Supercritical carbon dioxide-assisted silanization of multi-walled carbon nanotubes and their effect on the thermo-mechanical properties of epoxy nanocomposites

- Supercritical carbon dioxide was used as the solvent for silanizing MWCNTs.
- Epoxy composites were prepared with pristine and silanized MWCNTs.
- Pristine MWCNTs had little effect on the resin properties.
- Silanized MWCNTs enhanced the thermo-mechanical properties of the resin.
- Loading levels ∼0.2 wt% engendered the greatest property enhancements.

Supercritical carbon dioxide was employed as the solvent for the functionalization of multi-walled carbon nanotubes (MWCNTs) with an epoxy-capped silane. The silanization protocol was found to be a suitable green alternative to traditional routes that rely on organic solvents for grafting nearly monolayers of silane molecules onto the nanotube surfaces. The addition of silanized MWCNTs to a model epoxy markedly increased its Tg, and measurements of the network cooperativity length scale linked this change to a reduction in polymer segment mobility. Composites filled with low loading levels of both pristine and silanized MWCNTs exhibited significantly higher strain at break and toughness than the neat epoxy, and the greatest improvements were observed at low loading levels. SEM analysis of the composite fracture surfaces revealed that nanotube pullout was the primary failure mechanism in epoxy loaded with pristine MWCNTs while crack bridging predominated in composites containing silanized MWCNTs as the result of strong interfacial bonding with the matrix. The elevated Tg and toughness achieved with small additions of silanized MWCNTs promise to extend the engineering applications of the epoxy resin.

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