Synthesis of graphene materials by electrochemical exfoliation: Recent progress and future potential

Abstract Synthesis of structurally controlled graphene materials is critical for realizing their practical applications. The electrochemical exfoliation of graphite has emerged as a simple method to produce graphene materials. This review examines research progress in the last 5 years, from 2015 to 2019. Graphene material synthesis methods generally have a trade‐off between increasing production yield and achieving better material property control. The synthesis conditions for synthesizing pristine graphene, graphene oxide (GO), and graphene composites are significantly different. Thus, in this review, we first discuss synthesis methods for graphene materials with high C/O ratios from four aspects: graphite electrodes, equipment engineering, electrolytes, and additional reduction methods. Next, we survey synthesis methods for GO and examine how the pretreatment of the graphite electrodes, electrolytes, and operation parameters, such as applied voltages, electrolyte temperatures, and mechanical forces, affect the quality of GO. Further, we summarize electrochemical exfoliation methods used to dope graphene materials, introduce covalent functional groups, incorporate various nanoparticles, and assembly of graphene architectures. For all synthesis methods, we compare the properties of resulting graphene materials such as C/O ratios, lateral size, layer numbers, and quality characterized by Raman spectroscopy. Lastly, we propose our perspectives on further research. We hope this review stimulates more studies to realize the on‐demand production of graphene materials with desired properties using electrochemical exfoliation methods.