均聚物在二元混合溶剂中的构象与聚集行为：粗粒化分子动力学模拟

王志远; 李星业; 王铮; 尹玉华; 蒋润; 张朋飞; 李宝会

doi:10.11777/j.issn1000-3304.2025.25056

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均聚物在二元混合溶剂中的构象与聚集行为：粗粒化分子动力学模拟

研究论文 | 更新时间：2025-06-20

- 均聚物在二元混合溶剂中的构象与聚集行为：粗粒化分子动力学模拟
- Conformation and Aggregation Behavior of Homopolymers in Binary Mixed Solvents: Coarse-grained Molecular Dynamics Simulations
- 高分子学报 2025年页码：1-12
- 作者机构：
  
  1.弱光非线性光子学教育部重点实验室南开大学物理科学学院天津 300071
  2.东华大学先进纤维材料全国重点实验室先进低维材料中心材料科学与工程学院上海 201620
- 作者简介：
  
  E-mail: pfzhangphy@dhu.edu.cn;
  E-mail: baohui@nankai.edu.cn
- 基金信息：
  
  国家自然科学基金(基金号 ┣22173051;21829301);21774066,22473024,22073016┫;教育部创新团队发展计划(IRT1257);高等学校学科创新引智111计划(B16027)
- DOI：10.11777/j.issn1000-3304.2025.25056
  中图分类号：
- CSTR：32057.14.GFZXB.2025.7402
- 收稿日期：2025-03-02，
  
  录用日期：2025-04-22，
  
  网络出版日期：2025-06-20，
- 稿件说明：
移动端阅览
王志远, 李星业, 王铮, 尹玉华, 蒋润, 张朋飞, 李宝会. 均聚物在二元混合溶剂中的构象与聚集行为：粗粒化分子动力学模拟. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25056

Wang, Z. Y.; Li, X. Y.; Wang, Z.; Yin, Y. H.; Jiang, R.; Zhang, P. F.; Li, B. H. Conformation and aggregation behavior of homopolymers in binary mixed solvents: coarse-grained molecular dynamics simulations. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25056
王志远, 李星业, 王铮, 尹玉华, 蒋润, 张朋飞, 李宝会. 均聚物在二元混合溶剂中的构象与聚集行为：粗粒化分子动力学模拟. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25056 DOI： CSTR： 32057.14.GFZXB.2025.7402.

Wang, Z. Y.; Li, X. Y.; Wang, Z.; Yin, Y. H.; Jiang, R.; Zhang, P. F.; Li, B. H. Conformation and aggregation behavior of homopolymers in binary mixed solvents: coarse-grained molecular dynamics simulations. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25056 DOI： CSTR： 32057.14.GFZXB.2025.7402.

摘要

刺激-响应型聚合物因能对外界环境变化(如温度、溶液组成等)产生可逆的物理或化学响应，而具有广泛的应用前景. 这种响应可以表现为其链构象、溶解度等的变化.聚合物在混合溶剂中常表现出复杂的链构象和聚集行为，其中一个著名的例子是混致不溶(co-nonsolvency)，即聚合物在由两种良溶剂混合组成的溶液中溶解度降低的现象.然而，目前关于混致不溶现象的物理机理仍存在很大争议. 本文采用粗粒化分子动力学模拟，研究了均聚物单链和多链在混合溶剂中的链构象和聚集行为. 结果表明，在混合溶剂中，多链体系中聚合物的链构象显著不同于与其对应的单链体系的链构象，随着共溶剂比例的增加，链呈现出分散-聚集-再分散的转变，意味着混致不溶效应的发生；同时，共溶剂呈现液-液相分离

高分子和共溶剂共同形成聚集体，构成共溶剂的浓相；并且，在聚集体内部的总粒子数密度大于体系的平均粒子数密度.此外，聚合物与共溶剂之间的相互作用强度对聚合物的径向密度分布有显著影响；随着该相互作用强度的变大，聚集体内部总粒子数密度逐渐增大. 本研究揭示了混合溶剂中聚合物的微观结构的变化机制，并为理解聚合物在混合溶剂中的行为以及调控聚合物溶液的宏观性质提供理论依据.

Abstract

Stimuli-responsive polymers have broad application prospects because of their ability to exhibit reversible physical or chemical responses to external environmental changes (such as temperature and solvent composition

etc

.). Such a response can manifest as changes in the chain conformation

solubility

and other related properties. However

a unified understanding of the chain conformations and aggregation behavior of polymers in mixed solvents is lacking. A well-known example is co-nonsolvency

a phenomenon in which the solubility of a polymer decreases in a mixture of two good solvents. In this study

we investigated the chain conformations and aggregation behavior of homopolymers in both single- and multi-chain systems in binary good solvent mixture systems using coarse-grained molecular dynamics simulations. The results show that in mixed solvents

chain conformations in a multi-chain system are

significantly different from those in the corresponding single chain system. With increasing cosolvent fraction

polymers in multi-chain systems undergo a dispersion-aggregation-redispersion transition

where aggregation is induced by co-nonsolvency effects. In this case

the cosolvent undergoes liquid-liquid phase separation

where the polymer and cosolvent aggregate to form aggregates

constituting the cosolvent-rich phase. Furthermore

the total particle number density within an aggregate exceeded the average particle density of the system. In addition

the interaction strength between the polymer and cosolvent significantly affects the radial density distribution of the polymer. As the strength of this interaction increases

the total particle number density within an aggregate gradually increases. This study elucidates the mechanism of microstructural changes of polymers in mixed solvents and provides a theoretical foundation for understanding the behavior of polymers in mixed solvents

as well as for regulating the macroscopic properties of polymer solutions.

关键词

Keywords

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