LAUSR

Abstract Graphene materials have recently experienced rapid developments, but large-scale production of high-quality graphene is still desired. Electrochemical exfoliation method is considered as a promising approach to meet this requirement. Here we demonstrate a non-electrified electrochemical exfoliation method to produce high-quality graphene (NEEG) sheets. By direct electrochemical reaction between graphite powders and metallic Li in 1 M LiPF6/propylene carbonate electrolyte, continuous graphite exfoliation is achieved with a high yield of excess 80% without any consumption of electric energy. The as-prepared NEEG has high quality with few defects (ID/IG = 0.45), a high C/O ratio of 27.74 and excellent electronic conductivity of 102.5 S cm−1. As conductive additives in Li4Ti5O12 electrode for lithium ion batteries, NEEG contributes to higher capacity and initial coulombic efficiency than common thermally reduced graphene oxide. Given the advantages of NEEG, the non-electrified electrochemical exfoliation method is promising for the large-scale preparation of high-quality graphene sheets.