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An Iron‐Decorated Carbon Aerogel for Rechargeable Flow and Flexible Zn–Air Batteries

Mechanically stable and foldable air cathodes with exceptional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activities are key components of wearable metal–air batteries. Herein, a directional freeze‐casting and annealing approach is reported for the construction of a 3D honeycomb nanostructured, N,P‐doped carbon aerogel incorporating in situ grown FeP/Fe2O3 nanoparticles as the cathode in a flexible Zn–air battery (ZAB). The aqueous rechargeable Zn–air batteries assembled with this carbon aerogel exhibit a remarkable specific capacity of 648 mAh g−1 at a current density of 20 mA cm−2 with a good long‐term durability, outperforming those assembled with commercial Pt/C+RuO2 catalyst. Furthermore, such a foldable carbon aerogel with directional channels can serve as a freestanding air cathode for flexible solid‐state Zn–air batteries without the use of carbon paper/cloth and additives, giving a specific capacity of 676 mAh g−1 and an energy density of 517 Wh kg−1 at 5 mA cm−2 together with good cycling stability. This work offers a new strategy to design and synthesize highly effective bifunctional air cathodes to be applied in electrochemical energy devices.