两嵌段共聚物在二元混合溶剂中的自组装：混致不溶效应的影响

李星业; 王志远; 王铮; 尹玉华; 蒋润; 张朋飞; 李宝会

doi:10.11777/j.issn1000-3304.2025.25057

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两嵌段共聚物在二元混合溶剂中的自组装：混致不溶效应的影响

研究论文 | 更新时间：2025-04-30

- 两嵌段共聚物在二元混合溶剂中的自组装：混致不溶效应的影响
- Self-assembly of Diblock Copolymer in Binary Solvent Mixtures: Effect of Co-nonsolvency
- 高分子学报 2025年页码：1-11
- 作者机构：
  
  1.南开大学物理科学学院弱光非线性光子学教育部重点实验室天津 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
  baohui@nankai.edu.cn
- 基金信息：
  
  国家自然科学基金(基金号 ┣22173051;21829301);21774066,22073016,22473024┫;教育部创新团队发展计划(IRT1257);高等学校学科创新引智计划(B16027)
- DOI：10.11777/j.issn1000-3304.2025.25057
  中图分类号：
- CSTR：32057.14.GFZXB.2025.7386
- 收稿日期：2025-03-02，
  
  录用日期：2025-03-25，
  
  网络出版日期：2025-04-30，
- 稿件说明：
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李星业, 王志远, 王铮, 尹玉华, 蒋润, 张朋飞, 李宝会. 两嵌段共聚物在二元混合溶剂中的自组装：混致不溶效应的影响. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25057

Li, X. Y.; Wang, Z. Y.; Wang, Z.; Yin, Y. H.; Jiang, R.; Zhang, P. F.; Li, B. H. Self-assembly of diblock copolymer in binary solvent mixtures: effect of co-nonsolvency. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25057
李星业, 王志远, 王铮, 尹玉华, 蒋润, 张朋飞, 李宝会. 两嵌段共聚物在二元混合溶剂中的自组装：混致不溶效应的影响. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25057 DOI： CSTR： 32057.14.GFZXB.2025.7386.

Li, X. Y.; Wang, Z. Y.; Wang, Z.; Yin, Y. H.; Jiang, R.; Zhang, P. F.; Li, B. H. Self-assembly of diblock copolymer in binary solvent mixtures: effect of co-nonsolvency. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25057 DOI： CSTR： 32057.14.GFZXB.2025.7386.

摘要

采用模拟退火方法研究了AB两嵌段共聚物在二元混合溶剂中的自组装行为. 考察了共聚物的体积分数、溶剂的性质及组成对自组装聚集体形态的影响，构建了聚集体形态随不同参量变化的相图，获得了多种不同形态的胶束，并揭示了聚集体的形成机制. 体系中两种溶剂(称为S和O)均为B嵌段的良溶剂，并且S溶剂对B嵌段的吸引作用强于O溶剂，S溶剂为A嵌段的不良溶剂. 研究发现，当S溶剂的体积分数

较小且A嵌段的体积分数

较小，或者S溶剂与A嵌段间排斥作用较弱时，B嵌段的混致不溶效应起主导作用，共聚物主要形成以B嵌段为核、A嵌段为冠的胶束. 胶束的核中有大量的S溶剂，并伴随着S溶剂的液液相分离现象. 相反，当

较大且

S溶剂与A嵌段间排斥作用较强时，溶剂与A嵌段间的排斥作用起主导作用，共聚物主要形成以A嵌段为核、B嵌段为冠的胶束. 当

居间，或

较小且

较大时，上述两种作用的竞争导致共聚物形成多样化的补丁状、层状、聚集状和大蒜状等复杂胶束形态.

Abstract

Since the 20

century

the self-assembly of macromolecules has been a major focus in polymer science research

with block copolymers serving as a typical example. These systems form a variety of aggregates with distinct morphologies in selective solvents. Recently

the phenomenon of co-nonsolvency

where macromolecules become insoluble in a mixture of two miscible solvents

each of which is a good solvent for the macromolecules

has attracted widespread attention from researchers. In this study

we investigate the self-assembly of AB diblock copolymers in binary solvent mixtures using a simulated annealing technique. We examine the influence of the volume fraction of the A-blocks (

)

as well as the properties and composition of the mixed solvents

on the self-assembled behavior of diblock copolymers

and construct phase diagrams for various systems. In our simulations

both O- a

nd S-solvents are good solvents for the B-blocks

with S-solvents exhibiting a stronger attraction for B-blocks than O-solvents

while S-solvent is a poor solvent for the A-block. Our study reveals that when the volume fraction of S-solvent

is small and when

is small

or when the repulsive interaction between the A-block and S-solvent is weak

the co-nonsolvency effect of B-block predominantly leads to the formation of the micelles with a B-core and an A-corona. Conversely

when

is large and the repulsive interaction between A-block and S-solvent is significant

this repulsion predominantly leads to the formation of the micelles with an A-core and a B-corona. When

is intermediate

or when

is small but

is large

the combined influence of these competing effects allows for the formation of diverse micelles

including patchy micelles

aggregated micelles

lamellae micelles and garlic-shaped micelles. By calculating the average contact numbers between segments and solvents

as well as the radial density distribution of the different components

we find that the micelle cores induced by the co-nonsolvency effect contain a significant amount of S-solvent

accompanied by liquid-liquid phase separation of the S-solvent; whereas the micelle cores induced by repulsion do not contain any solvent. This work provides theoretical guidance for understanding and designing novel self-assembled micelles associated with the co-nonsolvency effect.

关键词

Keywords

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