Nacre Inspired Supertough and Flame-Retardant Reduced Graphene Oxide Composite Films

Nacre-like graphene composite films (GCFs) with high strength have been highly developed. However, the GCFs usually exhibit relatively poor toughness and poor flame resistance, seriously limiting their applications as structural materials. Here, reduced graphene oxide (rGO), halloysite nanotubes (HNTs), and flame-retarding modified lignin (F-lignin) were compounded to fabricate the rGO-HNTs-(F-lignin) film. In the rGO-HNTs-(Flignin) film, the F-lignin binds the rGO sheets and HNTs, enhancing the entanglement of HNTs and the interactions between HNTs and rGO sheets, and the macromolecular F-lignin also improves the ductility of the rGO-HNTs-(F-lignin) film, while the entangled HNTs conversely reinforce the F-lignin to prevent the F-lignin from fracture when the rGO-HNTs-(F-lignin) film is under stress, further increasing the ductility of the rGOHNTs-(F-lignin) film. The HNTs and F-lignin promote each other to enhance the strengthening and toughening effect on the rGO-HNTs-(F-lignin)-film, and endowing the rGO-HNTs-(F-lignin)-film with the superior mechanical properties of the tensile strength of 634 +/- 38 MPa, tensile fracture strain of 8.17 +/- 0.59 %, and toughness of 25.35 +/- 2.95 MJ/m3, respectively. The rGO-HNTs-(F-lignin) film also exhibits improved flameretardant properties due to the high flame retardancy of HNTs and F-lignin. These excellent integrated properties of the rGO-HNTs-(F-lignin) film will promote its potential applications as structural materials.