Self-healing Polyurethanes Based on Dynamic Imine Bonds: Influence of Imine Bond Dissociation Energy on the Optimal Self-healing Temperature

En-hao Zheng; Rong-rong Zhang; Hua-gong Yang; Zuo-peng Wang; Ya Gao; Fu-yang Song; Chong Yang; Zhao-sheng Hou

doi:10.11777/j.issn1000-3304.2025.25187

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Self-healing Polyurethanes Based on Dynamic Imine Bonds: Influence of Imine Bond Dissociation Energy on the Optimal Self-healing Temperature

Research Article | 更新时间：2026-02-01

- Self-healing Polyurethanes Based on Dynamic Imine Bonds: Influence of Imine Bond Dissociation Energy on the Optimal Self-healing Temperature
- Acta Polymerica Sinica Vol. 57, Issue 2, Pages: 409-421(2026)
- 作者机构：
  
  山东师范大学化学化工与材料科学学院济南 250014
- 作者简介：
  
  Zhao-sheng Hou, E-mail: houzs@sdnu.edu.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2025.25187
  CLC：
- CSTR：32057.14.GFZXB.2025.7486
- Received：10 August 2025，
  
  Accepted：09 October 2025，
  
  Published Online：25 December 2025，
  
  Published：20 February 2026
- 稿件说明：
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郑恩浩, 张荣荣, 杨化功, 王作鹏, 高雅, 宋福阳, 杨冲, 侯昭升. 基于动态亚胺键的自愈合聚氨酯：亚胺键解离能对最佳自愈合温度的影响. 高分子学报, 2026, 57(2), 409-421.

Zheng, E. H.; Zhang, R. R.; Yang， H. G.; Wang, Z. P.; Gao, Y.; Song, F. Y.; Yang, C.; Hou, Z. S. Self-healing polyurethanes based on dynamic imine bonds: influence of imine bond dissociation energy on the optimal self-healing temperature. Acta Polymerica Sinica (in Chinese), 2026, 57(2), 409-421.
郑恩浩, 张荣荣, 杨化功, 王作鹏, 高雅, 宋福阳, 杨冲, 侯昭升. 基于动态亚胺键的自愈合聚氨酯：亚胺键解离能对最佳自愈合温度的影响. 高分子学报, 2026, 57(2), 409-421. DOI： 10.11777/j.issn1000-3304.2025.25187. CSTR： 32057.14.GFZXB.2025.7486.

Zheng, E. H.; Zhang, R. R.; Yang， H. G.; Wang, Z. P.; Gao, Y.; Song, F. Y.; Yang, C.; Hou, Z. S. Self-healing polyurethanes based on dynamic imine bonds: influence of imine bond dissociation energy on the optimal self-healing temperature. Acta Polymerica Sinica (in Chinese), 2026, 57(2), 409-421. DOI： 10.11777/j.issn1000-3304.2025.25187. CSTR： 32057.14.GFZXB.2025.7486.

摘要

将解离能(BDE)不同的动态亚胺键引入聚氨酯(PU)网络中，系统研究了亚胺键BDE与PU自愈合性能之间关系，从而实现对最佳自愈合温度的调控. 本工作通过一步醛胺缩合合成了5种BDE介于553.1~596.5 kJ/mol的亚胺型三羟基化合物，将其作为交联剂对基于聚乙二醇的PU预聚物进行交联，并通过溶剂挥发得到系列PU膜材料. 核磁共振、红外光谱表征证实交联剂和PUs的化学结构. 采用愈合—拉伸测试评价了PU膜的在不同温度下的自愈合性能

结果表明PU膜的最佳愈合温度随着亚胺键BDE的增加而逐渐升高：低亚胺BDE (553.1 kJ/mol)的PU膜在40 ℃即可实现86.3%的最大愈合效率(

)；中等亚胺BDE (565.9 kJ/mol)的

可达82.7 %，最佳愈合温度为50 ℃；而较高亚胺BDE (596.

5 kJ/mol)的PU膜需60 ℃ 才能获得78.8%的最大愈合效率. 该研究初步揭示可通过调控动态亚胺键的 BDE值，从而为设计和制备适应不同温度的自愈合PU材料奠定理论基础.

Abstract

Dynamic imine bonds with various bond dissociation energies (BDE) were incorporated into polyurethane (PU) networks to establish a correlation between imine BDE and self-healing performance

thereby tailoring the optimum self-healing temperature of PUs. In the study

five imine-contained trihydroxy compounds with BDE ranging from 553.1 kJ/mol to 596.5 kJ/mol were first synthesized

via

aldimine condensation

the trihydroxy compounds were then used as crosslinker to react with poly(ethylene glycol)-based PU prepolymers

followed by solvent evaporation to yield a series of self-healing PU films.

H-/

C-NMR and FTIR techniques were adopted to confirm the chemical structures of the crosslinkers and PUs. The self-healing capacity of the PU films was evaluated by tensile testing of pristine and self-healed films at different healing temperature

and the results revealed that the optimum healing temperature increased gradually with the increment of imine BDE. PUs with low imine BDE (553.1 kJ/mol) exhibited maximum self-healing eff

iciency (

) of 86.3 % at 40 ℃; those with medium imine BDE (565.9 kJ/mol) required 50 ℃ to achieve

of 82.7%; whereas the

of PU films containing high imine BDE (596.5 kJ/mol) was 78.8% at healing temperature of 60 ℃. These findings preliminarily demonstrated that imine BDE could serve as a simple molecular switch for programming the optimal healing temperature of self-healable PUs

providing a design principle for next-generation self-healing materials.

关键词

Keywords

references

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