Simultaneous Electrochemical Dual‐Electrode Exfoliation of Graphite toward Scalable Production of High‐Quality Graphene

Abstract Developing scalable methods to produce large quantities of high‐quality and solution‐processable graphene is essential to bridge the gap between laboratory study and commercial applications. Here an efficient electrochemical dual‐electrode exfoliation approach is developed, which combines simultaneous anodic and cathodic exfoliation of graphite. Newly designed sandwich‐structured graphite electrodes which are wrapped in a confined space with porous metal mesh serve as both electrodes, enabling a sufficient ionic intercalation. Mechanism studies reveal that the combination of electrochemical intercalation with subsequent thermal decomposition results in drastic expansion of graphite toward high‐efficiency production of graphene with high quality. By precisely controlling the intercalation chemistry, the two‐step approach leads to graphene with outstanding yields (85% and 48% for cathode and anode, respectively) comprising few‐layer graphene (1–3 layers, >70%), ultralow defects ( I D / I G < 0.08), and high production rate (exceeding 25 g h −1 ). Moreover, its excellent electrical conductivity (>3 × 10 4 S m −1 ) and great solution dispersibility in N ‐methyl pyrrolidone (10 mg mL −1 ) enable the fabrication of highly conductive (11 Ω sq −1 ) and flexible graphene films by inkjet printing. This simple and efficient exfoliation approach will facilitate the development of large‐scale production of high‐quality graphene and holds great promise for its wide application.