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Mechanically Robust, Reprocessable, and Light-Controlled Healable Solvent-Free Lignin-Containing Polyurethane Elastomers Based on Dynamic Phenol-Carbamate Network
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    Mechanically Robust, Reprocessable, and Light-Controlled Healable Solvent-Free Lignin-Containing Polyurethane Elastomers Based on Dynamic Phenol-Carbamate Network
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    • Jin Peng
      Jin Peng
      School of Chemistry and Chemical Engineering, State Key Laboratory of Pulp and Paper Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of Technology, Wushan Road 381, Guangzhou 510640, P. R. China
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    • Haixu Wang
      Haixu Wang
      School of Chemistry and Chemical Engineering, State Key Laboratory of Pulp and Paper Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of Technology, Wushan Road 381, Guangzhou 510640, P. R. China
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    • Shusheng Chen*
      Shusheng Chen
      School of Advanced Manufacturing, Guangdong University of Technology, Jieyang 515200, P. R. China
      Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, P. R. China
      Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Waihuan Xi Road 100, Guangzhou, Guangdong 510006, P. R. China
      *Email: [email protected]
    • Weifeng Liu*
      Weifeng Liu
      School of Chemistry and Chemical Engineering, State Key Laboratory of Pulp and Paper Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of Technology, Wushan Road 381, Guangzhou 510640, P. R. China
      Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, P. R. China
      *Email: [email protected]
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    • Xueqing Qiu
      Xueqing Qiu
      Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, P. R. China
      Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Waihuan Xi Road 100, Guangzhou, Guangdong 510006, P. R. China
      More by Xueqing Qiu
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    Macromolecules

    Cite this: Macromolecules 2025, XXXX, XXX, XXX-XXX
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    https://doi.org/10.1021/acs.macromol.4c02258
    Published January 9, 2025
    © 2025 American Chemical Society

    Abstract

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    In this study, we introduce an innovative one-step, solvent-free approach for preparing lignin-containing polyurethane elastomers (LPUes) with nanomicro phase-separated structure and dynamic dual-cross-linking networks comprising both phenol-carbamate bonds (PCBs) and hydrogen bonds. This distinctive structural design imparted exceptional mechanical properties to the LPUes. The sample containing 22.9 wt % phenolized lignin exhibited tensile strength of 44.6 MPa, elongation at break of 714.6%, and toughness of 148.0 MJ/m3. The abundance of dynamic PCBs also conferred remarkable reprocessing capabilities, with these LPUes retaining over 98% for tensile strength and 94.4% for toughness after two hot-pressing cycles. Moreover, the incorporation of lignin endowed the LPUes with photothermal properties, facilitating efficient light-controlled self-healing and shape-memory functionalities. This work offers an innovative pathway to harmonize the mechanical properties and thermal adaptability in the development of sustainable and high-performance LPUes, thereby opening their avenues for diverse potential applications.

    © 2025 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.4c02258.

    • GPC spectra of AKL and CAL; tensile hysteresis stress-strain curves of 30CAL-1.2-PE1 and 30AKL-1.2-PE1 with a fixed strain of 600%; tensile hysteresis stress-strain curves of 30CAL-1.2-PE1 and 30AKL-1.2-PE1 at varying strains; tensile stress-strain curve of 30CAL-0.9-PT1; tensile stress-strain curves of 30PAL-0.9-PT1 and 30PAOH-0.9-PT1 before and after two hot-pressing cycles; synthetic formulations; mechanical properties, reprocessing properties, light-controlled self-healing properties; TG date; shape memory performance of LPUes; content of various hydroxyl groups and relative molecular weight of PAL and PAOH and mechanical properties of LPUes after aging for 3 days at 100 °C (PDF)

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    Macromolecules

    Cite this: Macromolecules 2025, XXXX, XXX, XXX-XXX
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.4c02258
    Published January 9, 2025
    © 2025 American Chemical Society

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