Enhancement of nitrogen self-doped nanocarbons electrocatalyst via tune-up solution plasma synthesis

The development of a metal-free carbon based electrocatalyst for the oxygen reduction reaction (ORR) is an essential issue for energy conversion systems. Herein, we suggest a tune-up solution plasma (SP) synthesis based on a simple one-step and cost-effective method to fabricate nitrogen self-doped graphitic carbon nanosheets (NGS) as an electrocatalyst. This novel strategy using a low-pass filter circuit provides plasma stability and energy control during discharge in pyridine, determining the graphitic structure of nanocarbons doped with nitrogen. Notably, NGS have a relatively high surface area (621 m² g^-1), and high contents of nitrogen bonded as pyridinic-N and pyrrolic-N of 55.5 and 21.3%, respectively. As an efficient metal-free electrocatalyst, NGS exhibit a high onset potential (-0.18 V vs. Ag/AgCl) and a 3.8 transferred electron pathway for ORR in alkaline solution, as well as better long-term durability (4% current decrease after 10 000 s of operation) than commercial Pt/C (22% current drop). From this point of view, the nitrogen self-doped graphitic carbon nanosheet material synthesized using the tune-up SP system is a promising catalyst for the ORR, as an alternative to a Pt catalyst for application in energy conversion devices.