Rapid microwave-assisted bulk production of high-quality reduced graphene oxide for lithium ion batteries

Graphene-based advanced electrodes with improved electrochemical properties have received increasing attention for use in lithium ion batteries (LIBs). The conventional synthesis of graphene via liquid phase exfoliation or chemical reduction of graphene oxide (GO) approaches, however, either involves prolonged processing or leads to the retainment of high-concentration oxygen functional groups (OFGs). Herein, bulk synthesis of high-quality reduced graphene oxide using microwave irradiation (MWrGO) within few seconds is reported. The electromagnetic interaction of GO with microwaves is elucidated at molecular level using reactive molecular dynamic simulations. The simulation suggests that higher power microwave irradiation results in significantly less retainment of OFGs and the formation of structural voids. The synthesized MWrGO samples are thoroughly characterized in terms of structural evolution and physicochemical properties. Specifically, a modified ID/IG-in ratio metric for Raman spectrum, wherein the intensity contribution of D’ peak is deducted from the apparent G peak, is proposed to investigate the structural evolution of synthesized MWrGO, which yields a more reliable evaluation of structural disorder over traditional ID/IG ratio. Li-ion half-cell studies demonstrate that the MWrGO is an excellent candidate for usage as high capacity anode (750.0 mAh g-1 with near-zero capacity loss) and high-performance cathode (high capacity retention of ~70% for LiCoO2 at 10 C) for LIBs.