CNT-Reinforced Self-Healable Epoxy Dynamic Networks Based on Disulfide Bond Exchange

[Image: see text] The design and utilization of polymers with healing capability have drawn increasing attention owing to their enhanced chain mobility and opportunity to heal minor cracks in composites. Rehealable thermoset polymers promise reduction in the maintenance cost and thus prolonged lifetime, reshaping, and recyclability. Introducing reversible covalent bonds is the mainstay strategy to achieve such plasticity in crosslinked polymers. Herein, we report a dynamic epoxy, which includes associative covalent adaptive networks (CANs) based on disulfide exchange bonds. Epoxy resin is chosen to study rehealing, as it is one of the most critical thermosetting polymers for various industries from aerospace to soft robotics. This study enlightens us about not only the consequences of CANs in the epoxy but also various factors such as soft segments and carbon nanotubes (CNTs). Epoxy dynamic networks are investigated in an attempt to explore the synergistic effect of the soft-segmented resins and CNTs on the healing and reshaping characteristics of epoxy networks along with varying stiffness. This research discusses epoxy dynamic networks in three main aspects: crosslink density, CAN density, and CNTs. Introducing soft segments into the epoxy network enhances the healing efficiency due to the increased chain mobility. A higher CAN density accelerates network rearrangement, improving the healing efficiency. It should also be noted that even with a low weight fraction of nanotubes, CNT-reinforced samples restored their initial strength more than neat samples after healing. The tensile strength of dynamic networks is at least 50 MPa, which is significant for their utility in primary or secondary structural components.