High-Yield Production of Few-Layer Graphene via New-fashioned Strategy Combining Resonance Ball Milling and Hydrothermal Exfoliation

Graphene shows great potential applications in functional coating, electrodes, and ultrasensitive sensors, but high-yield and scalable preparation of few-layer graphene (FLG) by mechanical exfoliation method is still a formidable challenge. In this work, a novel two-step method for high-yield preparation of FLG is developed by combining resonance ball milling and hydrothermal treatment. During the resonance ball milling process, the utilization of magnetic Fe3O4 nanoparticles as a new “particle wedge” is beneficial to facilitate fragment and delamination of graphitic layers. In addition, further hydrothermal treatment can enhance ball milling product (BMP) exfoliation because of the shear force driven by the Brownian motion of various molecules at high temperature and high pressure. As expected, the two-step method can have high exfoliation efficiency up to 92% (≤10 layers). Moreover, the FLG nanosheet ink can easily achieve the formation of FLG coatings on the surface of various substrates, resulting in good electrical conductivity, which possesses potential applications in various fields including functional coating, energy storages, and electrochemical sensors, etc. Our work provides a new-fashioned strategy for mechanical large-scale production of graphene.