In Situ Construction of LiF/Li3N/LixGa Hybrid SEI to Boost Long‐Lifespan Succinonitrile‐Based Solid‐State Lithium Metal Batteries

AbstractSuccinonitrile (SN)‐based in situ polymerized solid‐state electrolytes (SIPSSEs) for lithium batteries have attracted considerable attention due to their high ionic conductivity, wide electrochemical stability window (ESW), and potential for large‐scale applications. Despite these advantages, the polar cyano groups in SN molecules lead to significant interfacial problems upon direct contact with metallic lithium (Li), including unstable solid electrolyte interface (SEI) and the growth of Li dendrites, which impede the further application of SIPSSEs to solid‐state lithium metal batteries (SSLMBs). To address these challenges, here a GaF3‐modified SIPSSE (GSNE) is developed by incorporating GaF3 and fluoroethylene carbonate to passivate metallic Li and employing ethoxylated trimethylolpropane triacrylate to anchor SN molecules. As a result of this strategic electrolyte component design, GSNE achieves an ionic conductivity of 1.3 × 10−3 S cm−1 at 30 °C as well as wide ESW up to 4.6 V. Additionally, a LiF/Li3N/LixGa hybrid SEI is formed on the metallic Li surface through an in situ alloying reaction. This hybrid SEI demonstrates superior interfacial stability and fast Li⁺ transport kinetics, as confirmed by various advanced characterization techniques and theoretical calculations. Consequently, LiFePO4/GSNE/Li cells exhibit excellent rate performance and cycling stability. This work provides new insights into the designing of long‐lifespan SIPSSEs‐based SSLMBs.

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Details

Published: Feb 12, 2025
Vol/Issue: 35(28)
License: View

Authors

T

Tianqi Yang

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China; Department of Physics City University of Hong Kong Hong Kong 999077 China

J

Jiatao Lou

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518057 China

L

Liuyi Hu

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

Q

Qi Liu

Department of Physics City University of Hong Kong Hong Kong 999077 China; Shenzhen Research Institute City University of Hong Kong Shenzhen 518057 China

Z

Zhouyu Huang

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

Q

Qingru Zhou

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

H

Haiyuan Zhang

Tianneng Battery Group Co. Ltd. Changxing 313100 China

W

Wenlong Song

Tianneng Battery Group Co. Ltd. Changxing 313100 China

H

Hui Huang

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

Y

Yao Wang

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

X

Xinyong Tao

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

Y

Yang Xia

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

W

Wang Zhang

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

J

Jun Zhang

College of Materials Science and Engineering Zhejiang University of Technology Hangzhou 310014 China

Funding

National Natural Science Foundation of China Award: 21972127

Fundamental Research Funds for the Provincial Universities of Zhejiang Award: RF‐C2022008

Cite This Article

Tianqi Yang, Jiatao Lou, Liuyi Hu, et al. (2025). In Situ Construction of LiF/Li3N/LixGa Hybrid SEI to Boost Long‐Lifespan Succinonitrile‐Based Solid‐State Lithium Metal Batteries. Advanced Functional Materials, 35(28). https://doi.org/10.1002/adfm.202423719

In Situ Construction of LiF/Li3N/LixGa Hybrid SEI to Boost Long‐Lifespan Succinonitrile‐Based Solid‐State Lithium Metal Batteries

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