Photothermal Conversion Triggered Precisely Targeted Healing of Epoxy Resin Based on Thermoreversible Diels–Alder Network and Amino-Functionalized Carbon Nanotubes

In the present work, we demonstrated the recyclability and precisely targeted reparability of amino functionalized multiwall carbon nanotubes-epoxy resin based on dynamic covalent Diels-Alder (DA) network (NH₂-MWCNTs/DA-epoxy) by exploring the photothermal conversion of CNTs to trigger the reactions of dynamic chemical bonds. The covalent cross-linked networks of NH₂-MWCNTs/DA-epoxy resin change their topology to linear polymer by thermally activated reverse Diels-Alder (r-DA) reactions at high temperatures, which endues the resin with almost 100% recyclability. The self-healing property of the epoxy resin was confirmed by the complete elimination of cracks after the reconstruction of DA network induced by heating or near-infrared (NIR) irradiation. For heat-triggered self-healing process, heat energy may also act on those uninjured parts of the resin and cause the dissociation of the whole DA network. Therefore, redundant r-DA and DA reactions, which have no contribution to self-healing, are also triggered during thermal treatment, resulting in not only a waste of energy but also the deformation of the sample under external force. Meanwhile, for the NIR-triggered self-healing process, the samples can maintain well their original shape without observable deformation after irradiation. The NIR-triggered healing process, which uses MWCNTs as the photothermal convertor, have very good regional controllability by simply tuning the MWCNTs content, the distance from NIR laser source to sample, and the laser power. The injured samples can be locally repaired with high precision and efficiency without an obvious influence on those uninjured parts.