N-doped hierarchically macro/mesoporous carbon with excellent electrocatalytic activity and durability for oxygen reduction reaction

Abstract A novel kind of N-doped hierarchically porous carbon materials (HPC-Ns) has been successfully synthesized with hierarchically macro/mesoporous silica as a hard template followed by a simple N-doping procedure using low-cost and nontoxic urea as the nitrogen source. The synthesized HPC-N samples demonstrated extensive three-dimensional (3D) connected macroporosity and partially ordered mesoporosity, extremely large specific surface area, favorable graphitization degree, and high relative content of pyridinic N, which is active to the oxygen reduction reaction (ORR). Due to the combined contributions of the above features, the metal-free HPC-Ns demonstrated excellent performance in ORR with a highly comparable limiting current density but much higher current output stability and resistance towards the fuel crossover effect compared to the commercial Pt/C, as well as the dominant 4 e^- reduction mechanism. Thus, it is believed that HPC-N has the potential to be used in polymer electrolyte membrane fuel cells.