Mg vs. Zn Incorporation in High-Entropy Spinel Oxides: Toward Stable and High-Capacity Anodes for Lithium-Ion Batteries

Due to its unique high-entropy effect, high specific capacities, and enhanced structural stability, high-entropy oxides (HEOs) have become a promising anode material for lithium-ion batteries (LIBs). In this study, two six-component high-entropy spinel oxides (HESOs), (FeCoNiCrLiMg)3O4 and (FeCoNiCrLiZn)3O4, were synthesized for the first time using a solution combustion method. Their microstructures, electrochemical performance, and electronic structures were comprehensively studied. Structural characterization confirmed that both materials exhibit a single-phase spinel structure with uniform elemental distribution. At a current density of 1 A·g-1, 5M-Mg and 5M-Zn maintained specific capacities of 473 mAh·g-1 and 637 mAh·g-1, respectively, after 500 cycles, indicating outstanding cycling stability. Cyclic voltammetry analysis revealed distinct charge storage mechanisms: 5M-Mg is dominated by surface-controlled (capacitive) behavior, whereas 5M-Zn primarily follows a diffusion-controlled mechanism. Furthermore, first-principles calculations indicated that Zn incorporation enhances metallicity and increases electronic conductivity. These findings demonstrate that adjusting the Mg/Zn composition effectively tailors the electrochemical properties of HESOs, providing new insights into designing high-performance anode materials for LIBs. Supplementary Material File (main document.docx) - Download - 40.09 MB Information & Authors Information Version history Copyright This work is licensed under a Non Exclusive No Reuse License.

Authors Metrics & Citations Metrics Article Usage 176views 97downloads Citations Download citation chengjiao che, Jia Li, Jianqiang Bi, et al. Mg vs. Zn Incorporation in High-Entropy Spinel Oxides: Toward Stable and High-Capacity Anodes for Lithium-Ion Batteries. Authorea. 29 August 2025. DOI: https://doi.org/10.22541/au.175647954.46593975/v1 DOI: https://doi.org/10.22541/au.175647954.46593975/v1 If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download. For more information or tips please see 'Downloading to a citation manager' in the Help menu.