Novel Heteroatom-Doped Fe/N/C Electrocatalysts With Superior Activities for Oxygen Reduction Reaction in Both Acid and Alkaline Solutions.

The exploration of noble metal-free catalysts with efficient electrochemical performance toward oxygen reduction reaction in the acid electrolyte is very important for the development of fuel cells technology. Novel pyrolyzed heteroatom-doped Fe/N/C catalysts have been regarded as the most efficient electrocatalytic materials for ORR due to their tunable electronic structure, and distinctive chemical and physical properties. Herein, nitrogen- and sulfur-doped (Fe/N/C and Fe/N/C-S) electrocatalysts were synthesized using ferric chloride hexahydrate as the Fe precursor, N-rich polymer as N precursor, and Ketjen Black EC-600 (KJ600) as the carbon supports. Among these electrocatalysts, the as prepared S and N-doped Fe/N/C-S reveals the paramount ORR activity with a positive half-wave potential value ( ) 0.82 at 0.80 V vs. RHE in 0.1 mol/L HSO solution, which is comparable to the commercial Pt/C (Pt 20 wt%) electrocatalyst. The mass activity of the Fe/N/C-S catalyst can reach 45% (12.7 A g at 0.8 V) and 70% (5.3 A g at 0.95 V) of the Pt/C electrocatalyst in acidic and alkaline solutions. As result, ORR activity of PGM-free electrocatalysts measured by the rotating-ring disk electrode method increases in the following order: Fe/N/C<Fe/N/C-S, in both basic and acidic medium. This scientific work offers a facile approach to design and synthesizes efficient heteroatom-doped catalytic materials for electrochemical reactions in energy devices.