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[1]. 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[2].

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.