Fluorination Engineering for Stable Interfacial Chemistry in Deep Eutectic Amide-Based Electrolytes Enables High-Performance LiNi0.8Co0.1Mn0.1O2/Li Batteries

Yuanxin Gao; Xinyi Wang; Dong Lv; Zhang Zhang; Jiangpeng Li; Xiaoyan Feng; Jingchao Chai; Yun Zheng; Yu Peng; Yanqing Wang; Yingying Wang; Lingyu Zhu; Zhihong Liu

doi:10.1002/eem2.70157

Fluorination Engineering for Stable Interfacial Chemistry in Deep Eutectic Amide-Based Electrolytes Enables High-Performance LiNi_0.8Co_0.1Mn_0.1O₂/Li Batteries

Yuanxin Gao, Xinyi Wang, Dong Lv, Zhang Zhang, Jiangpeng Li, Xiaoyan Feng, Jingchao Chai^*, Yun Zheng, Yu Peng, Yanqing Wang, Yingying Wang, Lingyu Zhu^*, Zhihong Liu^*

^*Corresponding author for this work

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

1 Citation (Scopus)

Abstract

Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10⁻⁴S cm⁻¹) and anodic stability (>4.4 V vs Li⁺/Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li⁺ transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.

© 2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.

Original language	English
Article number	e70157
Number of pages	11
Journal	Energy & Environmental Materials
Online published	10 Sept 2025
DOIs	https://doi.org/10.1002/eem2.70157
Publication status	Online published - 10 Sept 2025

Funding

Y.G. and X.W. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (22209059, 22139001), Hubei Provincial Natural Science Fundation of China (2025AFA025, 2023AFB1117), the Young Talents Research Project of the Department of Education of Hubei Province (Grant No. Q20234401), and the Natural Science Foundation of Shandong Province (Grant No. ZR2021QB053).

UN SDGs

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

SDG 7 Affordable and Clean Energy

Research Keywords

fluoroamide
fluoroethylene carbonate
lithium metal battery
Ni-rich ternary cathode
non-flammable

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Cite this

Gao, Y., Wang, X., Lv, D., Zhang, Z., Li, J., Feng, X., Chai, J., Zheng, Y., Peng, Y., Wang, Y., Wang, Y., Zhu, L., & Liu, Z. (2025). Fluorination Engineering for Stable Interfacial Chemistry in Deep Eutectic Amide-Based Electrolytes Enables High-Performance LiNi_0.8Co_0.1Mn_0.1O₂/Li Batteries. Energy & Environmental Materials, Article e70157. Advance online publication. https://doi.org/10.1002/eem2.70157

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abstract = "Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10−4 S cm−1) and anodic stability (>4.4 V vs Li+/Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li+ transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.{\textcopyright} 2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.",

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author = "Yuanxin Gao and Xinyi Wang and Dong Lv and Zhang Zhang and Jiangpeng Li and Xiaoyan Feng and Jingchao Chai and Yun Zheng and Yu Peng and Yanqing Wang and Yingying Wang and Lingyu Zhu and Zhihong Liu",

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T1 - Fluorination Engineering for Stable Interfacial Chemistry in Deep Eutectic Amide-Based Electrolytes Enables High-Performance LiNi0.8Co0.1Mn0.1O2/Li Batteries

AU - Gao, Yuanxin

AU - Wang, Xinyi

AU - Lv, Dong

AU - Zhang, Zhang

AU - Li, Jiangpeng

AU - Feng, Xiaoyan

AU - Chai, Jingchao

AU - Zheng, Yun

AU - Peng, Yu

AU - Wang, Yanqing

AU - Wang, Yingying

AU - Zhu, Lingyu

AU - Liu, Zhihong

PY - 2025/9/10

Y1 - 2025/9/10

N2 - Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10−4 S cm−1) and anodic stability (>4.4 V vs Li+/Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li+ transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.© 2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.

AB - Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10−4 S cm−1) and anodic stability (>4.4 V vs Li+/Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li+ transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.© 2025 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.

KW - fluoroamide

KW - fluoroethylene carbonate

KW - lithium metal battery

KW - Ni-rich ternary cathode

KW - non-flammable

UR - https://www.webofscience.com/wos/woscc/full-record/WOS:001569464200001

U2 - 10.1002/eem2.70157

DO - 10.1002/eem2.70157

M3 - RGC 21 - Publication in refereed journal

SN - 2575-0356

JO - Energy & Environmental Materials

JF - Energy & Environmental Materials

M1 - e70157

ER -