Covalent cum noncovalent functionalizations of carbon nanotubes for effective reinforcement of a solution cast composite film

Although carbon nanotubes have impressive tensile properties, exploiting these properties in composites, especially those made by the common solution casting technique, seems to be elusive thus far. The reasons could be partly due to the poor nanotube dispersion and the weak nanotube/matrix interface. To solve this dual pronged problem, we combine noncovalent and covalent functionalizations of nanotubes in a single system by the design and application of a novel dispersant, hydroxyl polyimide-graft-bisphenol A diglyceryl acrylate (PI _OH-BDA), and use them with epoxidized single-walled carbon nanotubes (O-SWNTs). Our novel PI _OH-BDA dispersant functionalizes the nanotubes noncovalently to achieve good dispersion of the nanotubes because of the strong π-π interaction due to main chain and steric hindrance of the BDA side chain. PI _OH-BDA also functionalizes O-SWNTs covalently because it reacts with epoxide groups on the nanotubes, as well as the cyanate ester (CE) matrix used. The resulting solution-cast CE composites show 57%, 71%, and 124% increases in Young's modulus, tensile strength, and toughness over neat CE. These values are higher than those of composites reinforced with pristine SWNTs, epoxidized SWNTs, and pristine SWNTs dispersed with PI _OH-BDA. The modulus and strength increase per unit nanotube weight fraction, i.e., dE/dW _NT and dσ/dW _NT, are 175 GPa and 7220 MPa, respectively, which are significantly higher than those of other nanotube/thermosetting composites (22-70 GPa and 140-3540 MPa, respectively). Our study indicates that covalent cum noncovalent functionalization of nanotubes is an effective tool for improving both the nanotube dispersion and nanotube/matrix interfacial interaction, resulting in significantly improved mechanical reinforcement of the solution-cast composites.