Zn2+-coordinated hierarchical dynamic crosslinking in phenolized lignin-based polyurethane elastomers: mechanical self-reinforcement and dynamic adaptability enhancement

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요약

J. Mater. Chem. A, 2026, Advance ArticleDOI: 10.1039/D6TA01199C, PaperYaling Xu, Shusheng Chen, Weifeng Liu, Xueqing QiuHierarchical dynamic crosslinking integrating phenol-carbamate bonds, Zn2+ coordination bonds, and hydrogen bonds enables mechanically self…

본문

Zn2+-coordinated hierarchical dynamic crosslinking in phenolized lignin-based polyurethane elastomers: mechanical self-reinforcement and dynamic adaptability enhancement

* Corresponding authors

a School of Chemistry and Chemical Engineering, State Key Laboratory of Advanced Papermaking and Paper-based Materials, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of Technology, Guangzhou, P. R. China
E-mail: [email protected]

b School of Advanced Manufacturing, Guangdong University of Technology, Jieyang, P. R. China
E-mail: [email protected]

c Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang, P. R. China

d Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, P. R. China

Abstract

Lignin-based polyurethane elastomers (LPUes) offer a sustainable alternative to petroleum-derived counterparts yet often suffer from a trade-off between mechanical strength and dynamic reversibility. In this work, a multi-level dynamic crosslinking network comprising dynamic phenol-carbamate bonds, metal-coordination bonds, and hydrogen bonds was innovatively constructed by introducing Zn2+ into phenolized lignin-based polyurethane elastomers (Zn-LPUes). The resulting Zn-LPUes achieve an optimal balance of high mechanical performance and dynamic functionality. The optimized sample exhibits a tensile strength of 42.8 MPa, an elongation at break of 1569%, and a toughness of 270.5 MJ m−3. Notably, mechanical training efficiently induces and stabilizes chain orientation, resulting in a 50.4% tensile strength enhancement to 64.5 MPa. The hierarchical dynamic bonding enables excellent reprocessability, with 97.4% tensile strength retention after two hot-pressing cycles and over 80% retention after five cycles. Moreover, such Zn-LPUes demonstrate efficient near-infrared (NIR)-triggered self-healing, recovering 74.8% of tensile strength and 93.4% of elongation at break after 20 min of irradiation. This work provides a viable strategy to reconcile mechanical robustness with dynamic reversibility in sustainable elastomers, advancing the development of high-performance biomass-derived materials.