Strong and Stiff Aramid Nanofiber/Carbon Nanotube Nanocomposites

Small but strong carbon nanotubes (CNTs) are fillers of choice for composite reinforcement owing to their extraordinary modulus and strength. However, the mechanical properties of the nanocomposites are still much below those for mechanical parameters of individual nanotubes. The gap between the expectation and experimental results arises not only from imperfect dispersion and poor load transfer but also from the unavailability of strong polymers that can be effectively utilized within the composites of nanotubes. Aramid nanofibers (ANFs) with analogous morphological features to nanotubes represent a potential choice to complement nanotubes given their intrinsic high mechanical performance and the dispersible nature, which enables solvent-based processing methods. In this work, we showed that composite films made from ANFs and multiwalled CNTs (MWCNTs) by vacuum-assisted flocculation and vacuum-assisted layer-by-layer assembly exhibited high ultimate strength of up to 383 MPa and Young's modulus (stiffness) of up to 35 GPa, which represent the highest values among all the reported random CNT nanocomposites. Detailed studies using different imaging and spectroscopic characterizations suggested that the multiple interfacial interactions between nanotubes and ANFs including hydrogen bonding and π–π stacking are likely the key parameters responsible for the observed mechanical improvement. Importantly, our studies further revealed the attractive thermomechanical characteristics of these nanocomposites with high thermal stability (up to 520 °C) and ultralow coefficients of thermal expansion (2–6 ppm·K–1). Our results indicated that ANFs are promising nanoscale building blocks for functional ultrastrong and stiff materials potentially extendable to nanocomposites based on other nanoscale fillers.