Issue

Vol. 16 (2024)

Boosting High-Voltage Practical Lithium Metal Batteries with Tailored Additives

https://doi.org/10.1007/s40820-024-01479-1
Jinhai You
College of Energy, Xiamen University, Xiamen 361005, People’s Republic of China
Qiong Wang
State Key Lab of Physical Chemistry of Solid Surface, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People’s Republic of China
Runhong Wei
Laboratory for Soft Matter and Biophysics, Department of Physics and Astronomy, KU Leuven, 3001 Leuven, Belgium
Li Deng
State Key Lab of Physical Chemistry of Solid Surface, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, People’s Republic of China
Yiyang Hu
College of Energy, Xiamen University, Xiamen 361005, People’s Republic of China
Li Niu
Laboratory for Soft Matter and Biophysics, Department of Physics and Astronomy, KU Leuven, 3001 Leuven, Belgium
Jingkai Wang
Magnetism Key Laboratory of Zhejiang Province, College of Materials and Chemistry, China Jiliang University, Hangzhou 310018, People’s Republic of China
Xiaomei Zheng
Magnetism Key Laboratory of Zhejiang Province, College of Materials and Chemistry, China Jiliang University, Hangzhou 310018, People’s Republic of China
Junwei Li
Department of Chemical Engineering, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
Yao Zhou
College of Energy, Xiamen University, Xiamen 361005, People’s Republic of China
Jun‑Tao Li
College of Energy, Xiamen University, Xiamen 361005, People’s Republic of China

Corresponding Author: Jun‑Tao Li

jtli@xmu.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 257

Abstract

The lithium (Li) metal anode is widely regarded as an ideal anode material for high-energy-density batteries. However, uncontrolled Li dendrite growth often leads to unfavorable interfaces and low Coulombic efficiency (CE), limiting its broader application. Herein, an ether-based electrolyte (termed FGN-182) is formulated, exhibiting ultra-stable Li metal anodes through the incorporation of LiFSI and LiNO3 as dual salts. The synergistic effect of the dual salts facilitates the formation of a highly robust SEI film with fast Li+ transport kinetics. Notably, Li||Cu half cells exhibit an average CE reaching up to 99.56%. In particular, pouch cells equipped with high-loading lithium cobalt oxide (LCO, 3 mAh cm−2) cathodes, ultrathin Li chips (25 μm), and lean electrolytes (5 g Ah−1) demonstrate outstanding cycling performance, retaining 80% capacity after 125 cycles. To address the gas issue in the cathode under high voltage, cathode additives 1,3,6-tricyanohexane is incorporated with FGN-182; the resulting high-voltage LCO||Li (4.4 V) pouch cells can cycle steadily over 93 cycles. This study demonstrates that, even with the use of ether-based electrolytes, it is possible to simultaneously achieve significant improvements in both high Li utilization and electrolyte tolerance to high voltage by exploring appropriate functional additives for both the cathode and anode.


Highlights:
1 FGN-182 electrolytes exhibit highly reversible Li plating/stripping with an average Coulombic efficiency reaching up to 99.56% determined from Auerbach’s test.
2 The gas-evolution process of LiNO3 in high-voltage lithium cobalt oxide (LCO) cathodes is revealed by in situ differential electrochemical mass spectrometry.
3 Pouch cells equipped with high-loading LCO (3 mAh cm−2) cathodes, ultrathin Li chips (25 μm), and lean electrolytes (5 g Ah−1) using optimized electrolyte (FGN-182 + 1%HTCN) demonstrate outstanding cycling performance.

Keywords

Li metal anode Li dendrites LiNO3 1,3,6-tricyanohexane Pouch cells
You, Jinhai, Qiong Wang, Runhong Wei, Li Deng, Yiyang Hu, Li Niu, Jingkai Wang, Xiaomei Zheng, Junwei Li, Yao Zhou, and Jun‑Tao Li. 2024. “Boosting High-Voltage Practical Lithium Metal Batteries With Tailored Additives”. Nano-Micro Letters 16 (July):257. https://doi.org/10.1007/s40820-024-01479-1.
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