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Structural Manipulation of Aminal-crosslinked Polybutadiene for Recyclable and Healable Elastomers

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Abstract

Recently, increasingly growing efforts have been devoted to incorporating dynamic covalent bonds into covalently crosslinked networks to address the persistent trade-offs between chemical crosslinking and malleability. Herein, a series of dynamic aminal bond crosslinked polybutadiene rubbers (PAPB) are prepared by crosslinking aldehyde group-terminated polybutadiene rubber (APB) with piperazine. By varying the molecular weight of APB, the crosslinking density of PAPB is changed, which offers the platform to regulate the mechanical characteristics and dynamic properties. Specially, with the decrease of APB molecular weight, i.e. with the increase of crosslinking density, the modulus of PAPB gradually increases while the elongation at break conversely decreases, and the activation energy for network rearrangement initially decreases and then increases. The resultant PAPB exhibit vitrimer-like behaviors that can alter the network topologies at elevated temperatures without the loss of structural integrity through dissociative aminal exchange reactions, while the protic source can accelerate aminal dissociation and result in network dissolution even at room temperature. Due to the aminal exchange, PAPB are thermally malleable and can almost restore the original mechanical characteristics after recycling; besides, they are capable of healing at a relatively low crosslinking density.

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Acknowledgments

The work was financially supported by the National Science Fund for Distinguished Young Scholars (No. 51825303) and the National Natural Science Foundation of China (Nos. 52073097 and 51790503).

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Authors and Affiliations

  1. Department of Polymer Materials and Engineering, South China University of Technology, Guangzhou, 510640, China

    Zheng-Hai Tang, Hui Zeng, Si-Qi Wei, Si-Wu Wu & Bao-Chun Guo

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  1. Zheng-Hai Tang
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  2. Hui Zeng
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  3. Si-Qi Wei
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  5. Bao-Chun Guo
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Correspondence to Zheng-Hai Tang or Bao-Chun Guo.

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Tang, ZH., Zeng, H., Wei, SQ. et al. Structural Manipulation of Aminal-crosslinked Polybutadiene for Recyclable and Healable Elastomers. Chin J Polym Sci 39, 1337–1344 (2021). https://doi.org/10.1007/s10118-021-2626-8

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