Phosphorization‐Induced Void‐Containing Fe₃O₄ Nanoparticles Enabling Low Lithiation/Delithiation Potential for High‐Performance Lithium‐Ion Batteries

Abstract

In terms of Fe 3 O 4 -based anodes, enormous academic progress has been achieved over the past two decades; however, even with excellent half-cell performance, the relatively high lithiation potential and unsatisfactory initial coulombic efficiency (ICE) represent two major barriers to their commercial application, at present. We propose partially phosphorized Fe 3 O 4 (PÀ Fe 3 O 4 ) with interior void spaces induced by phosphorization to enhance the Li + storage property of Fe 3 O 4 -based anodes. PÀ Fe 3 O 4 anodes offer a much higher capacity at low potential compared with bare Fe 3 O 4 electrodes. Additionally, the welldesigned nanostructure with preferable specific surface area prevents the initial irreversible lithium loss, which contributes to a brilliant ICE (80.8 % at 100 mA g À 1 ). Moreover, in-situ X-ray diffraction proves that the formation of the Li x Fe 3 O 4 phase results from an initial intercalation process. In particular, the output voltage and energy density of PÀ Fe 3 O 4 full-cells are much greater than those of Fe 3 O 4 full-cells. In this work, the PÀ Fe 3 O 4 full-cell exhibits a capacity of 680 mAh g À 1 at 200 mA g À 1 as well as an excellent rate capability of 267 mAh g À 1 with a current density up to 1000 mA g À 1 . This study presents a new strategy to enhance Li + storage of Fe 3 O 4 enabling low lithiation/delithiation potential and high ICE, which may offer exciting opportunities toward designing highperformance full-cells with commercial cathodes.

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