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Promoting high-voltage stability through local lattice distortion of halide solid electrolytes

Zhenyou Song, Tengrui Wang, Hua Yang, Wang Hay Kan (), Yuwei Chen, Qian Yu, Likuo Wang, Yini Zhang, Yiming Dai, Huaican Chen, Wen Yin, Takashi Honda, Maxim Avdeev, Henghui Xu, Jiwei Ma, Yunhui Huang () and Wei Luo ()
Additional contact information
Zhenyou Song: Tongji University
Tengrui Wang: Tongji University
Hua Yang: Spallation Neutron Source Science Center
Wang Hay Kan: Spallation Neutron Source Science Center
Yuwei Chen: Tongji University
Qian Yu: Tongji University
Likuo Wang: Tongji University
Yini Zhang: Tongji University
Yiming Dai: Tongji University
Huaican Chen: Spallation Neutron Source Science Center
Wen Yin: Spallation Neutron Source Science Center
Takashi Honda: High Energy Accelerator Research Organization (KEK)
Maxim Avdeev: Australian Nuclear Science and Technology Organisation (ANSTO)
Henghui Xu: Huazhong University of Science and Technology
Jiwei Ma: Tongji University
Yunhui Huang: Huazhong University of Science and Technology
Wei Luo: Tongji University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl−, which effectively curbs kinetics of their oxidation. The confinement is realized by substituting In with multiple elements in Li3InCl6 to give a high-entropy Li2.75Y0.16Er0.16Yb0.16In0.25Zr0.25Cl6. Meanwhile, the lattice distortion promotes longer Li-Cl bonds, facilitating favorable activation of Li+. Our results show that this high-entropy halide electrolyte boosts the cycle stability of all-solid-state battery by 250% improvement over 500 cycles. In particular, the cell provides a higher discharge capacity of 185 mAh g−1 by increasing the charge cut-off voltage to 4.6 V at a small current rate of 0.2 C, which is more challenging to electrolytes|cathode stability. These findings deepen our understanding of high-entropy materials, advancing their use in energy-related applications.

Date: 2024
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DOI: 10.1038/s41467-024-45864-1

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