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<p>While valued for their mechanical properties, conventional polyurethane elastomers lack self-healing capabilities, leading to irreversible damage and limited-service life. To address this, in this study, we designed and synthesized a novel intrinsic self-healing polyurethane elastomer by integrating a dual dynamic network comprising multiple hydrogen bonds and nitrogen-coordinated boroxane rings. This system was constructed via the stepwise polycondensation of polytetrahydrofuranediol (PTMEG-2000), isophorone diisocyanate (IPDI), 4,4′-methylenebis(2-chloroaniline) (MOCA), 2-formylphenylboronic acid (FBA), and 2,6-pyridinediol (PDM). The resulting elastomer exhibited significant strain-induced strengthening and efficient autonomous healing at room temperature (25&#xa0;°C). Specifically, at an optimal PDM/MOCA molar ratio of 60/40 (PU<sub>HB-60/40</sub>), the material achieved a tensile strength of 18.8&#xa0;MPa with a healing efficiency of 94.7%, elongation at break of 2132% (91.7% recovery), and toughness of 117.0&#xa0;MJ/m<sup>3</sup> (86.7% recovery). The dynamic reversible bonds enabled repeated self-healing at the same fracture site. Furthermore, the material demonstrated excellent recyclability; where after dissolution and reprocessing, its mechanical properties remained largely intact. This study presented a viable molecular strategy for fabricating robust, self-healing, and recyclable elastomers that operate under ambient conditions, offering broad potential for sustainable material applications.</p>

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Preparation of room-temperature self-healing recyclable polyurethane elastomers based on a multiple hydrogen/nitrogen coordination boro-oxygen bonds system

  • 期刊论文

  • 发表日期：

    2026年3月10日

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  • Yuchen Jiao,
  • Ming Zhou,
  • Bo Pu,
  • Xiaoling Yang,
  • Chenyiting Li,
  • Liangliang Xia,
  • Guilin Deng,
  • Yunyao Wei,
  • Jing Zhong,
  • Zheng Wu,
  • Shi Chen,
  • Jian Wang,
  • Yujun Zhou

摘要

While valued for their mechanical properties, conventional polyurethane elastomers lack self-healing capabilities, leading to irreversible damage and limited-service life. To address this, in this study, we designed and synthesized a novel intrinsic self-healing polyurethane elastomer by integrating a dual dynamic network comprising multiple hydrogen bonds and nitrogen-coordinated boroxane rings. This system was constructed via the stepwise polycondensation of polytetrahydrofuranediol (PTMEG-2000), isophorone diisocyanate (IPDI), 4,4′-methylenebis(2-chloroaniline) (MOCA), 2-formylphenylboronic acid (FBA), and 2,6-pyridinediol (PDM). The resulting elastomer exhibited significant strain-induced strengthening and efficient autonomous healing at room temperature (25 °C). Specifically, at an optimal PDM/MOCA molar ratio of 60/40 (PUHB-60/40), the material achieved a tensile strength of 18.8 MPa with a healing efficiency of 94.7%, elongation at break of 2132% (91.7% recovery), and toughness of 117.0 MJ/m3 (86.7% recovery). The dynamic reversible bonds enabled repeated self-healing at the same fracture site. Furthermore, the material demonstrated excellent recyclability; where after dissolution and reprocessing, its mechanical properties remained largely intact. This study presented a viable molecular strategy for fabricating robust, self-healing, and recyclable elastomers that operate under ambient conditions, offering broad potential for sustainable material applications.