A big step forward for composite application in the sector of structural materials is given by the use of Multi-Wall Carbon Nanotubes (MWCNTs) functionalized with hydrogen bonding moieties, such as barbiturate and thymine, to activate self-healing mechanisms and integrate additional functionalities. These materials with multiple healing properties at the same damaged site, imparted by hydrogen bonds, will also have the potential to improve material reliability, extend the service life, reduce replacement costs, and improve product safety. This revolutionary approach is obtained by integrating the non-covalent interactions coupled with the conventional covalent approach used to cross-link the polymer. The objective of this work is to characterize rubber-toughened supramolecular self-healing epoxy formulations based on unfunctionalized and functionalized MWCNTs using Tunneling Atomic Force Microscopy (TUNA). This advanced technique clearly shows the effect produced by the hydrogen bonding moieties acting as reversible healing elements by their simultaneous donor and acceptor character, and covalently linked to MWCNTs to originate self-healing nanocomposites. In particular, TUNA proved to be very effective for the morphology study of both the unfunctionalized and functionalized carbon nanotube-based conductive networks, thus providing useful insights aimed at understanding the influence of the intrinsic nature of the nanocharge on the final properties of the multifunctional composites.
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