Atomically Dispersed Fe-Co Dual Metal Sites as Bifunctional Oxygen Electrocatalysts for Rechargeable and Flexible Zn-Air Batteries

Single-metal site catalysts have exhibited highly efficient electrocatalytic properties due to their unique coordination environments and adjustable local structures for reactant adsorption and electron transfer. They have been widely studied for many electrochemical reactions, including oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). However, it remains a significant challenge to realize high-efficiency bifunctional catalysis (ORR/OER) with single-metal-type active sites. Herein, we report atomically dispersed Fe-Co dual metal sites (FeCo-NC) derived from Fe and Co codoped zeolitic imidazolate frameworks (ZIF-8s), aiming to build up multiple active sites for bifunctional ORR/OER catalysts. The atomically dispersed FeCo-NC catalyst shows excellent bifunctional catalytic activity in alkaline media for the ORR (E-1/2 = 0.877 V) and the OER (E-j=10 = 1.579 V). Moreover, its outstanding stability during the ORR and the OER is comparable to noblemetal catalysts (Pt/C and RuO2). The atomic dispersion state, coordination structure, and the charge density difference of the dual metal site FeCo-NC were characterized and determined using advanced physical characterization and density functional theory (DFT) calculations. The FeCo-N-6 moieties are likely the main active sites simultaneously for the ORR and the OER with improved performance relative to the traditional single Fe and Co site catalysts. We further incorporated the FeCo-NC catalyst into an air electrode for fabricating rechargeable and flexible Zn-air batteries, generating a superior power density (372 mW cm(-2)) and long-cycle (over 190 h) stability. This work would provide a method to design and synthesize atomically dispersed multi-metal site catalysts for advanced electrocatalysis.

Automated summary

This study presents atomically dispersed Fe-Co dual metal sites derived from Fe and Co codoped zeolitic imidazolate frameworks, showing excellent bifunctional catalytic activity for ORR and OER in alkaline media. The FeCo-NC catalyst exhibits outstanding stability and is integrated into an air electrode for fabricating rechargeable and flexible Zn-air batteries, achieving a high power density and long-cycle stability. This work offers a method to design and synthesize atomically dispersed multi-metal site catalysts for advanced electrocatalysis.