Synergistic toughening of polymer nanocomposites by hydrogen-bond assisted three-dimensional network of functionalized graphene oxide and carbon nanotubes

We report a facile method to enhance mechanical properties of polymer nanocomposites using three-dimensional (3D) network structures of functionalized graphene oxide (GO) and multi-walled carbon nanotubes (MWCNTs) in a polymer matrix. The GO and MWCNTs were functionalized using Fisher indole and diazonium-salt reactions to produce pyridine (Py) moiety on the GO and MWCNTs. The functionalized GO (Py-RGO) and MWCNT (Py-MWCNT) nanocomposites exhibited hydrogen-bond assisted 3D network structures in a polyimide (PI) matrix. By incorporating 1 wt% of carbon materials (0.9 wt% Py-RGO and 0.1 wt% Py-MWCNTs) in a PI, the tensile strength and modulus of the ternary nanocomposites reached 581 MPa and 31 GPa, respectively, which was an enhancement of 221% and 312% compared with pristine PI. The fracture energy of the PI/Py-RGO/Py-MWCNT nanocomposites improved 200% and approached 29.7 MJ m⁻³. The formation of the 3D network structure of the functionalized carbon nanomaterials is considered to significantly affect load transfer of nanofillers in the polymer matrix, and produce high performance polymer nanocomposites.