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Synthesis, gas barrier and molecular simulation of intrinsic high-barrier polyimide bearing carbazole and amide

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Abstract

A novel diamine (3,6-CAPDA) bearing carbazole and amide group was prepared. On the basis of 3,6-CAPDA and pyromellitic dianhydride (PMDA), a high-barrier polyimide (3,6-CAPPI) was obtained through a two-step polymerization method. The 3,6-CAPPI displays excellent barrier performances and thermal stability. Its oxygen permeability (OP) and water vapor permeability (WVP) are low to 2.63 cm3·mil·m−2·day−1 and 3.22 g·mil·m−2·day−1, respectively. The 5% weight-loss temperature (Td5%) and glass transition temperature (Tg) are up to 526 °C and 431 °C, respectively. Through a combination of molecular simulation, X-ray diffraction and positron annihilation test, the effet of polymer structure on the barrier properties are fully explored. The results demonstrate that the introduction of carbazole and amide groups not only improves the chain order and rigidity, but also enhances the interchain force of polyimide, which thereby bring about enhancement of crystallinity and decreases of free volume and chain movement of 3,6-CAPPI. These factors lower the gas diffusivity and solubility in polymer matrix. Simultaneous decreases of gas diffusivity and solubility give rise to the notable enhancement of gas barrier for 3,6-CAPPI.

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Acknowledgments

This work was supported by the National Natural Science Foundation of China (No. 51603066), NSAF (U1930203, U1730142), the Natural Science Foundation of Hunan Province (No. 2019JJ40071); the Science Research Project of Hunan Provincial Department of Education (No. 18A257) and the Student Innovation and Entrepreneurship Training Program of China (No. 201911535005). We would like to thank Prof. Zhiquan Chen from Hubei Nuclear Solid Physics Key Laboratory, Department of Physics, Wuhan University for their help in the measurement of the polymer free volume.

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  1. National and Local Joint Engineering Center of Advanced Packaging Materials R & D Technology, Key Laboratory of Advanced Packaging Materials and Technology of Hunan Province, School of Packaging and Materials Engineering, Hunan University of Technology, Zhuzhou, 412007, P. R. China

    Yi-Wu Liu, Ao Tang, Jing-Hua Tan, Pan He, Xiang Zhang, Ding Wu, Yu-Hui Li & Xian-Qing Zhao

  2. Key Laboratory of Polymeric Materials and Application Technology of Hunan Province, Key Laboratory of Advanced Functional Polymer Materials of Colleges, College of Chemistry, Universities of Hunan Province, Xiangtan University, Xiangtan, 411105, P. R. China

    Hai-Liang Zhang

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  1. Yi-Wu Liu
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Liu, YW., Tang, A., Tan, JH. et al. Synthesis, gas barrier and molecular simulation of intrinsic high-barrier polyimide bearing carbazole and amide. J Polym Res 28, 31 (2021). https://doi.org/10.1007/s10965-020-02394-w

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