April 30, 2024 | Ki-Hun Nam, Zhongling Wang, Jessica Luo, Cynthia Huang, Marie F. Millares, Alexis Pace, Lei Wang, Steven T. King, Lu Ma, Steven Ehrlich, Jianming Bai, Esther S. Takeuchi, Amy C. Marschilok, Shan Yan, Kenneth J. Takeuchi, and Marca M. Doeff
The study investigates the electrochemical performance of high-entropy spinel oxide ferrites (HESO) as conversion anode materials for lithium-ion batteries. Four different HESO compositions, each containing five or six metals, were synthesized using a simple combustion synthesis method and evaluated in lithium half-cells. The HESO materials demonstrated superior electrochemical performance compared to conventional spinel ferrites like Fe₃O₄ and MgFe₂O₄, maintaining capacities above 600 mAh g⁻¹ for 150 cycles. X-ray absorption spectroscopy (XAS) analysis revealed that Fe, Co, Ni, and Cu were reduced to the elemental state during the first discharge, while Mn was only slightly reduced. Upon recharge, Fe was reoxidized to an average oxidation state of about +2.6, while Co, Ni, and Cu remained in the metallic state. The ability of Fe to be oxidized beyond +2 contributed to the high capacities observed, and the presence of metallic elements provided an electronically conductive network that enhanced charge transfer. The HESO materials showed good rate capability and stable capacity retention, making them promising candidates for next-generation LIB anodes.The study investigates the electrochemical performance of high-entropy spinel oxide ferrites (HESO) as conversion anode materials for lithium-ion batteries. Four different HESO compositions, each containing five or six metals, were synthesized using a simple combustion synthesis method and evaluated in lithium half-cells. The HESO materials demonstrated superior electrochemical performance compared to conventional spinel ferrites like Fe₃O₄ and MgFe₂O₄, maintaining capacities above 600 mAh g⁻¹ for 150 cycles. X-ray absorption spectroscopy (XAS) analysis revealed that Fe, Co, Ni, and Cu were reduced to the elemental state during the first discharge, while Mn was only slightly reduced. Upon recharge, Fe was reoxidized to an average oxidation state of about +2.6, while Co, Ni, and Cu remained in the metallic state. The ability of Fe to be oxidized beyond +2 contributed to the high capacities observed, and the presence of metallic elements provided an electronically conductive network that enhanced charge transfer. The HESO materials showed good rate capability and stable capacity retention, making them promising candidates for next-generation LIB anodes.