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<p>A self-healing polyacrylate resin system was engineered via emulsion polymerization, integrating dynamic Cr<sup>3</sup>⁺-carboxylate/amine coordination bonds and quadruple hydrogen-bonding UPy motifs. This dual-network design significantly enhanced both mechanical properties and self-healing performance. Synthesis of the UPy-functional methacrylate monomer (UPy-MA) from 2-amino-4-hydroxy-6-methylpyrimidine and isocyanatoethyl methacrylate was confirmed by FT-IR and <sup>1</sup>H NMR spectroscopy. Subsequent polymerization yielded the target coordination polymer, with Cr<sup>3</sup>⁺-ligand coordination (–COOH/–NH) and UPy dimerization verified by FT-IR and UV–Vis spectroscopy. Compared with the single Cr<sup>3</sup>⁺ ion metal coordination system (Poly@Cr), the dual dynamic bond synergistic system (Poly@Cr-UPy) showed breakthrough performance improvements. Specifically, when the UPy-MA addition amount was 0.6 g, the tensile strength reached 11.61&#xa0;MPa, which was 2.8 times higher than that of Poly@Cr (4.1&#xa0;MPa). Cyclic tensile testing revealed non-overlapping hysteresis loops due to delayed bond reformation during continuous cycling. Remarkably, introducing 24-h inter-cycle recovery periods enabled complete bond reorganization and hysteresis loop closure. Moreover, after repairing at 40&#xa0;°C for 8&#xa0;h, the tensile strength achieved 85% recovery. Contact angle analysis of the membrane before and after repair confirms that localized abrasion damage was fully restored within 10&#xa0;min. This work establishes quantitative structure–property relationships in self-healing polymers, providing both experimental validation and a theoretical framework for designing supramolecular networks based on synergistic metal coordination and multivalent hydrogen bonding.</p>

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Synthesis and self-healing performance of polyacrylate resin based on synergistic effect of metal coordination bonds and hydrogen-bonding

  • 期刊论文

  • 发表日期：

    2026年3月24日

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  • Jiaman Dai,
  • Ting Hu,
  • Shuxin Liu,
  • Xue Li,
  • Wenxi Zheng,
  • Hualin Chen

摘要

A self-healing polyacrylate resin system was engineered via emulsion polymerization, integrating dynamic Cr3⁺-carboxylate/amine coordination bonds and quadruple hydrogen-bonding UPy motifs. This dual-network design significantly enhanced both mechanical properties and self-healing performance. Synthesis of the UPy-functional methacrylate monomer (UPy-MA) from 2-amino-4-hydroxy-6-methylpyrimidine and isocyanatoethyl methacrylate was confirmed by FT-IR and 1H NMR spectroscopy. Subsequent polymerization yielded the target coordination polymer, with Cr3⁺-ligand coordination (–COOH/–NH) and UPy dimerization verified by FT-IR and UV–Vis spectroscopy. Compared with the single Cr3⁺ ion metal coordination system (Poly@Cr), the dual dynamic bond synergistic system (Poly@Cr-UPy) showed breakthrough performance improvements. Specifically, when the UPy-MA addition amount was 0.6 g, the tensile strength reached 11.61 MPa, which was 2.8 times higher than that of Poly@Cr (4.1 MPa). Cyclic tensile testing revealed non-overlapping hysteresis loops due to delayed bond reformation during continuous cycling. Remarkably, introducing 24-h inter-cycle recovery periods enabled complete bond reorganization and hysteresis loop closure. Moreover, after repairing at 40 °C for 8 h, the tensile strength achieved 85% recovery. Contact angle analysis of the membrane before and after repair confirms that localized abrasion damage was fully restored within 10 min. This work establishes quantitative structure–property relationships in self-healing polymers, providing both experimental validation and a theoretical framework for designing supramolecular networks based on synergistic metal coordination and multivalent hydrogen bonding.