Graphene-supported non-precious metal electrocatalysts for oxygen reduction reactions: the active center and catalytic mechanism

Abstract

In this work, non-precious metal catalysts (FeCoN) were loaded onto the surface of N-modified graphene (N-G), graphite and activated carbon during a simple yet effective chemical process. The oxygen reduction reaction (ORR) performance of the as-prepared catalysts with different pyrolysis temperatures were evaluated in 0.5 M H₂SO₄. The use of N-G at a pyrolysis temperature of 750 °C yielded the highest catalyst activity, while both the metal nitrides (MeN) and pyridinic N were demonstrated as the active center for the ORR. The pyridinic-N, which sits surrounding MeN works synergistically with metal nitrides to enhance the catalytic activity of the MeN/N-G composite. A maximum power density output of 130 mW cm⁻² at 0.25 V was achieved in a membrane electrode assembly (MEA) using FeCoN-N-G as a cathode catalyst. The mechanism of the ORR at the catalyst and the nature of the active center are discussed.