Volume 136, Issue 17 e202400303
Forschungsartikel

Long-cycling and High-voltage Solid State Lithium Metal Batteries Enabled by Fluorinated and Crosslinked Polyether Electrolytes

Jie Zhu

Jie Zhu

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Ruiqi Zhao

Ruiqi Zhao

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Jinping Zhang

Jinping Zhang

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Xingchen Song

Xingchen Song

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Jie Liu

Jie Liu

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Nuo Xu

Nuo Xu

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Hongtao Zhang

Corresponding Author

Hongtao Zhang

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Xiangjian Wan

Xiangjian Wan

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Xinyi Ji

Corresponding Author

Xinyi Ji

School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin, 300350 China E-mail: s

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Yanfeng Ma

Yanfeng Ma

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Chenxi Li

Chenxi Li

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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Yongsheng Chen

Corresponding Author

Yongsheng Chen

The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin, 300071 China

State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin, 300071 China

Renewable Energy Conversion and Storage Center (RECAST), Nankai University, Tianjin, 300071 China

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First published: 05 March 2024

Abstract

Solid-state lithium metal batteries (LMBs), constructed through the in situ fabrication of polymer electrolytes, are considered a critical strategy for the next-generation battery systems with high energy density and enhanced safety. However, the constrained oxidation stability of polymers, such as the extensively utilized polyethers, limits their applications in high-voltage batteries and further energy density improvements. Herein, an in situ fabricated fluorinated and crosslinked polyether-based gel polymer electrolyte, FGPE, is presented, exhibiting a high oxidation potential (5.1 V). The fluorinated polyether significantly improves compatibility with both lithium metal and high-voltage cathode, attributed to the electron-withdrawing −CF3 group and the generated LiF-rich electrolyte/electrode interphase. Consequently, the solid-state Li||LiNi0.6Co0.2Mn0.2O2 batteries employing FGPE demonstrate exceptional cycling performances of 1000 cycles with 78 % retention, representing one of the best results ever reported for polymer electrolytes. Moreover, FGPE enables batteries to operate at 4.7 V, realizing the highest operating voltage of polyether-based batteries to date. Notably, our designed in situ FGPE provides the solid-state batteries with exceptional cycling stability even at practical conditions, including high cathode loading (21 mg cm−2) and industry-level 18650-type cylindrical cells (1.3 Ah, 500 cycles). This work provides critical insights into the development of oxidation-stable polymer electrolytes and the advancement of practical high-voltage LMBs.

Conflict of interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material of this article.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.