Synergistic Toughening of Graphene Films by Addition of Hydroxylated Carbon Nanotube

Graphene attracts great attention due to its excellent properties. However, the mechanical of assembled graphene-based film is usually inferior than its inherent mechanical properties. Herein, we construct a high-performance graphene-based film via vacuum filtration process by using graphene as matrix and hydroxylated Carbon Nanotube (CNT) as reinforcement agent. The synergistic interaction of hydrogen bonds between CNT and graphene Oxide (GO) and ionic bonds between Fe
²⁺
on CNT and GO significantly improve the mechanical properties of free-standing and flexible rGO/CNT film. Scanning Electron Microscopic (SEM) imaging and stress transfer mechanism analysis show that the introduction of CNT can hinder the slippage of GO sheets and promote the stress transfer under the continuous loading. The obtained rGO/CNT film shows high toughness of 3 MJ/m
³
, which is 3.6 times higher than that of GO sheets. This facile and scalable strategy can pave the way for the fabrication of high-performance graphene-based film in various applications.