▎ 摘　　要

The field of Al batteries immensely demands the development of highly efficient cathode materials which can provide large storage capacities along with maintaining a constant high voltage. In this work, using the first-principles calculations, we have proposed the graphene/hexagonal boron nitride heterostructure (G/hBN) as a suitable cathode material for Al batteries. We have systematically investigated the binding, electronic, and electrochemical properties for the AlCl4-adsorbed/intercalated G/hBN heterostructure in various possibilities, and a necessary comparison has also been executed with the pristine monolayer of graphene and hBN. It is observed that the binding strength of AlCl4 has significantly improved on the outer surfaces of graphene and hBN and in interlayer spaces of the G/hBN heterostructure compared to monolayer hBN, besides maintaining a similar strong binding as that of monolayer graphene. The lower diffusion barrier (0.01 eV) ensures a faster charge/discharge rate in the G/hBN heterostructure as the Al battery cathode. On systematically observing the incorporation of AlCl4 in G/hBN through the voltage profile study, it is determined that the G/hBN heterostructure can deliver both a high voltage of 2.14 V as well as a high storage capacity of 183 mA h/g, whereas monolayers of graphene and hBN are either good at delivering higher storage capacity or better net voltage. All of these results motivate us toward the usage of the G/hBN heterostructure as the potential cathode material for the Al battery and provide valuable insights into the exploration of other 2D heterostructures for the highly efficient Al batteries.