Platinum-Coated Hollow Graphene Nanocages as Cathode Used in Lithium-Oxygen Batteries

One of the formidable challenges facing aprotic lithium-oxygen (Li-O₂) batteries is the high charge overpotential, which induces the formation of byproducts, loss in efficiency, and poor cycling performance. Herein, the synthesis of the ultrasmall Pt-coated hollow graphene nanocages as cathode in Li-O₂ batteries is reported. The charge voltage plateau can reduce to 3.2 V at the current density of 100 mA g⁻¹, even maintain below 3.5 V when the current density increased to 500 mA g⁻¹. The unique hollow graphene nanocages matrix can not only provide numerous nanoscale tri-phase regions as active sites for efficient oxygen reduction, but also offer sufficient amount of mesoscale pores for rapid oxygen diffusion. Furthermore, with strong atomic-level oxygen absorption into its subsurface, ultrasmall Pt catalytically serves as the nucleation site for Li₂O₂ growth. The Li₂O₂ is subsequently induced into a favorable form with small size and amorphous state, decomposed more easily during recharge. Meanwhile, the conductive hollow graphene substrate can enhance the catalytic activity of noble metal Pt catalysts due to the graphene-metal interfacial interaction. Benefiting from the above synergistic effects between the hollow graphene nanocages and the nanosized Pt catalysts, the ultrasmall Pt-decorated graphene nanocage cathode exhibits enhanced electrochemical performances.