Epoxy Vitrimer with Excellent Mechanical Properties and High T g for Detachable Structural Adhesives

作者：Anping Dong, Qiguang Liu, Huarui Yao, Jiahao Ma, Jue Cheng, Junying Zhang · 发表于：ACS Applied Materials & Interfaces · 年份：2025 · DOI：10.1021/acsami.4c22337 · 被引用次数：27 · 研究领域：Polymer composites and self-healing、Synthesis and properties of polymers、Silicone and Siloxane Chemistry

It is a long-standing challenge for thermoset resins to simultaneously achieve outstanding thermomechanical and mechanical properties as well as rapid network reconfiguration due to the trade-off between chemical bond transformation and stability of the network. The design of the vitrimer network topology is an effective strategy to address the above issues. Here, we prepared an epoxy vitrimer material (DGEBA–API–MHHPA) with excellent mechanical properties and high glass-transition temperature ( T g ) by introducing rigid-flexible integrated side chains [1-(3-aminopropyl) imidazole (API)], which endow DGEBA–API–MHHPA multiple interactions including “internal antiplasticization” effect, intermolecular hydrogen bonds, and π–π interactions. Moreover, the introduction of Zn 2+ facilitates transesterification, enabling the fast rearrangement of the network. Specifically, the relaxation time of DGEBA–API 0.2 –MHHPA 0.8 –Zn reaches 65 s at 200 °C. Meanwhile, Zn 2+ –imidazole coordination bonds with energy dissipation improve the toughness of the vitrimer network. The resulting DGEBA–API 0.2 –MHHPA 0.8 –Zn exhibits self-healing and recyclable behaviors and possesses 80.3 MPa of tensile strength, 3.25 GPa of Young’s modulus, 7.2 MPa·m 1/2 of fracture toughness ( K IC ), and T g of 129 °C. Concurrently, DGEBA–API 0.2 –MHHPA 0.8 –Zn can be applied as detachable structural adhesives for various substrates and can be used as matrixes of recyclable and electrically self-healing composites....