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Zn-air battery (ZAB) has distinguished itself as new generation of energystorage device due to the high theoretical energy density and its performancerelies on the oxygen reduction reaction (ORR) performance of the cathodecatalysts. Single atomic Fe anchored N-doped carbon (Fe-N-C) has emerged as apromising ORR electrocatalyst because of the maximum utilization of Fe atoms.However, to obtain high-rate and stable Fe-N-C remains challenging. A novel andfacile approach to fabricate Fe-N-C catalyst (PC-Fe-50) with outstanding ORRperformance superior to commercial platinum catalyst and iron phthalocyanine(FePc), is proposed here. When mixed with commercial OER catalyst (RuO2) andemployed as the air cathode in ZAB, a high energy density of 809 W h kg-1, highpower density of 128 mW cm-2, and stable cycling rechargeable performance areobtained. By means of density functional theory calculations, we revealed thatthe abundant N dopants (7.47 at%) in carbon play significant roles on FeNxmoieties with two most common configurations (FeN4C10, denoted as D1; FeN4C12,denoted as D2). The binding energies of ORR intermediates on Fe center areadjusted. By comparing the activity of possible structures and FePc molecule,we find the realistic active sites in PC-Fe-50 catalyst may be the D2 combiningthe adjacent N atoms, instead of D1, the widely recognized active structure inreported Fe-N-C catalysts.

Single Atomic Fe anchored Porous Carbon with Rich Graphitic Nitrogen as Electrocatalysts for Oxygen Reduction Reaction and Zn-Air Batteries