High N-content holey few-layered graphene electrocatalysts: scalable solvent-less production

Abstract

Few layered nitrogen doped graphene (NG) attracts great interest in energy storage and conversion applications due to its electronic and catalytic properties. However, its bulk production cannot be envisioned by the current synthetic methods. Here we report a facile, solvent-less, low cost and high yield process for the synthesis of NG. Mechanochemical solid-state exfoliation allows scalable synthesis of holey and crumple nitrogen-doped few-layered graphene from graphite with controlled high concentration N doping and a high surface area through ball-milling. By adjusting the ratio of starting materials, the nitrogen content can be modulated from 4.87 to 17.83 at.%. Furthermore, the types of nitrogen-containing species in few-layered graphene can also be controlled. The resultant NG exhibits superior oxygen reduction reaction performance and more reliable stability than commercial Pt/C catalysts.