Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks

Xiao-Wen Zhou; Jing Huang; Xu-Hui Zhang; Ting Li; Yang Wang; Shi-Bo Wang; Bi-Hua Xia; Wei-Fu Dong

doi:10.1007/s10118-023-2997-0

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Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks

RESEARCH ARTICLE | Updated：2023-11-27

- Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks
- Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks
- 高分子科学（英文版） 2023年41卷第12期页码：1868-1878
- Affiliations：
  
  The Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China
- Author bio：
  
  jinghuang@jiangnan.edu.cn (J.H.)
  wfdong@jiangnan.edu.cn (W.F.D.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 21975108 and 52103082), Fundamental Research Funds for the Central Universities (No. JUSRP122016), Wuxi "Light of Taihu Lake" Science and Technology Research Plan (Basic Research, No. K20221008).;Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-023-2997-0.
- DOI：10.1007/s10118-023-2997-0
  中图分类号： M
- 收稿：2023-03-21，
  
  修回：2023-4-29，
  
  录用：2023-5-5，
  
  网络首发：2023-06-15，
  
  纸质出版：2023-12-01
- Accepted：
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Zhou, X. W.; Huang, J.; Zhang, X. H.; Li, T.; Wang, Y.; Wang, S. B.; Xia, B. H.; Dong, W. F. Design of tough, yet strong, heat-resistant PLA/PBAT blends with reconfigurable shape memory behavior by engineering exchangeable covalent crosslinks. Chinese J. Polym. Sci. 2023, 41, 1868–1878

Xiao-Wen Zhou, Jing Huang, Xu-Hui Zhang, et al. Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks[J]. Chinese Journal of Polymer Science, 2023, 41(12): 1868-1878.
Zhou, X. W.; Huang, J.; Zhang, X. H.; Li, T.; Wang, Y.; Wang, S. B.; Xia, B. H.; Dong, W. F. Design of tough, yet strong, heat-resistant PLA/PBAT blends with reconfigurable shape memory behavior by engineering exchangeable covalent crosslinks. Chinese J. Polym. Sci. 2023, 41, 1868–1878 DOI： 10.1007/s10118-023-2997-0.

Xiao-Wen Zhou, Jing Huang, Xu-Hui Zhang, et al. Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks[J]. Chinese Journal of Polymer Science, 2023, 41(12): 1868-1878. DOI： 10.1007/s10118-023-2997-0.

摘要

Exchangeable hydroxyl-ester crosslinks were programmed into biodegradable PLA/PBAT blends by straightforward reactive blending. The resultant vitrimeric PLA/PBAT blends show concurrently and significantly enhanced tensile strength

toughness

and heat resistance due to the greatly improved interfacial adhesion and the network structure. Moreover

the vitrimeic PLA/PBAT blends exhibit good reconfigurable shape memory behavior.

Abstract

Polylactide (PLA) has often been blended with biodegradable poly(butylene adipate-

-terephthalate) (PBAT) to improve its toughness. However

the strength and heat resistance of PLA are always sacrificed. Herein

exchangeable hydroxyl-ester crosslinks are constructed in PLA/PBAT blends by successively introducing a tertiary amine-containing polyol

bis-(2-hydroxyethyl)amino-tris (hydroxymethyl)methane (BTM) and 4

4’-diphenylmethane diisocyanate (MDI)

via

reactive blending. BTM can react with both PLA and PBAT by transesterification

generating PLA or PBAT chains with terminal or pendant hydroxyl groups

which can then react with MDI to form networks. With internal catalysis of tertiary amine moiety in BTM

transesterification between the residual hydroxyl groups and ester bonds can occur at high temperatures

endowing the PLA/PBAT network with vitrimeric properties. Owning to the transesterification and chain extension reactions with MDI between PLA and PBAT

the interfacial adhesion is greatly improved. As a result of the excellent interfacial adhesion and the network structure

the prepared PLA/PBAT blends show greatly enhanced heat resistance and toughness (more than 40 times that of PLA) while maintaining high stiffness comparable to PLA. Furthermore

the prepared PLA/PBAT blends exhibit promising reconfigurable shape memory behavior. The present work provides a new and facile way to achieve high-performance and functional biodegradable polymeric materials.

关键词

Keywords

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