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An Interfacial Dynamic Crosslinking Approach toward Catalyst-free and Mechanically Robust Elastomeric Vitrimer with a Segregated Structure

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Abstract

Elastomeric vitrimers with covalent adaptable networks are promising candidates to overcome the intrinsic drawbacks of conventional covalently-crosslinked elastomers; however, most elastomeric vitrimers show poor mechanical properties and require the addition of exogenous catalysts. Herein, we fabricate a catalyst-free and mechanically robust elastomeric vitrimer by constructing a segregated structure of sodium alginate (SA) in the continuous matrix of epoxidized natural rubber (ENR), and further crosslinking the composite by exchangeable hydroxyl ester bonds at the ENR-SA interfaces. The manufacturing process of the elastomeric vitrimer is facile and environmentally friendly without hazardous solvents or exogenous catalysts, as the abundant hydroxyl groups of the segregated SA phase can act as catalyst to activate the crosslinking reaction and promote the dynamic transesterification reaction. Interestingly, the segregated SA structure bears most of the load owing to its high modulus and small deformability, and thus ruptures preferentially upon deformation, leading to efficient energy dissipation. Moreover, the periodic stiffness fluctuation between rigid segregated SA phase and soft ENR matrix is beneficial to the crack-resisting. As a result, the elastomeric vitrimer manifests exceptional combination of catalyst-free, defect-tolerance, high tensile strength and toughness. In addition, the elastomeric vitrimer also exhibits multi-shape memory behavior which may further broaden its applications.

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Acknowledgments

This work was financially supported by the National Natural Science Foundation of China (Nos. 51873110 and 51790501), State Key Laboratory of Polymer Materials Engineering (No. sklpme2019-2-14), and the Fundamental Research Funds for Central Universities.

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Authors and Affiliations

  1. State Key Laboratory of Polymer Materials Engineering, College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065, China

    Yong Zhu, Jing-Li Gao, Lin-Jun Zhang, Yan Peng, Hao Wang, Fang-Wei Ling, Guang-Su Huang & Jin-Rong Wu

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  1. Yong Zhu
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  2. Jing-Li Gao
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  3. Lin-Jun Zhang
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  4. Yan Peng
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Correspondence to Jin-Rong Wu.

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An Interfacial Dynamic Crosslinking Approach toward Catalyst-free and Mechanically Robust Elastomeric Vitrimer with a Segregated Structure

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Zhu, Y., Gao, JL., Zhang, LJ. et al. An Interfacial Dynamic Crosslinking Approach toward Catalyst-free and Mechanically Robust Elastomeric Vitrimer with a Segregated Structure. Chin J Polym Sci 39, 201–210 (2021). https://doi.org/10.1007/s10118-020-2479-6

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