Ni₃Fe‐N Doped Carbon Sheets as a Bifunctional Electrocatalyst for Air Cathodes

A promising bifunctional electrocatalyst is reported for air cathodes consisting of Ni 3 Fe nanoparticles embedded in porous nitrogen‐doped carbon sheets (Ni 3 Fe/N‐C sheets) by a facile and effective pyrolysis‐based route with sodium chloride (NaCl) crystals as a template. The Ni 3 Fe/N‐C sheets show excellent catalytic activity, selectivity, and durability toward both the oxygen‐reduction and oxygen‐evolution reactions (ORR and OER). They are shown to provide a superior, low‐cost cathode for a rechargeable Zn‐air battery. At a discharge–charge current density of 10 mA cm −2 , the Ni 3 Fe/N‐C sheets enable a Zn–air battery to cycle steadily up to 420 h with only a small increase in the round‐trip overpotential, outperforming the more costly Pt/C + IrO 2 mixture catalyst (160 h). With the simplicity and scalability of the synthetic approach and its remarkable bifunctional electrocatalytic performance, the Ni 3 Fe/N‐C sheets offer a promising rechargeable air cathode operating at room temperature in an alkaline electrolyte.