All-Solid-State Mg-Air Battery Enhanced with Free-Standing N-Doped 3D Nanoporous Graphene

Nitrogen (N) doping of graphene with a three-dimensional (3D) porous structure, high flexibility, and low cost exhibits potential for developing metal-air batteries to power electric/electronic devices. The optimization of N-doping into graphene and the design of interconnected and monolithic graphene-based 3D porous structures are crucial for mass/ion diffusion and the final oxygen reduction reaction (ORR)/battery performance. Aqueous-type and all-solid-state primary Mg-air batteries using N-doped nanoporous graphene as air cathodes are assembled. N-doped nanoporous graphene with 50-150 nm pores and approximate to 99% porosity is found to exhibit a Pt-comparable ORR performance, along with satisfactory durability in both neutral and alkaline media. Remarkably, the all-solid-state battery exhibits a peak power density of 72.1 mW cm-2; this value is higher than that of a battery using Pt/carbon cathodes (54.3 mW cm-2) owing to the enhanced catalytic activity induced by N-doping and rapid air breathing in the 3D porous structure. Additionally, the all-solid-state battery demonstrates better performances than the aqueous-type battery owing to slow corrosion of the Mg anode by solid electrolytes. This study sheds light on the design of free-standing and catalytically active 3D nanoporous graphene that enhances the performance of both Mg-air batteries and various carbon-neutral-technologies using neutral electrolytes. All-solid-state primary Mg-air batteries designed using the free-standing N-doped nanoporous graphene cathode exhibit better discharge performances than the Pt-cathode-based aqueous-type and all-solid-state batteries. This is achieved by the sequential cooperation of N-doping and rapid air breathing in the 3D porous structures and slow corrosion of the Mg anode by solid electrolytes.image