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

Zn-air battery (ZAB) has distinguished itself as new generation of energy storage device due to the high theoretical energy density and its performance relies on the oxygen reduction reaction (ORR) performance of the cathode catalysts. Single atomic Fe anchored N-doped carbon (Fe-N-C) has emerged as a promising ORR electrocatalyst because of the maximum utilization of Fe atoms. However, to obtain high-rate and stable Fe-N-C remains challenging. A novel and facile approach to fabricate Fe-N-C catalyst (PC-Fe-50) with outstanding ORR performance superior to commercial platinum catalyst and iron phthalocyanine (FePc), is proposed here. When mixed with commercial OER catalyst (RuO2) and employed as the air cathode in ZAB, a high energy density of 809 W h kg-1, high power density of 128 mW cm-2, and stable cycling rechargeable performance are obtained. By means of density functional theory calculations, we revealed that the abundant N dopants (7.47 at%) in carbon play significant roles on FeNx moieties with two most common configurations (FeN4C10, denoted as D1; FeN4C12, denoted as D2). The binding energies of ORR intermediates on Fe center are adjusted. 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 combining the adjacent N atoms, instead of D1, the widely recognized active structure in reported Fe-N-C catalysts.