The emergence of graphene has attracted great attention in various applications. One is as a 2-D catalyst support due to its high specific surface area and conductivity. However, the agglomeration caused by interaction between individual layers makes graphene unsuitable for the dispersion of precious metal particles. Synthesis of a three-dimensional architecture to suppressing its aggregation and doping with heteroatoms to tailor the catalytic support properties of graphene is a critical challenge to secure the applicability of graphene as electrode material.

Herein, we report a cheap ion-exchange/activation combination method for large scale synthesis of the nitrogen-self-doped three-dimensional graphene-like networks (N-3D GNs) as catalyst support for fuel cell applications. In this process, the nitrogen-containing resin is exchanged with metal ions to catalyze the graphitization, followed by treatment in KOH/ethanol solution for pore-forming to increase the surface area of the materials. In the resulting N-3D GNs support, the novel structure provides multi-dimensional inter-connected pores that facilitate the diffusion of the reactants and by-products. The high specific surface area enables the preparation of highly dispersed metal particles and graphene-like structure, resulting in excellent electronic conductivity. While the doped nitrogen can change the growth behavior of the subsequently deposited catalyst particles, resulting in catalyst-support interactions to increase the activity and durability of Pt catalyst. As a catalyst for oxygen reduction reaction (ORR), the Pt nanoparticles supported on N-3D GNs gives more than double mass activity and almost no degradation in surface area after 5,000 cycles compared with commercial Pt/C catalyst. The enhanced performance in terms of mass activity and stability of the Pt/N-3D GNs compared with that of commercial Pt/C catalyst shows their potential applications in fuel cells.