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  • Title: Enhanced Li-Ion Diffusion and Cycling Stability of Ni-Free High-Entropy Spinel Oxide Anodes with High-Concentration Oxygen Vacancies.
    Author: Xiao B, Wu G, Wang T, Wei Z, Xie Z, Sui Y, Qi J, Wei F, Zhang X, Tang LB, Zheng JC.
    Journal: ACS Appl Mater Interfaces; 2023 Jan 18; 15(2):2792-2803. PubMed ID: 36606677.
    Abstract:
    High-entropy oxide (HEO) is an emerging type of anode material for lithium-ion batteries with excellent properties, where high-concentration oxygen vacancies can effectively enhance the diffusion coefficient of lithium ions. In this study, Ni-free spinel-type HEOs ((FeCoCrMnZn)3O4 and (FeCoCrMnMg)3O4) were prepared via ball milling, and the effects of zinc and magnesium on the concentration of oxygen vacancy (OV), lithium-ion diffusion coefficient (DLi+), and electrochemical performance of HEOs were investigated. Ab initio calculations show that the addition of zinc narrows down the band gap and thus improves the electrical conductivity. X-ray photoelectron spectroscopy (XPS) results show that (FeCoCrMnZn)3O4 (42.7%) and (FeCoCrMnMg)3O4 (42.5%) have high OV concentration. During charge/discharge, the OV concentration of (FeCoCrMnZn)3O4 is higher than that of (FeCoCrMnMg)3O4. The galvanostatic intermittent titration technique (GITT) results show that the DLi+ value of (FeCoCrMnZn)3O4 is higher than that of (FeCoCrMnMg)3O4 during charge and discharge. All of that can improve its specific discharge capacity and enhance its cycle stability. (FeCoCrMnZn)3O4 achieved a discharge capacity of 828.6 mAh g-1 at 2.0 A g-1 after 2000 cycles. This work provides a deep understanding of the structure and performance of HEO.
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