Utilizing High-Capacity Spinel-Structured High-Entropy Oxide (CrMnFeCoCu)3O4 as a Graphite Alternative in Lithium-Ion Batteries

Abstract

In the realm of advanced anode materials for lithium-ion batteries, this study explores the electrochemical performance of a high-entropy oxide (HEO) with a unique spinel structure. The equiatomic composition of CrMnFeCoCu was synthesized and subjected to a comprehensive materials characterization process, including X-ray diffraction and microscopy techniques. The multicomponent alloy exhibited a multiphase structure, comprising two face-centered cubic (FCC) phases and an oxide phase. Upon oxidation, the material transformed into a spinel oxide with a minor presence of CuO. The resulting high-entropy oxide demonstrated excellent electrochemical behavior when utilized as an anode material. Cyclic voltammetry revealed distinctive reduction peaks attributed to cation reduction and solid electrolyte interphase (SEI) layer formation, while subsequent cycles showcased high reversibility. Electrochemical impedance spectroscopy indicated a decrease in charge transfer resistance during cycling, emphasizing the remarkable electrochemical performance. Galvanostatic charge/discharge tests displayed characteristic voltage profiles, with an initial irreversible capacity attributed to SEI layer formation. The HEO exhibited promising rate capability, surpassing commercial graphite at higher current densities. The battery achieved 80% (275 mAh g−1) of its initial stable capacity at a current density of 500 mA g−1 by the 312th cycle. Post-mortem analysis revealed structural amorphization during cycling, contributing to the observed electrochemical behavior. This research highlights the potential of HEOs as advanced anode materials for lithium-ion batteries, combining unique structural features with favorable electrochemical properties.