Ultratough reduced graphene oxide composite films synergistically toughened and reinforced by polydopamine wrapped carbon nanotubes

Nacre like graphene based composite films (GCFs) have been developed over the last decade. Although the progress in ultrastrong GCFs is remarkable, fabricating GCFs with excellent integrated properties of strength, flexibility, and toughness still remains a challenge. Here, a ternary GCF of reduced graphene oxide (rGO), polydopamine (PDA) and multi-walled carbon nanotubes (MWCNTs) was developed. The MWCNTs were modified by PDA to form PDA@MWCNTs which were then compounded with GO to fabricate the rGO-PDA@MWCNT films by evaporation-induced assembly and chemical reduction. The preparation was simple, cheap and environmentally-friendly. The PDA increased the dispersion of MWCNTs in the rGO-PDA@MWCNT films, crosslinked the rGO sheets, and enhanced the entanglement of MWCNTs and the interactions between MWCNTs and rGO sheets. Benefiting from the synergistic effect of PDA and MWCNTs, the rGO-PDA@MWCNT films exhibited excellent integrated properties by increasing strength, tensile fracture strain and toughness to 579 ± 35 MPa, 12.03 ± 0.56%, and 34.03 ± 1.60 MJ/m 3 , which were 2.26, 2.02 and 4.94 times that of pure rGO films, respectively. The rGO-PDA@MWCNT films also exhibited a high conductivity of 612 ± 68 S/cm and excellent structural stability under extreme environments. These excellent integrated properties of the rGO-PDA@MWCNT films will promote their applications in aerospace engineering, flexible electrical devices and artificial muscle.