A Spinel (FeNiCrMnMgAl)3O4 High Entropy Oxide as a Cycling Stable Anode Material for Li-Ion Batteries

Abstract

Recently, high entropy oxides (HEO) with special stabilization effects have been widely investigated as new anode materials for lithium-ion batteries. However, the lithium storage mechanism of HEO is still under debate. In this work, we applied a modified solution combustion synthesis method with a subsequent ball milling refinement process to prepare a six-component (FeNiCrMnMgAl)3O4 spinel high entropy oxide (6-SHEO). The novel 6-SHEO anode features outstanding electrochemical performance, enabling a stable capacity of 657 mAh g−1 at a current rate of 0.2 A g−1 after 200 cycles, and good high-rate capability with 350 mAh g−1 even at 4 A g−1. In addition, the lithium storage behavior of this 6-SHEO anode was explored in detail through in-situ XRD and ex-situ TEM approaches. Surprisingly, a reversible spinel to rock salt phase transition behavior and spinel phase residue phenomenon was firstly observed by this route. Furthermore, for better understanding of the phase change behavior in this 6-SHEO anode, a high-energy ball milling approach was applied to induce a similar spinel to rock salt phase transformation for the first time, which generates fresh insight into the mechanism of the phase change behavior in this 6-SHEO anode.