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

ACS Nano. 2022 May 24;16(5):7890-7903. doi: 10.1021/acsnano.2c00547. Epub 2022 Apr 18.

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 (ΔEORR-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.

Keywords: Zn−air battery; bifunctional O2 electrocatalysis; d-band center; metal−organic framework; single atom catalyst.