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Solvent-Free Synthesis of Self-Healable and Recyclable Crosslinked Polyurethane Based on Dynamic Oxime-Urethane Bonds

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Abstract

Polyurethane is widely used for its versatility in design and range of performance. Self-healing and recyclable dynamic polyurethane networks have attracted extensive attention due to their potential to extend service life and ensure safety in use, as well as to promote sustainable use of resources. Developing green and environment-friendly methods to obtain this material is an interesting and challenging task, as the majority of current dynamic polyurethane networks utilize the solution polymerization method. The use of solvents makes the processes complicated, harmful to environment, and increase the cost. Poly(oxime-urethanes) (POUs) are emerging dynamic polyurethanes and show great potential in diverse fields, such as biomaterials, hot melt adhesives, and flexible electronics. In this study, we utilized the solubility properties of dimethylglyoxime in raw material poly(ethylene glycol) to prepare POUs through bulk polymerization for the first time. This method is simple, convenient and cost-efficient. Simultaneously, copper ion coordination improves POUs strength and dynamic properties, with mechanical strength up from 0.54 MPa to 1.03 MPa and self-healing recovery rate up from 85.5% to 91.8%, and activation energy down from 119.6 kJ/mol to 95.4 kJ/mol. To demonstrate the application of this technology, self-healing and stretchable circuits are constructed from this dynamic polyurethane network.

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Acknowledgments

This work was financially supported by the National Key Research and Development Program of China (No. 2021YFC2101800), the National Natural Science Foundation of China (Nos. 52173117 and 21991123), the Natural Science Foundation of Shanghai (No. 20ZR1402500), Belt & Road Young Scientist Exchanges Project of Science and Technology Commission Foundation of Shanghai (No. 20520741000), Ningbo 2025 Science and Technology Major Project (No. 2019B10068) and the Science and Technology Commission of Shanghai (No. 20DZ2254900).

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Authors and Affiliations

  1. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Institute of Functional Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, China

    Yuepeng Wang, Lei Yang, Luzhi Zhang, Hongfei Huang, Bo Qian, Shijia Gu & Zhengwei You

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  1. Yuepeng Wang
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  2. Lei Yang
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  3. Luzhi Zhang
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Correspondence to Zhengwei You.

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Wang, Y., Yang, L., Zhang, L. et al. Solvent-Free Synthesis of Self-Healable and Recyclable Crosslinked Polyurethane Based on Dynamic Oxime-Urethane Bonds. Chin J Polym Sci 41, 1725–1732 (2023). https://doi.org/10.1007/s10118-023-3009-0

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