FeNi Nanoparticles Coated on N‐doped Ultrathin Graphene‐like Nanosheets as Stable Bifunctional Catalyst for Zn‐Air Batteries

High‐performance and low‐cost bifunctional catalysts are crucial to energy conversion and storage devices. Herein, a novel oxygen electrode catalyst with high oxygen evolution reaction and oxygen reduction reaction (OER/ORR) performance is reported based on bimetal FeNi nanoparticles anchored on N‐doped graphene‐like carbon (FeNi/N−C). The complete 2D ultrathin carbon nanosheet is induced by etching and stripping of molten sodium chloride and its ions in the carbonization process at suitable temperature. The obtained FeNi/N−C catalyst exhibits rapid reaction kinetics for OER, efficient four electron transfer for ORR, and outstanding bifunctional performance with reversible oxygen electrode index of 0.87 V for OER/ORR. Zn‐air batteries with a high open‐circuit voltage of 1.46 V and a stable discharge voltage of 1.23 V are assembled using liquid electrolytes, zinc sheet as Zn‐electrode and FeNi/N−C coating on carbon cloth as air‐electrode. The specific capacity is as high as 816 mAh g −1 and there is extremely little decay after charge‐discharge cycle time of 275 h for the FeNi/N−C as oxygen electrode catalyst in Zn‐air battery, which are much better than that assembled with Pt/C−RuO 2 catalyst.