Issue

Vol. 17 (2025)

Electron Acceptor-Driven Solid Electrolyte Interphases with Elevated LiF Content for 4.7 V Lithium Metal Batteries

https://doi.org/10.1007/s40820-025-01663-x
Yongbiao Mu
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Zifan Liao
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Youqi Chu
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Qing Zhang
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Lingfeng Zou
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Lin Yang
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Yitian Feng
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Haixiang Ren
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Meisheng Han
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China
Lin Zeng
Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen 518055, People’s Republic of China

Corresponding Author: Lin Zeng

zengl3@sustech.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 163

Abstract

High-voltage lithium (Li) metal batteries (LMBs) face substantial challenges, including Li dendrite growth and instability in high-voltage cathodes such as LiNi0.8Mn0.1Co0.1O2 (NCM811), which impede their practical applications and long-term stability. To address these challenges, tris(pentafluorophenyl)borane additive as an electron acceptor is introduced into an ethyl methyl carbonate/fluoroethylene carbonate-based electrolyte. This approach effectively engineers robust dual interfaces on the Li metal anode and the NCM811 cathode, thereby mitigating dendritic growth of Li and enhancing the stability of the cathode. This additive-driven strategy enables LMBs to operate at ultra-high voltages up to 4.7 V. Consequently, Li||Cu cells achieve a coulombic efficiency of 98.96%, and Li||Li symmetric cells extend their cycle life to an impressive 4000 h. Li||NCM811 full cells maintain a high capacity retention of 87.8% after 100 cycles at 4.7 V. Additionally, Li||LNMO full cells exhibit exceptional rate capability, delivering 132.2 mAh g−1 at 10 C and retaining 95.0% capacity after 250 cycles at 1 C and 5 V. As a result, NCM811||graphite pouch cells maintain a 93.4% capacity retention after 1100 cycles at 1 C. These findings underscore the efficacy of additive engineering in addressing Li dendrite formation and instability of cathode under high voltage, thereby paving the road for durable, high-performance LMBs.


Highlights:
1 A tris(pentafluorophenyl)borane additive as an electron acceptor is incorporated into an ethyl methyl carbonate/fluoroethylene carbonate/lithium nitrate electrolyte.
2 This approach effectively engineers durable dual interfaces on both lithium metal anode and LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode, which mitigates dendritic growth and enhances cathode stability.
3 The additive-driven strategy enables lithium metal batteries to operate at ultra-high voltage up to 4.7 V and high mass loading of 14.0 mg cm−2 for NCM811 cathode, thus resulting in exceptional cycling performance.

Keywords

Lithium metal batteries High-voltage cathodes Electron acceptor Dendrite formation Dual interfaces
Mu, Yongbiao, Zifan Liao, Youqi Chu, Qing Zhang, Lingfeng Zou, Lin Yang, Yitian Feng, Haixiang Ren, Meisheng Han, and Lin Zeng. 2025. “Electron Acceptor-Driven Solid Electrolyte Interphases With Elevated LiF Content for 4.7 V Lithium Metal Batteries”. Nano-Micro Letters 17 (February):163. https://doi.org/10.1007/s40820-025-01663-x.
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