In this paper, catalyst-free room-temperature healing epoxy vitrimer-like materials (S-vitrimer) are introduced. The S-vitrimer can be healed at room temperature without any external stimuli such as solvent, pressure, heat, and catalyst through an aromatic disulfide exchange reaction and a hydrogen bond because the glass transition temperature of the S-vitrimer is lower than room temperature. Self-healing materials are attracting widespread attention nowadays with their potential to increase the durability of the materials. However, there is still elevating need for research, considering the limitations of various self-healing methods. To the best of our knowledge, epoxy-based catalyst-free room-temperature healing materials have not been investigated until now, yet they are promising to make self-healing easier. Moreover, the S-vitrimer showed higher healing efficiency when healed for a longer time and at a higher temperature. Especially when healed at room temperature for 96 h, the S-vitrimer presented an 80% healing efficiency. The S-vitrimer also showed an 80% healing efficiency when healed at 60 °C for 48 h. To investigate the factors affecting self-healing behavior, three control experiments were carried out. Control experiments showed that the S-vitrimer is healed mainly due to a disulfide exchange reaction, but hydrogen bonds also contribute to self-healing behavior. Also, it was found that tightly packed segments can hinder self-healing through control experiments.

Nowadays, self-healing materials have been studied actively in electronics, soft robotics, aerospace, and automobiles because they can prolong the life span of the materials. However, overcoming the trade-off relationship between mechanical properties and self-healing performance is challenging. Herein, graphene oxide-polyaniline (GO-PANI) filler was introduced to overcome this challenge because GO has a highly excellent modulus, and nitrogen atoms in PANI can endow a self-healing ability through hydrogen bonds. Aside from the hydrogen bond in PANI, the hydrogen bond in the carbonyl group and the disulfide exchange bond in the epoxy matrix also helped the materials heal efficiently. Therefore, the modulus of SV-GPN1 (Self-healing Vitrimer-GO-PANI1) reached 770 MPa, and a 65.0% healing efficiency was demonstrated. The modulus and self-healing efficiency were enhanced after adding GO-PANI filler. The self-healing ability, however, deteriorated when adding more GO-PANI filler because it hindered the collision between the molecules. Meanwhile, SV-GPN1 was excellent in reproducibility, which was proven by the experiment that 16.50 mm thick SV-GPN1 also displayed a self-healing ability. Thus, SV-GPN1 can be applied to structural materials in industries like aerospace because of its self-healing ability, excellent modulus, and reproducibility.

This study highlights the challenge of mechanoluminescence (ML) stress sensors losing ML intensity over time. Self-healing epoxy networks offer a promising strategy to restore light emission and enhance sensor sustainability.