AbstractPolymeric species have been introduced to low molecular weight gelators to tailor their nucleation and rheological behavior. This work combines polymers and molecular gels (MGs) in a different manner by using polymers as the major component in a solution. Additionally, using polymers above their entanglement molecular weight is a step towards building polymer–MG composite materials. Specifically, a cholesterol-pyridine (CP) molecular gel was introduced to poly(ethylene oxide-co-epichlorohydrin) (EO-EPI) and poly(vinyl acetate) (PVAc), which have dissimilar chain conformations in anisole. Dynamic light scattering, scanning electron microscopy, and temperature-dependent small- and wide-angle X-ray studies were utilized to investigate the influence of the solution properties of high molecular weight EO-EPI and PVAc on the CP network structure. The collapsed chain conformation and aggregation of EO-EPI led to isolated, branched CP fiber networks, resulting in unexpectedly high dissociation temperatures. In contrast, PVAc gels displayed transient fiber networks, as evidenced by fiber wrapping and bundling. Cooperative interactions between PVAc and CP resulted in gels with dissociation temperatures higher than those of pure CP gels. These structural characteristics significantly influenced the gel mechanics. The collapsed chain conformation of EO-EPI led to weaker, more viscous gels, and the freely extended PVAc chain conformation led to interconnected, elastic gels independent of the molecular gel concentration.Polymer chain conformation was utilized to control the nucleation of a cholesterol-pyridine molecular gel. Collapsed chain conformations influence gel structure and dissociation behavior by acting as physical barriers that lead to confinement effects and permanent networks. An extended polymer chain conformation allowed for polymer–molecular-gel interactions and increased dissociation temperatures due to its highly ordered structure, resulting in transient networks. Additionally, the high molecular weight polymer solution behavior guided solution mechanics, where collapsed chains lead to viscous solutions and gels and extended chains led to elastic gel networks.

中文翻译：

---

高分子量聚合物添加剂对低分子量凝胶的成核作用

摘要聚合物种类已被引入低分子量凝胶剂以调整其成核和流变行为。这项工作通过使用聚合物作为溶液中的主要成分，以不同的方式将聚合物和分子凝胶 (MG) 结合起来。此外，使用高于其缠结分子量的聚合物是朝着构建聚合物-MG 复合材料迈出的一步。具体来说，将胆固醇-吡啶 (CP) 分子凝胶引入聚 (环氧乙烷-共-表氯醇) (EO-EPI) 和聚 (醋酸乙烯酯) (PVAc)，它们在苯甲醚中具有不同的链构象。利用动态光散射、扫描电子显微镜和随温度变化的小角度和广角 X 射线研究来研究高分子量 EO-EPI 和 PVAc 的溶液性质对 CP 网络结构的影响。EO-EPI 的折叠链构象和聚集导致孤立的、支化的 CP 纤维网络，导致意外的高解离温度。相比之下，PVAc 凝胶显示出瞬时纤维网络，如纤维包裹和捆绑所证明的那样。PVAc 和 CP 之间的协同相互作用导致凝胶的解离温度高于纯 CP 凝胶的解离温度。这些结构特征显着影响了凝胶力学。EO-EPI 的折叠链构象导致凝胶变弱、更粘稠，而自由延伸的 PVAc 链构象导致相互连接的弹性凝胶，与分子凝胶浓度无关。聚合物链构象用于控制胆固醇-吡啶的成核分子凝胶。折叠的链构象通过充当导致限制效应和永久网络的物理障碍来影响凝胶结构和解离行为。由于其高度有序的结构，延伸的聚合物链构象允许聚合物-分子-凝胶相互作用并增加解离温度，从而产生瞬态网络。此外，高分子量聚合物溶液行为指导溶液力学，其中坍塌的链导致粘性溶液和凝胶，延伸的链导致弹性凝胶网络。