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

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Abstract

Polylactide (PLA) has often been blended with biodegradable poly(butylene adipate-co-terephthalate) (PBAT) to improve it toughness. However, the strength and heat resistance of PLA are always sacrificed. Herein, exchangeable hydroxyl-ester crosslinks ar constructed in PLA/PBAT blends by successively introducing a tertiary amine-containing polyol, bis-(2-hydroxyethyl)amino-tri (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.

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Acknowledgments

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).

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  1. The Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China

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

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

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Zhou, XW., Huang, J., Zhang, XH. et al. Design of Tough, yet Strong, Heat-resistant PLA/PBAT Blends with Reconfigurable Shape Memory Behavior by Engineering Exchangeable Covalent Crosslinks. Chin J Polym Sci 41, 1868–1878 (2023). https://doi.org/10.1007/s10118-023-2997-0

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