Volume 136, Issue 16 e202400562
Forschungsartikel

Surface Lattice Modulation Enables Stable Cycling of High-Loading All-solid-state Batteries at High Voltages

Hong-Shen Zhang

Hong-Shen Zhang

CAS Key Laboratory of Molecular Nanostructure and Nanotechnol-ogy, and Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (CAS), No.2 Zhongguancun North First Street, 100190 Beijing, P. R. China

University of Chinese Academy of Sciences, No.19(A) Yuquan Road, 100049 Beijing, P. R. China

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Xin-Cheng Lei

Xin-Cheng Lei

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, No. 8 Zhongguancun South Third Street, 100190 Beijing, P. R. China

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Prof. Dong Su

Prof. Dong Su

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, No. 8 Zhongguancun South Third Street, 100190 Beijing, P. R. China

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Si-Jie Guo

Si-Jie Guo

CAS Key Laboratory of Molecular Nanostructure and Nanotechnol-ogy, and Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (CAS), No.2 Zhongguancun North First Street, 100190 Beijing, P. R. China

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Jia-Cheng Zhu

Jia-Cheng Zhu

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, No. 8 Zhongguancun South Third Street, 100190 Beijing, P. R. China

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Prof. Xue-Feng Wang

Prof. Xue-Feng Wang

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, No. 8 Zhongguancun South Third Street, 100190 Beijing, P. R. China

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Xing Zhang

Xing Zhang

CAS Key Laboratory of Molecular Nanostructure and Nanotechnol-ogy, and Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (CAS), No.2 Zhongguancun North First Street, 100190 Beijing, P. R. China

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Ting-Ting Wu

Ting-Ting Wu

CAS Key Laboratory of Molecular Nanostructure and Nanotechnol-ogy, and Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (CAS), No.2 Zhongguancun North First Street, 100190 Beijing, P. R. China

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Si-Qi Lu

Si-Qi Lu

CAS Key Laboratory of Molecular Nanostructure and Nanotechnol-ogy, and Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (CAS), No.2 Zhongguancun North First Street, 100190 Beijing, P. R. China

University of Chinese Academy of Sciences, No.19(A) Yuquan Road, 100049 Beijing, P. R. China

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Prof. Yu-Tao Li

Corresponding Author

Prof. Yu-Tao Li

Beijing Frontier Research Center on Clean Energy, Huairou Division, Institute of Physics, Chinese Academy of Sciences, Yongle North Second Street, Yanqi Economic Development Zone, Huairou District, 101400 Beijing, P. R. China

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Prof. An-Min Cao

Corresponding Author

Prof. An-Min Cao

CAS Key Laboratory of Molecular Nanostructure and Nanotechnol-ogy, and Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences (CAS), No.2 Zhongguancun North First Street, 100190 Beijing, P. R. China

University of Chinese Academy of Sciences, No.19(A) Yuquan Road, 100049 Beijing, P. R. China

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First published: 21 February 2024

Abstract

Halide solid electrolytes, known for their high ionic conductivity at room temperature and good oxidative stability, face notable challenges in all–solid–state Li–ion batteries (ASSBs), especially with unstable cathode/solid electrolyte (SE) interface and increasing interfacial resistance during cycling. In this work, we have developed an Al3+–doped, cation–disordered epitaxial nanolayer on the LiCoO2 surface by reacting it with an artificially constructed AlPO4 nanoshell; this lithium–deficient layer featuring a rock–salt–like phase effectively suppresses oxidative decomposition of Li3InCl6 electrolyte and stabilizes the cathode/SE interface at 4.5 V. The ASSBs with the halide electrolyte Li3InCl6 and a high–loading LiCoO2 cathode demonstrated high discharge capacity and long cycling life from 3 to 4.5 V. Our findings emphasize the importance of specialized cathode surface modification in preventing SE degradation and achieving stable cycling of halide–based ASSBs at high voltages.

Conflict of interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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