高分子玻璃化转变的链长依赖性

罗锦添; 徐全印; 徐文生; 左彪

doi:10.11777/j.issn1000-3304.2024.24218

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高分子玻璃化转变的链长依赖性

综述 | 更新时间：2025-04-01

- 高分子玻璃化转变的链长依赖性
- Chain Length Dependence of Glass Transition in Polymers
- 高分子学报 2025年56卷第4期页码：539-550
- 作者机构：
  
  1.浙江理工大学化学与化工学院浙江省高分子材料表界面科学重点实验室杭州 310018
  2.中国科学院长春应用化学研究所长春 130022
- 作者简介：
  
  [ "左彪，男，1986年生. 浙江理工大学教授，博士生导师，微纳高分子及界面课题组负责人. 分别于2008、2011、2014年获浙江理工大学学士、硕士和博士学位，之后留校工作，2021年晋升教授职称；曾在日本九州大学、美国普林斯顿大学开展访问研究. 2021年获得国家优秀青年基金资助，荣获中国化学会青年化学奖. 从事表界面和微纳受限高分子动力学研究，研究包括界面高分子多级弛豫、多尺度松弛，纳米受限高分子动力学以及高分子玻璃化、物理老化等非平衡态问题，发展了表征固体高分子表面流变和分子运动的新方法，发现了高分子表面瞬时橡胶态新现象、揭示了表面动力学“伪缠结”机制等，在Nature, Phys. Rev. Lett.、Nat. Commun、Prog. Polym. Sci.、J. Phys. Chem. Lett.和Macromolecules等期刊发表论文60余篇，受到国内外科技媒体和学术机构报道." ]
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2024.24218
  中图分类号：
- CSTR：32057.14.GFZXB.2024.7306
- 收稿日期：2024-08-31，
  
  录用日期：2024-10-23，
  
  纸质出版日期：2025-04-20
- 稿件说明：
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罗锦添, 徐全印, 徐文生, 左彪. 高分子玻璃化转变的链长依赖性. 高分子学报, 2025, 56(4), 539-550

Luo, J. T.; Xu, Q. Y.; Xu, W. S.; Zuo, B. Chain length dependence of glass transition in polymers. Acta Polymerica Sinica, 2025, 56(4), 539-550
罗锦添, 徐全印, 徐文生, 左彪. 高分子玻璃化转变的链长依赖性. 高分子学报, 2025, 56(4), 539-550 DOI： 10.11777/j.issn1000-3304.2024.24218. CSTR： 32057.14.GFZXB.2024.7306.

Luo, J. T.; Xu, Q. Y.; Xu, W. S.; Zuo, B. Chain length dependence of glass transition in polymers. Acta Polymerica Sinica, 2025, 56(4), 539-550 DOI： 10.11777/j.issn1000-3304.2024.24218. CSTR： 32057.14.GFZXB.2024.7306.

摘要

玻璃化转变的微观机制是凝聚态物理最重要的科学问题之一. 由于链的连通性，高分子表现比小分子物质更复杂的玻璃化行为. 本综述对半个多世纪以来，科学家对高分子玻璃化转变链长依赖性的研究进行了总结. 介绍了高分子玻璃化温度(

)和脆度指数(

)等性质随链长增加而增大并趋于饱和的普遍现象；总结了解释和描述

和

随链长变化的3种主要机制：即高运动活性链末端促进高分子协同运动，从而降低

和

；局部链刚性随链长增加而增大从而减弱链段运动能力，使

升高；分子链内次级松弛单元的耦合和动态促进激活链段松弛，造成

随链长增大而增大. 希望通过对高分子玻璃化现象和机理的总结与讨论帮助读者加深对长链大分子玻璃化转变的认识和理解.

Abstract

Glass transition is one of the most important properties of condensed matter. Chain connectivity endows polymers with complex glass transition behaviour that varies with the chain length. We have summarized more than half a century of research on the chain length dependence of glass transition of polymers. In the first part

we discussed the general phenomenon of the increase in glass transition temperature (

) and dynamical fragility (

) with increasing chain length until they reach saturation values. In the second part

the mechanisms proposed in the past decades to explain the general behaviour of the polymer glass transition were reviewed

including (1) the chain end effect

i.e.

the chain ends associated with extra mobility and excess conformational freedom play a role in accelerating segmental movement and lowering polymer

; (2) the chain stiffness effect

i.e.

the polymer chains stiffened as the molecular weight in

creased

leading to an increase in

with chain length before reaching the thresholds; (3) intramolecular coupling effect

i.e.

dynamic couplings of secondary relaxations along the chains facilitate the segmental relaxation

leading to an increase of

with the chain length. We hope this review helps the readers gain a deeper understanding of the glass transition of polymers and the associated molecular mechanisms.

关键词

Keywords

references

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