A cathode homogenization strategy for enabling long-cycle-life all-solid-state lithium batteries

Longfei Cui, Shu Zhang, Jiangwei Ju (), Tao Liu, Yue Zheng, Jiahao Xu, Yantao Wang, Jiedong Li, Jingwen Zhao, Jun Ma, Jinzhi Wang, Gaojie Xu, Ting-Shan Chan, Yu-Cheng Huang, Shu-Chih Haw, Jin-Ming Chen, Zhiwei Hu and Guanglei Cui ()
Additional contact information
Longfei Cui: Chinese Academy of Sciences
Shu Zhang: Chinese Academy of Sciences
Jiangwei Ju: Chinese Academy of Sciences
Tao Liu: Chinese Academy of Sciences
Yue Zheng: Chinese Academy of Sciences
Jiahao Xu: Chinese Academy of Sciences
Yantao Wang: Chinese Academy of Sciences
Jiedong Li: Chinese Academy of Sciences
Jingwen Zhao: Chinese Academy of Sciences
Jun Ma: Chinese Academy of Sciences
Jinzhi Wang: Chinese Academy of Sciences
Gaojie Xu: Chinese Academy of Sciences
Ting-Shan Chan: National Synchrotron Radiation Research Center
Yu-Cheng Huang: National Synchrotron Radiation Research Center
Shu-Chih Haw: National Synchrotron Radiation Research Center
Jin-Ming Chen: National Yang Ming Chiao Tung University (NYCU)
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Guanglei Cui: Chinese Academy of Sciences

Nature Energy, 2024, vol. 9, issue 9, 1084-1094

Abstract: Abstract All-solid-state lithium batteries typically employ heterogeneous composite cathodes where conductive additives are introduced to improve mixed conduction. These electrochemically inactive additives are not fully compatible with layered oxide cathodes that undergo large volume change, significantly reducing battery energy density and cycle life. Here we propose a cathode homogenization strategy by cold pressing a zero-strain cathode material with efficient mixed conduction throughout the (dis)charge process. Li1.75Ti2(Ge0.25P0.75S3.8Se0.2)3 possesses considerable Li+/electronic conductivity of 0.22/242 mS cm−1 when fully charged, increasing monotonically to 0.66/412 mS cm−1 when fully discharged. It delivers a specific capacity of 250 mAh g−1 and undergoes a 1.2% volume change. Homogeneous cathodes composed of 100% Li1.75Ti2(Ge0.25P0.75S3.8Se0.2)3 enable room-temperature all-solid-state lithium batteries to achieve a cycle life of over 20,000 cycles at 2.5 C with a specific capacity retention of 70% and a high energy density of 390 Wh kg−1 at the cell level at 0.1 C. This cathode homogenization strategy contrasts to the conventional cathode heterogeneous design, potentially improving the viability of all-solid-state lithium batteries for commercial applications.

Date: 2024
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DOI: 10.1038/s41560-024-01596-6

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