Electrochemically Exfoliated Graphene Electrode for High-Performance Rechargeable Chloroaluminate and Dual-Ion Batteries

The current state-of-the-art positive electrode material for chloroaluminate ion batteries (AIBs) or dual-ion batteries (DIBs) is highly crystalline graphite; however, the rate capability of this material at high discharge currents is significantly reduced by the modest conductivity of graphite. This limitation is addressed through the use of graphene-based positive electrodes, which can improve the rate capability of these batteries due to their higher conductivity. However, conventional methods of graphene production induce a significant number of defects, which impair the performance of AIBs and DIBs. Herein, we report the use of a defect-free graphene positive electrode, which was produced using the electrochemical exfoliation of graphite in an aqueous solution with the aid of Co²⁺ as an antioxidant. The Co-treated graphene electrode achieved high capacities of 150 mAh g^-1 in DIBs and 130 mAh g^-1 in AIBs with high rate capability for both batteries. The charge-discharge mechanism of the batteries is examined using in situ Raman spectroscopy, and the results revealed that the intercalation density of [AlCl₄]^- or [PF₆]^- increased from a dilute staging index graphite intercalation compound (GIC) to a stage 1 GIC within the operating voltage window. The simple production method of high-quality graphene in conjunction with its high performance in DIBs should enable the use of graphene for DIB technologies.