Interlocking Matrix and Filler for Enhanced Individualization and Reinforcement in Polymer–Single-Walled Carbon Nanotube Composites

Poor individualization and interfacial adhesion prevent single-walled carbon nanotube (SWNT)–polymer composites from reaching outstanding mechanical properties. With much larger diameters, but common structural features (high aspect ratio and absence of functional groups for covalent or supramolecular attachment with the polymer), carbon fibers face similar problems, which are addressed by covering the fibers with a thin layer of polymer. This sizing strategy has allowed carbon fibers to become the filler of choice for the highest performing materials. Inspired by this, here we investigate the use of the mechanical bond to wrap SWNTs with a layer of polymeric material to produce SWNTs mechanically interlocked with a layer of polymer. We first validate the formation of mechanically interlocked nanotubes (MINTs) using mixtures of SWNTs of relatively large average diameter (1.6 ± 0.4 nm), which are commercially available at reasonable prices and therefore could be technologically relevant as polymer fillers. We then design and synthesize by ring-opening metathesis polymerization (ROMP) a polymer decorated with multiple U-shaped molecules, which are later ring-closed around the SWNTs using metathesis. The obtained hybrids contain a high degree of individualized SWNTs and exhibit significantly increased mechanical properties when compared to the matrix polymer. We envision that this strategy could be employed to produce SWNTs interlocked with polymer layers with various designs for polymer reinforcement.