Boosting electrochemical performance of activated carbon by tuning effective pores and synergistic effects of active species.

Clean energy conversion/storage techniques have become increasingly significant because of the increasing energy consumption. Regarding practical applications like zinc-air batteries and supercapacitors, electrode materials are essential and often require both porous networks and active species to enhance their electrochemical performance. Nitrogen-doped porous carbon (NPC) is a kind of promising material, which provides efficient active sites and large surface areas for energy conversion/storage applications. However, rational modulation of properties for maximizing NPC performance is still a challenge. Herein, a promising NPC material derived from natural biomass is successfully synthesized by following a stepwise preparation method. Physisorption and X-ray photoelectron spectroscopy (XPS) analyses demonstrate both pore structures and nitrogen species of the NPC have been delicately tuned. The optimized sample NPC-800-m exhibits excellent performance in both oxygen reduction reaction (ORR) and three-electrode supercapacitor measurement. Moreover, the homemade zinc-air battery and symmetric supercapacitor assembled with NPC-800-m also display outstanding energy and power density as well as durable stability. Density functional theory (DFT) calculations further confirm the synergistic effects among graphitic, pyridinic and pyrrolic nitrogen. The existence of multispecies of nitrogen combined with the optimized pore structure is the key to the high electrochemical performance for NPC-800-m. This work not only provides feasible and green synthetic methodology but also offers original insights into the effective pores and the synergistic effects of different nitrogen species in the NPC materials.