Dual‐Strategy of Cation‐Doping and Nanoengineering Enables Fast and Stable Sodium‐Ion Storage in a Novel Fe/Mn‐Based Layered Oxide Cathode

Abstract

Abstract Iron/manganese‐based layered transition metal oxides have risen to prominence as prospective cathodes for sodium‐ion batteries (SIBs) owing to their abundant resources and high theoretical specific capacities, yet they still suffer from rapid capacity fading. Herein, a dual‐strategy is developed to boost the Na‐storage performance of the Fe/Mn‐based layered oxide cathode by copper (Cu) doping and nanoengineering. The P2‐Na0.76Cu0.22Fe0.30Mn0.48O2 cathode material synthesized by electrospinning exhibits the pearl necklace‐like hierarchical nanostructures assembled by nanograins with sizes of 50–150 nm. The synergistic effects of Cu doping and nanotechnology enable high Na+ coefficients and low ionic migration energy barrier, as well as highly reversible structure evolution and Cu/Fe/Mn valence variation upon repeated sodium insertion/extraction; thus, the P2‐Na0.76Cu0.22Fe0.30Mn0.48O2 nano‐necklaces yield fabulous rate capability (125.4 mA h g−1 at 0.1 C with 56.5 mA h g−1 at 20 C) and excellent cyclic stability (≈79% capacity retention after 300 cycles). Additionally, a promising energy density of 177.4 Wh kg−1 is demonstrated in a prototype soft‐package Na‐ion full battery constructed by the tailored nano‐necklaces cathode and hard carbon anode. This work symbolizes a step forward in the development of Fe/Mn‐based layered oxides as high‐performance cathodes for SIBs.

Keywords

• electrospinning
• Fe/Mn‐based layered oxide cathodes
• nanoengineering
• nanostructures
• reaction mechanisms
• sodium‐ion batteries