Entropy-increased LiMn2O4-based positive electrodes for fast-charging lithium metal batteries

Weihao Zeng, Fanjie Xia, Juan Wang, Jinlong Yang, Haoyang Peng, Wei Shu, Quan Li, Hong Wang, Guan Wang, Shichun Mu () and Jinsong Wu ()
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Weihao Zeng: Wuhan University of Technology
Fanjie Xia: Wuhan University of Technology
Juan Wang: Wuhan University of Technology
Jinlong Yang: Shenzhen University
Haoyang Peng: Wuhan University of Technology
Wei Shu: Wuhan University of Technology
Quan Li: Wuhan University of Technology
Hong Wang: Wuhan University of Technology
Guan Wang: Wuhan University of Technology
Shichun Mu: Wuhan University of Technology
Jinsong Wu: Wuhan University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Fast-charging, non-aqueous lithium-based batteries are desired for practical applications. In this regard, LiMn2O4 is considered an appealing positive electrode active material because of its favourable ionic diffusivity due to the presence of three-dimensional Li-ion diffusion channels. However, LiMn2O4 exhibits inadequate rate capabilities and rapid structural degradation at high currents. To circumvent these issues, here we introduce quintuple low-valence cations to increase the entropy of LiMn2O4. As a result, the entropy-increased LiMn2O4-based material, i.e., LiMn1.9Cu0.02Mg0.02Fe0.02Zn0.02Ni0.02O4, when tested in non-aqueous lithium metal coin cell configuration, enable 1000 cell cycles at 1.48 A g−1 (corresponding to a cell charging time of 4 minutes) and 25°C with a discharge capacity retention of about 80%. We demonstrate that the increased entropy in LiMn2O4 leads to an increase in the disordering of dopant cations and a contracted local structure, where the enlarged LiO4 space and enhanced Mn-O covalency improve the Li-ion transport and stabilize the diffusion channels. We also prove that stress caused by cycling at a high cell state of charge is relieved through elastic deformation via a solid-solution transition, thus avoiding structural degradation upon prolonged cycling.

Date: 2024
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DOI: 10.1038/s41467-024-51168-1

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