Spontaneous intercalation of long-chain alkyl ammonium into edge-selectively oxidized graphite to efficiently produce high-quality graphene

Mass production of high-quality graphene nanosheets (GNs) is essential for practical applications. We report that oxidation of graphite by low concentration KMnO₄ at relatively high temperature (60 °C) leads to edge-selectively oxidized graphite (EOG) which preserves the high crystalline graphitic structure on its basal planes while the edges are functionalized by oxygen-containing groups. Long-chain tetradecyl-ammonium salt (C₁₄N⁺) could be spontaneously intercalated into EOG to form intercalated EOG-C₁₄N⁺ compounds. Gentle and short-time sonication of EOG-C₁₄N⁺ in toluene can full exfoliate EOG into edge-oxidized graphene nanosheets (EOGNs) with concentration of 0.67 mg/ml, monolayer population up to 90% and lateral size from 1 μm to >100 μm. The EOG and EOGN films show excellent electrical conductance, which is far superior to their graphene oxide (GO) counterparts. Our method provides an efficient way to produce high-quality GNs, and the resultant EOG also can be directly used for production of multifunctional materials and devices.