N‐Doped Carbon Nanotubes Derived from Graphene Oxide with Embedment of FeCo Nanoparticles as Bifunctional Air Electrode for Rechargeable Liquid and Flexible All‐Solid‐State Zinc–Air Batteries

Abstract This work reports a novel approach for the synthesis of FeCo alloy nanoparticles (NPs) embedded in the N,P‐codoped carbon coated nitrogen‐doped carbon nanotubes (NPC/FeCo@NCNTs). Specifically, the synthesis of NCNT is achieved by the calcination of graphene oxide‐coated polystyrene spheres with Fe3+, Co2+ and melamine adsorbed, during which graphene oxide is transformed into carbon nanotubes and simultaneously nitrogen is doped into the graphitic structure. The NPC/FeCo@NCNT is demonstrated to be an efficient and durable bifunctional catalyst for oxygen evolution (OER) and oxygen reduction reaction (ORR). It only needs an overpotential of 339.5 mV to deliver 10 mA cm−2 for OER and an onset potential of 0.92 V to drive ORR. Its bifunctional catalytic activities outperform those of the composite catalyst Pt/C + RuO2 and most bifunctional catalysts reported. The experimental results and density functional theory calculations have demonstrated that the interplay between FeCo NPs and NCNT and the presence of N,P‐codoped carbon structure play important roles in increasing the catalytic activities of the NPC/FeCo@NCNT. More impressively, the NPC/FeCo@NCNT can be used as the air‐electrode catalyst, improving the performance of rechargeable liquid and flexible all‐solid‐state zinc–air batteries.