Chem. J. Chinese Universities ›› 2025, Vol. 46 ›› Issue (9): 20250098.doi: 10.7503/cjcu20250098

• Polymer Chemistry • Previous Articles     Next Articles

Robust, Self-healing Polyurethane Hydrogel Enabled by Dual Crosslinking of Dynamic Disulfide and Hydrogen Bonds

YANG Bing1, DING Xia1, XU Jun2, LI Ye3, GU Rui2, ZHANG Hui1, HOU Zhaosheng2()   

  1. 1.School of Intelligence Engineering,Shandong Management University,Jinan 250357,China
    2.College of Chemistry,Chemical Engineering and Materials Science,Shandong Normal University,Jinan 250014,China
    3.Jinan Kangqiao Pharmaceutical Co. ,Ltd. ,Jinan 250101,China
  • Received:2025-04-03 Online:2025-09-10 Published:2025-07-07
  • Contact: HOU Zhaosheng E-mail:houzs@sdnu.edu.cn
  • Supported by:
    the Natural Science Foundation of Shandong Province, China(ZR2022MB099)

Abstract:

This study developed a new kind of self-healing polyurethane hydrogels(SPUGs) through a synergistic crosslinking strategy combining dynamic covalent disulfide bonds and non-covalent hydrogen bonds. A specifically synthesized quadrifunctional crosslinker, 3,3'-disulfanediylbis(propane-1,2-diol), was employed to react with poly(ethylene glycol)-based polyurethane prepolymers, followed by solvent-exchange method to produce SPUGs. The physicochemical properties of SPUGs and lyophilized gels(DSPUGs) were characterized comprehensively, and the results revealed that the dual-crosslinked systems exhibited enhanced thermal stability[temperature at 5% mass loss(T5%)>250 ℃] and low glass transition temperature(Tg<0 ℃). With the increase of disulfide bond content, the surface hydrophilicity and equilibrium swelling ratio of SPUGs reduced, while water-retaining capacity increased. Mechanical tests demonstrated that SPUGs exhibited elastic deformation and possessed outstanding tensile properties, compressive toughness and fatigue-resistant capacities. SPUG-II with a moderate crosslinking density achieved a maximum tensile strength of 112.2 kPa, elongation at break of 459.4% and fracture toughness of 267.6 kJ/m3. The double dynamic bonds endowed SPUGs with high self-healing efficiency(≥90% at 50 ℃ for 2 h) and redox-triggered reversible gel-sol transitions. Methyl thiazolyl tetrazolium(MTT) assays confirmed favorable cytocompatibility with cell survival rate exceeding 80% after 72 h incubation. The SPUG hydrogels with superior mechanical properties, reversible gel-sol transitions, high self-healing capability, and good biocompatibility indicated promising prospects in biomedical applications.

Key words: Polyurethane hydrogel, Self-healing, Toughness, Disulfide bond, Hydrogen bond

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