Abstract

Iron-based single-atom catalysts (SACs) are considered to the most promising catalysts to replace Pt for efficient oxygen reduction reaction (ORR). However, the precise synthesis of high-performance SACs and the understanding of their ORR origin remain challenging. In this work, microporous nitrogen-doped carbon with abundant and accessible atomically dispersed N-coordinated Fe sites (Fe-N-C) is prepared by molecular-confined coupling pyrolysis strategy. The Fe-N-C exhibits excellent ORR activities in acid (E1/2 of 0.78 V vs. RHE) and alkaline (E1/2 of 0.91 V vs. RHE) electrolytes. When integrated into a rechargeable aqueous Zinc-air battery (ZAB), both large specific capacity (770 mAh g−1) and high peak power density (240 mW cm−2) are achieved. Remarkably, the as-prepared ZAB presents amazing charge-discharge cycle performance of 1600 h at the large current density, which is 52.5 times of that using Pt/C+RuO2. Furthermore, all-solid-state ZAB delivers ultra-robust cycling stability even under bending. This work may advance a critical step towards the design of rational and controlled preparation of remarkable and ultra-stable catalysts.

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