Strategic Modulation of Target-Specific Isolated Fe,Co Single-Atom Active Sites for Oxygen Electrocatalysis Impacting High Power Zn–Air Battery

Abstract

An effective modulation of the active sites in a bifunctional electrocatalyst is essentially desired, and it is a challenge to outperform the state-of-the-art catalysts toward oxygen electrocatalysis. Herein, we report the development of a bifunctional electrocatalyst having target-specific Fe-N₄/C and Co-N₄/C isolated active sites, exhibiting a symbiotic effect on overall oxygen electrocatalysis performances. The dualism of N-dopants and binary metals lower the d-band centers of both Fe and Co in the Fe,Co,N-C catalyst, improving the overpotential of the overall electrocatalytic processes (Δ<i>E</i>_ORR-OER = 0.74 ± 0.02 V vs RHE). Finally, the Fe,Co,N-C showed a high areal power density of 198.4 mW cm^-2 and 158 mW cm^-2 in the respective liquid and solid-state Zn-air batteries (ZABs), demonstrating suitable candidature of the active material as air cathode material in ZABs.