Abstract

Developing iron-based single-atom catalysts (Fe SACs) with low cost, high activity and stability is vital for commercialising sustainable energy technologies. However, accurately controlling and identifying structure–activity relationships of Fe SACs remains a significant challenge. Herein, we report Fe/N co-doped carbon nanofiber membranes with highly exposed Fe-N4 sites (Fe/NCNFs), synthesized by electrospinning and pyrolysis. The three-dimensional (3D) hierarchical structure and atomically dispersed pyrrole-type Fe (III)-N4 active sites provide the as-prepared catalyst with a positive half-wave potential of 0.87 V and an ultralow Tafel slope of 53 mV dec−1. As an air cathode catalyst for liquid Zn − air batteries, it delivers a high open-circuit voltage (1.474 V), a large peak power density (190 mW cm−2) and a high durability of 2000 cycles at 5 mA cm−2. As a self-standing air cathode, the as-assembled solid-state Zn − air batteries also show stable cycling with a small discharge/charge voltage gap of 0.65 V, indicating great prospects for developing portable zinc − air batteries.

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