High-Efficiency Lithium Metal Anode Enabled by a Concentrated/Fluorinated Ester Electrolyte

Lithium (Li) metal anode (LMA) has received growing attention due to its highest theoretical capacity (3860 mA h g-1) and the lowest redox potential (-3.04 V versus standard hydrogen electrode). However, the practical application of LMA is obstructed by the detrimental side reactions between Li meta...

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Veröffentlicht in:ACS applied materials & interfaces 2020-06, Vol.12 (24), p.27794-27802
Hauptverfasser: Chen, Shijian, Xiang, Yuxuan, Zheng, Guorui, Liao, Ying, Ren, Fucheng, Zheng, Yezhen, He, Huajin, Zheng, Bizhu, Liu, Xiangsi, Xu, Ningbo, Luo, Mingzeng, Zheng, Jianming, Yang, Yong
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container_issue 24
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container_title ACS applied materials & interfaces
container_volume 12
creator Chen, Shijian
Xiang, Yuxuan
Zheng, Guorui
Liao, Ying
Ren, Fucheng
Zheng, Yezhen
He, Huajin
Zheng, Bizhu
Liu, Xiangsi
Xu, Ningbo
Luo, Mingzeng
Zheng, Jianming
Yang, Yong
description Lithium (Li) metal anode (LMA) has received growing attention due to its highest theoretical capacity (3860 mA h g-1) and the lowest redox potential (-3.04 V versus standard hydrogen electrode). However, the practical application of LMA is obstructed by the detrimental side reactions between Li metal and organic electrolytes, especially when cycled in traditional carbonate ester electrolytes. Herein, we propose a novel fluorinated carbonate ester-based electrolyte by combining diethyl fluorocarbonate (ETFEC) solvent and 5 M high LiFSI concentration (M=mol L-1). Using this electrolyte, an ultra-high Li plating/stripping Coulombic efficiency (CE) of 99.1% can be obtained in Li||Cu cells and a stable cycle performance of Li||LiFePO4 is achieved under the conditions of limited Li metal (5 mA h cm-2), moderate loading LiFePO4 (7~8 mg cm-2) and lean electrolyte (40 uL). The fundamental functioning mechanism of this novel electrolyte has been carefully investigated by scanning electronic microscopy (SEM), operando optical microscopy (OM), electrochemical impedance spectroscopy (EIS), X-ray photoelectron spectroscopy (XPS) and solid state nuclear magnetic resonance (SS-NMR). The results demonstrate that this optimized electrolyte facilitates the formation of a high Li+ conductive SEI layer enriched with LiF and inorganic sulfur-containing species, which can effectively suppress the side reactions between electrolyte and Li metal and prevent the formation of dead Li.
doi_str_mv 10.1021/acsami.0c06930
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However, the practical application of LMA is obstructed by the detrimental side reactions between Li metal and organic electrolytes, especially when cycled in traditional carbonate ester electrolytes. Herein, we propose a novel fluorinated carbonate ester-based electrolyte by combining diethyl fluorocarbonate (ETFEC) solvent and 5 M high LiFSI concentration (M=mol L-1). Using this electrolyte, an ultra-high Li plating/stripping Coulombic efficiency (CE) of 99.1% can be obtained in Li||Cu cells and a stable cycle performance of Li||LiFePO4 is achieved under the conditions of limited Li metal (5 mA h cm-2), moderate loading LiFePO4 (7~8 mg cm-2) and lean electrolyte (40 uL). The fundamental functioning mechanism of this novel electrolyte has been carefully investigated by scanning electronic microscopy (SEM), operando optical microscopy (OM), electrochemical impedance spectroscopy (EIS), X-ray photoelectron spectroscopy (XPS) and solid state nuclear magnetic resonance (SS-NMR). 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