A series of supramolecular comb polymers (SCPs) with adhesive and healable characteristics have been generated through the copolymerisation of methacrylate monomers featuring aromatic amide functionalities with lauryl methacrylate. By varying the amide functionality and loading of the supramolecular monomers, the properties of the resulting SCPs can be tailored, ultimately providing stable films at room temperature. As the loading of the amide-bearing monomer was increased, the phase separation between the hard and soft domains was enhanced, promoting larger hard-domain aggregation, as observed via atomic force microscopy (AFM). The mechanical properties of the SCPs correlated to the loading of the amide-bearing monomers, by increasing the mol% incorporation the resulting SCPs transition from possessing high strain to high ultimate tensile strength (UTS) and Young's modulus (YM). Over several re-adhesion cycles, the SCPs were shown to retain their shear strength when thermally adhered to both glass and aluminium substrates. Additionally, the SCPs exhibited healable properties at elevated temperatures (> 45 °C) allowing for the recovery of mechanical properties post-damage.
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