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Preparation of multi-function graphene materials through electrode-distance controlled electrochemical exfoliation

Preparation of graphene materials with different microstructures is of great significance for the specific applications in various areas. Here, a modified electrochemical exfoliation method with controlled electrode distance is proposed to prepare exfoliated graphene, graphene quantum dots, and graphene oxide (EGr, EGQD, and EGO). Compared with electrolysis at a fixed location, the modified electrode distance can effectively tune the insertion speed and direction, as well as the kinetic rates of exfoliation processes. Specifically, at a short electrode distance of 3 cm, it produced high-quality EGr with the size above 5 μm and thickness below 5 layers; when the electrode distance increased to 30 cm, EGQD with the size below 5 nm was produced. Further, the distance between 3 and 30 cm facilitates producing EGO with ca. 15% O content. In addition, it is found that the reaction temperature, optimized electrolyte, and controlled potential can further optimize the exfoliation processes, which can achieve a high exfoliation rate of ca. 2000, 140, and 1500 g h−1 for EGr, EGQD, and EGO preparation in an industrial-scale system, respectively. These modified graphene materials can be directly applied in various areas. For example, EGr can act as an effective component to increase one order of the dielectric property of PVDF; EGQD can effectively generate a PL spectrum at ca. 550 nm; EGO can facilely form a conductive and flexible film through self-assembly.