Enriched graphitic N in nitrogen-doped graphene as a superior metal-free electrocatalyst for the oxygen reduction reaction

Nitrogen-doped graphene (N-G) is considered as a promising catalyst for the oxygen reduction reaction (ORR). However, the contributions of pyridinic N, pyrrolic N and graphitic N in N-G for the ORR catalytic activity are controversial. In this work, the contents of pyridinic N, pyrrolic N and graphitic N in N-G were transformed by annealing at different temperatures. It is found that the total N content in N-G is not the critical factor to determine the ORR activity. An increase in the annealing temperature can enhance the content of graphitic N in N-G, causing an improved catalytic ORR activity, which confirms that graphitic N is the active component. Moreover, the enriched graphitic N in the N-G-1000 catalyst shows a half-wave potential (E1/2) of 0.862 V, 29 mV higher than that of the commercial Pt/C catalyst (0.833 V), which is one of the best reported for ORR metal-free catalysts.