中性二嵌段共聚物的理想渗透离子结构。这些发现提供了对含离子聚合物中导电和坚固纳米结构设计的见解。