Customized Design of LiF-Rich SEI Layer on Lithium Metal Anode for High Flame Retardant Electrolyte

Haibo Li; Xiaoya Qu; Yicai Pan; Na Li; Chuancong Zhou; Zaowen Zhao; Zhenyue Xing; Xiaodong Shi; Xinlong Tian; Peng Wang

doi:10.1002/cey2.70077

Customized Design of LiF-Rich SEI Layer on Lithium Metal Anode for High Flame Retardant Electrolyte

Haibo Li (Co-first Author), Xiaoya Qu (Co-first Author), Yicai Pan, Na Li^*, Chuancong Zhou, Zaowen Zhao, Zhenyue Xing, Xiaodong Shi^*, Xinlong Tian^*, Peng Wang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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Abstract

Gel polymer electrolytes (GPEs) with high flame-retardant concentration can remarkably reduce the thermal runaway risk of lithium metal batteries (LMBs). However, higher flame-retardant content in GPEs always leads to increased leakage of active component and severe lithium corrosion, which greatly hinders the service life of LMBs. Herein, GPEs with high-loading triphenyl phosphate (TPP) are originally fabricated by coaxial electrospinning and stabilized by dual confinement effects, including chemisorption of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), and physical encapsulation of polyacrylonitrile (PAN)/PVDF-HFP. These effects arise from the strong polar interactions between the -CF₃group in PVDF-HFP and P=O group in TPP, as well as the superior anti-swelling property of PAN. To mitigate TPP-induced corrosion during cycling, the optimized Li anode is armored with LiF-rich solid electrolyte interphase (SEI) layer through immersing it in fluoroethylene carbonate-containing electrolyte. As expected, the corresponding Li||Li symmetric cells deliver long-term stable cycling behavior over 2400 h at 0.5 mA cm^-2, and the LiFePO₄||Li batteries hold a high-capacity retention ratio of 81.7% after 6000 cycles at 10 C with excellent flame retardancy. These findings offer new insight into designing the SEI layer for lithium metal in flame-retardant electrolytes, thus promoting the development and application of high-security LMBs.

© 2025 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.

Original language	English
Article number	e70077
Number of pages	11
Journal	Carbon Energy
Volume	7
Issue number	11
Online published	23 Sept 2025
DOIs	https://doi.org/10.1002/cey2.70077
Publication status	Published - Nov 2025

Funding

The authors thank the financial support from the National Natural Science Foundation of China (52404316, 52474325), the S&T program of Hebei Province (225A4404D), the Natural Science Foundation of Hainan Province (524RC475), the Collaborative Innovation Center of Marine Science and Technology of Hainan University (XTCX2022HYC14), and the Xingtai City Natural Science Foundation (2023ZZ027). Additionally, this study is partially supported by the Pico Election Microscopy Center of Hainan University.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

dual confinement effects
gel polymer electrolyte
lithium metal batteries
solid electrolyte interphase layer

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This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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title = "Customized Design of LiF-Rich SEI Layer on Lithium Metal Anode for High Flame Retardant Electrolyte",

abstract = "Gel polymer electrolytes (GPEs) with high flame-retardant concentration can remarkably reduce the thermal runaway risk of lithium metal batteries (LMBs). However, higher flame-retardant content in GPEs always leads to increased leakage of active component and severe lithium corrosion, which greatly hinders the service life of LMBs. Herein, GPEs with high-loading triphenyl phosphate (TPP) are originally fabricated by coaxial electrospinning and stabilized by dual confinement effects, including chemisorption of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), and physical encapsulation of polyacrylonitrile (PAN)/PVDF-HFP. These effects arise from the strong polar interactions between the -CF3 group in PVDF-HFP and P=O group in TPP, as well as the superior anti-swelling property of PAN. To mitigate TPP-induced corrosion during cycling, the optimized Li anode is armored with LiF-rich solid electrolyte interphase (SEI) layer through immersing it in fluoroethylene carbonate-containing electrolyte. As expected, the corresponding Li||Li symmetric cells deliver long-term stable cycling behavior over 2400 h at 0.5 mA cm-2, and the LiFePO4||Li batteries hold a high-capacity retention ratio of 81.7% after 6000 cycles at 10 C with excellent flame retardancy. These findings offer new insight into designing the SEI layer for lithium metal in flame-retardant electrolytes, thus promoting the development and application of high-security LMBs.{\textcopyright} 2025 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.",

keywords = "dual confinement effects, gel polymer electrolyte, lithium metal batteries, solid electrolyte interphase layer",

author = "Haibo Li and Xiaoya Qu and Yicai Pan and Na Li and Chuancong Zhou and Zaowen Zhao and Zhenyue Xing and Xiaodong Shi and Xinlong Tian and Peng Wang",

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T1 - Customized Design of LiF-Rich SEI Layer on Lithium Metal Anode for High Flame Retardant Electrolyte

AU - Li, Haibo

AU - Qu, Xiaoya

AU - Pan, Yicai

AU - Li, Na

AU - Zhou, Chuancong

AU - Zhao, Zaowen

AU - Xing, Zhenyue

AU - Shi, Xiaodong

AU - Tian, Xinlong

AU - Wang, Peng

PY - 2025/11

Y1 - 2025/11

N2 - Gel polymer electrolytes (GPEs) with high flame-retardant concentration can remarkably reduce the thermal runaway risk of lithium metal batteries (LMBs). However, higher flame-retardant content in GPEs always leads to increased leakage of active component and severe lithium corrosion, which greatly hinders the service life of LMBs. Herein, GPEs with high-loading triphenyl phosphate (TPP) are originally fabricated by coaxial electrospinning and stabilized by dual confinement effects, including chemisorption of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), and physical encapsulation of polyacrylonitrile (PAN)/PVDF-HFP. These effects arise from the strong polar interactions between the -CF3 group in PVDF-HFP and P=O group in TPP, as well as the superior anti-swelling property of PAN. To mitigate TPP-induced corrosion during cycling, the optimized Li anode is armored with LiF-rich solid electrolyte interphase (SEI) layer through immersing it in fluoroethylene carbonate-containing electrolyte. As expected, the corresponding Li||Li symmetric cells deliver long-term stable cycling behavior over 2400 h at 0.5 mA cm-2, and the LiFePO4||Li batteries hold a high-capacity retention ratio of 81.7% after 6000 cycles at 10 C with excellent flame retardancy. These findings offer new insight into designing the SEI layer for lithium metal in flame-retardant electrolytes, thus promoting the development and application of high-security LMBs.© 2025 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.

AB - Gel polymer electrolytes (GPEs) with high flame-retardant concentration can remarkably reduce the thermal runaway risk of lithium metal batteries (LMBs). However, higher flame-retardant content in GPEs always leads to increased leakage of active component and severe lithium corrosion, which greatly hinders the service life of LMBs. Herein, GPEs with high-loading triphenyl phosphate (TPP) are originally fabricated by coaxial electrospinning and stabilized by dual confinement effects, including chemisorption of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), and physical encapsulation of polyacrylonitrile (PAN)/PVDF-HFP. These effects arise from the strong polar interactions between the -CF3 group in PVDF-HFP and P=O group in TPP, as well as the superior anti-swelling property of PAN. To mitigate TPP-induced corrosion during cycling, the optimized Li anode is armored with LiF-rich solid electrolyte interphase (SEI) layer through immersing it in fluoroethylene carbonate-containing electrolyte. As expected, the corresponding Li||Li symmetric cells deliver long-term stable cycling behavior over 2400 h at 0.5 mA cm-2, and the LiFePO4||Li batteries hold a high-capacity retention ratio of 81.7% after 6000 cycles at 10 C with excellent flame retardancy. These findings offer new insight into designing the SEI layer for lithium metal in flame-retardant electrolytes, thus promoting the development and application of high-security LMBs.© 2025 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.

KW - dual confinement effects

KW - gel polymer electrolyte

KW - lithium metal batteries

KW - solid electrolyte interphase layer

UR - https://www.webofscience.com/wos/woscc/full-record/WOS:001576956700001

U2 - 10.1002/cey2.70077

DO - 10.1002/cey2.70077

M3 - RGC 21 - Publication in refereed journal

SN - 2637-9368

VL - 7

JO - Carbon Energy

JF - Carbon Energy

IS - 11

M1 - e70077

ER -

Customized Design of LiF-Rich SEI Layer on Lithium Metal Anode for High Flame Retardant Electrolyte

Abstract

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UN SDGs

Research Keywords

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