Hierarchical Micron-Sized Mesoporous/Macroporous Graphene with Well-Tuned Surface Oxygen Chemistry for High Capacity and Cycling Stability Li–O₂ Battery

Nonaqueous Li–O2 battery is recognized as one of the most promising energy storage devices for electric vehicles due to its super-high energy density. At present, carbon or catalyst-supporting carbon materials are widely used for cathode materials of Li–O2 battery. However, the unique electrode reaction and complex side reactions lead to numerous hurdles that have to be overcome. The pore blocking caused by the solid products and the byproducts generated from the side reactions severely limit the capacity performance and cycling stability. Thus, there is a great need to develop carbon materials with optimized pore structure and tunable surface chemistry to meet the special requirement of Li–O2 battery. Here, we propose a strategy of vacuum-promoted thermal expansion to fabricate one micron-sized graphene matrix with a hierarchical meso-/macroporous structure, combining with a following deoxygenation treatment to adjust the surface chemistry by reducing the amount of oxygen and selectively removing partial unstable groups. The as-made graphene demonstrates dramatically tailored pore characteristics and a well-tuned surface chemical environment. When applied in Li–O2 battery as cathode, it exhibits an outstanding capacity up to 19 800 mA h g–1 and is capable of enduring over 50 cycles with a curtaining capacity of 1000 mA h g–1 at a current density of 1000 mA g–1. This will provide a novel pathway for the design of cathodes for Li–O2 battery.