巨型分子的黏弹性研究进展

罗锦添; 欧阳希凯; 刘庚鑫

doi:10.11777/j.issn1000-3304.2020.20056

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巨型分子的黏弹性研究进展

专论 | 更新时间：2021-01-26

- 巨型分子的黏弹性研究进展
- Progress in the Viscoelasticity Study of Giant Molecules
- 高分子学报 2020年51卷第7期页码：687-697
- 作者机构：
  
  东华大学先进低维材料中心纤维材料改性国家重点实验室材料科学与工程学院　上海 201620
- 作者简介：
  
  [ "刘庚鑫，男，1989年生. 东华大学先进低维材料中心特聘研究员，博士生导师. 2010年获得中国科学技术大学高分子科学与工程系理学学士学位，2015年于美国阿克伦大学高分子科学系获博士学位，导师王十庆教授. 随后，在阿克伦大学高分子科学系程正迪教授课题组进行博士后研究. 于2018年9月入职东华大学. 曾获：Frank Kelly Award (2013年，阿克伦大学高分子科学与工程学院)，优秀自费留学生奖学金(2014年，国家留学基金委). 研究方向为巨型分子的动力学、高分子非线性流变学及应用" ]
- 基金信息：
  
  国家自然科学基金青年基金(基金号 21903013)资助项目
- DOI：10.11777/j.issn1000-3304.2020.20056
  中图分类号：
- 纸质出版日期：2020-7，
  
  网络出版日期：2020-6-24，
  
  收稿日期：2020-3-5，
  
  修回日期：2020-4-14，
扫描看全文
罗锦添, 欧阳希凯, 刘庚鑫. 巨型分子的黏弹性研究进展[J]. 高分子学报, 2020,51(7):687-697.

Jin-tian Luo, Xi-kai Ouyang, Geng-xin Liu. Progress in the Viscoelasticity Study of Giant Molecules[J]. Acta Polymerica Sinica, 2020,51(7):687-697.
罗锦添, 欧阳希凯, 刘庚鑫. 巨型分子的黏弹性研究进展[J]. 高分子学报, 2020,51(7):687-697. DOI： 10.11777/j.issn1000-3304.2020.20056.

Jin-tian Luo, Xi-kai Ouyang, Geng-xin Liu. Progress in the Viscoelasticity Study of Giant Molecules[J]. Acta Polymerica Sinica, 2020,51(7):687-697. DOI： 10.11777/j.issn1000-3304.2020.20056.

摘要

巨型分子是一类新型高分子，其构建基元为结构更具刚性的分子纳米粒子，如多面体齐聚倍半硅氧烷(POSS)等. 将多个分子纳米粒子三维连接而形成的一类巨型分子能够保持三维形状，这不同于传统的一维链状高分子. 我们采用流变学手段研究了一系列处于本体条件、且具有不同直径的巨型分子，发现在玻璃化转变温度之上，其动力学由其直径决定. 这与传统高分子中缠结主导的动力学截然不同：当巨型分子的直径跨过临界直径时，其松弛时间增加至少10

倍；在临界直径以上的巨型分子不能扩散和松弛，表现出储能模量的平台，而且模量随温度线性增加，对应于分子纳米粒子的受限运动. 跳出传统高分子的框架，巨型分子展现出不同于“蛇形运动”、“缠结”和“管子模型”的新规律，成为连接高分子体系和胶体体系的桥梁. 随机一级相变理论推测，玻璃化转变时协同运动区域的直径大约为微观运动单元直径的6倍，这个分界与实验中巨型分子的临界直径一致，因此我们将这种类似于玻璃化的状态称为协同玻璃态. 以这些巨型分子为代表的软团簇或可类比为玻璃化中的协同运动区域，将为研究玻璃化转变提供新的实验支持.

Abstract

Giant molecules are a new type of precise polymers whose building blocks are rather rigid molecular nanoparticles

e.g.

polyhedral oligomeric silsesquioxane (POSS). Giant molecules containing a large number of molecular nanoparticles connected in 3-dimension have persistent 3-dimensional shape

and are different from traditional chain-like polymers. We studied a series of hydrophilic giant molecules and associated clusters of hydrophobic giant molecules. Their dynamics in the bulk state

above their glass transition temperature (

) is governed by their diameter

unlike the dynamics of traditional polymers which is governed by entanglement. The relaxation of giant molecules slows down by at least 10

when their diameters increases across the critical diameter. Giant molecules that are larger than the critical diameter cannot relax or diffuse. The exhibited elastic modulus plateau is proportional to temperature

corresponding to the confinement on individual “nanoatom”. 3-Dimensional giant molecules exhibit new rules other than reptation

entanglement

and tube in traditional polymer

and may bridge polymers and colloids. Random First Order Transition theory derived that

at the onset of glass transition

cooperative rearranging regions are 6 times the diameter of basic moving units. This is in accordance with our results. We claim large giant molecules are in a glass-like state

namely cooperative glass. Soft clusters such as giant molecules may resemble the cooperative rearranging region

thus experimentally supporting deeper understanding on glass transition.

关键词

巨型分子流变学动力学软团簇协同玻璃态缠结

Keywords

Giant moleculesRheologyDynamicsSoft-clusterCooperative glassEntanglement

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