Exfoliation Behavior of Large Anionic Graphite Flakes in Liquid Produced by Salt-Assisted Ball Milling

Functionalization of graphite is crucial for efficient and effective exfoliation to graphene. When negative charges are fixed to the edges of natural graphite, the resulting anionic graphite shows negative charging in a polar solvent. This enhanced negative charging is assumed to contribute the exfoliation of graphite during liquid-phase exfoliation (LPE). In this study, we prepared large anionic graphite flakes (~10 μm) by salt-assisted ball milling, as well as natural graphite flakes of the same size for comparison. During the LPE process, centrifugation speed and solvent type have dominant effects on graphene concentration and quality (e.g., size and thickness), so we investigated these factors for anionic graphite flakes in detail. The anionic graphite showed higher exfoliation efficiency in every type of solvent (isopropanol, methyl ethyl ketone, acetone, and water-based cosolvent) compared with the natural graphite. Monolayer graphene, with an average size of 80–200 nm, was obtained with relatively high yield (>10%) at only 3 min of sonication. The small size of graphene was due to edge fragmentation during the LPE process. The recyclability of the sediment and the characterization of the exfoliated powders for anionic graphene were also investigated.