Highly Conductive, Mechanically Strong Graphene Monolith Assembled by Three-dimensional Printing of Large Graphene Oxide

The manufacturing of three-dimensional (3D) graphene monolith with high mechanical and electrical performance has become an urgent issue in view of their potential applications in energy and electronics fields. Due to the structure rigidity and poor liquid-phase processing capability of graphene sheets, it is challenging to fabricate 3D graphene monolith with high mechanical performance, including strength, toughness and resiliency. Graphene oxide (GO) shows an improved dispersibility and reduction-restorable conductivity, which enables it to effectively balance the processing and comprehensive performances of graphene monolith. Here, we demonstrate a strategy to fabricate high-performance, shape-designable 3D graphene monolith through a 3D printing method based on large-sized graphene oxide (LGO) fluid ink. The concentration of the LGO ink for printing is as low as 20 mg/mL. The resulting monolith exhibits low density (12.8 mg/cm), high electrical conductivity (41.1 S/m), high specific strength (10.7 × 10 N·m/Kg) and compressibility (up to 80% compressive strain). Such a 3D printing technique enables plenty of complicated monolith structures and broadens the application range of graphene.