Volume 136, Issue 38 e202409435

Forschungsartikel

In Situ Analysis of Interfacial Morphological and Chemical Evolution in All-Solid-State Lithium-Metal Batteries

Dr. Xu-Sheng Zhang

CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 People's Republic of China

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Dr. Jing Wan,

Dr. Jing Wan

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Dr. Zhen-Zhen Shen,

Dr. Zhen-Zhen Shen

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Shuang-Yan Lang,

Prof. Dr. Shuang-Yan Lang

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Sen Xin,

Prof. Dr. Sen Xin

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Rui Wen,

Corresponding Author

Prof. Dr. Rui Wen

[email protected]

orcid.org/0000-0003-2644-7452

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Yu-Guo Guo,

Corresponding Author

Prof. Dr. Yu-Guo Guo

[email protected]

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Li-Jun Wan,

Corresponding Author

Prof. Dr. Li-Jun Wan

[email protected]

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Dr. Xu-Sheng Zhang,

Dr. Xu-Sheng Zhang

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Dr. Jing Wan,

Dr. Jing Wan

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Dr. Zhen-Zhen Shen,

Dr. Zhen-Zhen Shen

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Shuang-Yan Lang,

Prof. Dr. Shuang-Yan Lang

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Sen Xin,

Prof. Dr. Sen Xin

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Rui Wen,

Corresponding Author

Prof. Dr. Rui Wen

[email protected]

orcid.org/0000-0003-2644-7452

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Yu-Guo Guo,

Corresponding Author

Prof. Dr. Yu-Guo Guo

[email protected]

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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Prof. Dr. Li-Jun Wan,

Corresponding Author

Prof. Dr. Li-Jun Wan

[email protected]

University of Chinese Academy of Sciences, Beijing, 100190 People's Republic of China

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First published: 30 June 2024

https://doi.org/10.1002/ange.202409435

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Abstract

In situ analysis of Li plating/stripping processes and evolution of solid electrolyte interphase (SEI) are critical for optimizing all-solid-state Li metal batteries (ASSLMB). However, the buried solid-solid interfaces present a challenge for detection which preclude the employment of multiple analysis techniques. Herein, by employing complementary in situ characterizations, morphological/chemical evolution, Li plating/stripping dynamics and SEI dynamics were directly detected. As a mixed ionic-electronic conducting interface, Li|Li₁₀GeP₂S₁₂ (LGPS) performed distinct interfacial morphological/chemical evolution and dynamics from ionic-conducting/electronic-isolating interface like Li|Li₃PS₄ (LPS), which were revealed by combination of in situ atomic force microscopy and in situ X-ray photoelectron spectroscopy. Though Li plating speed in LGPS was higher than LPS, speed of SSE decomposition was similar and ~85 % interfacial SSE turned into SEI during plating and remained unchanged in stripping. To leverage strengths of different SSEs, an LPS-LGPS-LPS sandwich electrolyte was developed, demonstrating enhanced ionic conductivity and improved interfacial stability with less SSE decomposition (25 %). Using in situ Kelvin probe force microscopy, Li-ion behavior at interface between different SSEs was effectively visualized, uncovering distribution of Li ions at LGPS|LPS interface under different potentials.

Conflict of Interests

The authors declare no conflict of interest.

Open Research

Data Availability Statement

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

Supporting Information

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Volume136, Issue38

September 16, 2024

e202409435

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In Situ Analysis of Interfacial Morphological and Chemical Evolution in All-Solid-State Lithium-Metal Batteries

Abstract

Conflict of Interests

Open Research

Data Availability Statement

Supporting Information

References

References

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In Situ Analysis of Interfacial Morphological and Chemical Evolution in All-Solid-State Lithium-Metal Batteries

Abstract

Conflict of Interests

Open Research

Data Availability Statement

Supporting Information

References

References

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