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Journal Article

High-Entropy Phase Stabilization Engineering Enables High-Performance Layered Cathode for Sodium-Ion Batteries

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Hu,  Zhiwei
Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

Wang, B., Ma, J., Wang, K., Wang, D., Xu, G., Wang, X., et al. (2024). High-Entropy Phase Stabilization Engineering Enables High-Performance Layered Cathode for Sodium-Ion Batteries. Advanced Energy Materials, 14(23): 2401090, pp. 1-8. doi:10.1002/aenm.202401090.


Cite as: https://hdl.handle.net/21.11116/0000-000F-3766-1
Abstract
O3-type layered oxides are considered as one of the most promising cathode materials for rechargeable sodium-ion batteries (SIBs) due to their appealing energy density and feasible synthesis. Nevertheless, it undergoes complicated phase transitions and pronounced structural degradation during the cycling of charge/discharge process, rendering severe volumetric strain and poor cycling performance. Herein, a zero-strain high-entropy NaNi0.2Fe0.2Mn0.35Cu0.05Zn0.1Sn0.1O2 cathode for SIBs is presented by high-entropy phase stabilization engineering. It is verified that this low-nickel cobalt-free high-entropy cathode can deliver a highly reversible phase evolution, zero volumetric strain, and a significantly improved cycling performance in full cells (87% capacity retention after 500 cycles at 3.0 C). Combining X-ray absorption spectra and first-principles calculations, the varied elemental functions in the high-entropy framework are clearly elucidated, namely, Ni/Fe/Cu acts as charge compensators, while Mn/Zn/Sn serve as interlayer slipping inhibitors through enhanced charge localization besides their stable valence states. By addressing the volumetric strain and cycling instability concerns for O3-type cathode materials, this work presents a promising strategy for inhibiting irreversible phase transitions and structural degradation in intercalation electrodes, which significantly boosts the development of commercially feasible cathodes for high-performance SIBs. © 2024 Wiley-VCH GmbH.