Self-organized hetero-nanodomains actuating super Li+ conduction in glass ceramics

Yantao Wang, Hongtao Qu, Bowen Liu, Xiaoju Li, Jiangwei Ju (), Jiedong Li, Shu Zhang, Jun Ma, Chao Li, Zhiwei Hu, Chung-Kai Chang, Hwo-Shuenn Sheu, Longfei Cui, Feng Jiang, Ernst R. H. Eck, Arno P. M. Kentgens (), Guanglei Cui () and Liquan Chen
Additional contact information
Yantao Wang: Chinese Academy of Sciences
Hongtao Qu: Radboud University
Bowen Liu: Tianjin University of Technology
Xiaoju Li: Shandong University
Jiangwei Ju: Chinese Academy of Sciences
Jiedong Li: Chinese Academy of Sciences
Shu Zhang: Chinese Academy of Sciences
Jun Ma: Chinese Academy of Sciences
Chao Li: Tianjin University of Technology
Zhiwei Hu: Max Plank Institute for Chemical Physics of Solids
Chung-Kai Chang: National Synchrotron Radiation Research Center
Hwo-Shuenn Sheu: National Synchrotron Radiation Research Center
Longfei Cui: Chinese Academy of Sciences
Feng Jiang: Chinese Academy of Sciences
Ernst R. H. Eck: Radboud University
Arno P. M. Kentgens: Radboud University
Guanglei Cui: Chinese Academy of Sciences
Liquan Chen: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Easy-to-manufacture Li2S-P2S5 glass ceramics are the key to large-scale all-solid-state lithium batteries from an industrial point of view, while their commercialization is greatly hampered by the low room temperature Li+ conductivity, especially due to the lack of solutions. Herein, we propose a nanocrystallization strategy to fabricate super Li+-conductive glass ceramics. Through regulating the nucleation energy, the crystallites within glass ceramics can self-organize into hetero-nanodomains during the solid-state reaction. Cryogenic transmission electron microscope and electron holography directly demonstrate the numerous closely spaced grain boundaries with enriched charge carriers, which actuate superior Li+-conduction as confirmed by variable-temperature solid-state nuclear magnetic resonance. Glass ceramics with a record Li+ conductivity of 13.2 mS cm−1 are prepared. The high Li+ conductivity ensures stable operation of a 220 μm thick LiNi0.6Mn0.2Co0.2O2 composite cathode (8 mAh cm−2), with which the all-solid-state lithium battery reaches a high energy density of 420 Wh kg−1 by cell mass and 834 Wh L−1 by cell volume at room temperature. These findings bring about powerful new degrees of freedom for engineering super ionic conductors.

Date: 2023
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DOI: 10.1038/s41467-023-35982-7

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