High rate and stable cycling of lithium metal anode
Abstract
Lithium (Li) metal is an ideal anode material for rechargeable batteries. However, dendritic Li growth and limited Coulombic efficiency (CE) during repeated Li deposition/stripping processes have prevented the application of this anode in rechargeable Li metal batteries, especially for use at high current densities. Here, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide (LiFSI) salt enables the high rate cycling of a Li metal anode at high CE (up to 99.1 %) without dendrite growth. With 4 M LiFSI in 1,2-dimethoxyethane (DME) as the electrolyte, a Li|Li cell can be cycled at high rates (10 mA cm-2) for more than 6000 cycles with no increase in the cell impedance, and a Cu|Li cell can be cycled at 4 mA cm-2 for more than 1000 cycles with an average CE of 98.4%. These excellent high rate performances can be attributed to the increased solvent coordination and increased availability of Li+ concentration in the electrolyte. Lastly, further development of this electrolyte may lead to practical applications for Li metal anode in rechargeable batteries. The fundamental mechanisms behind the high rate ion exchange and stability of the electrolytes also shine light on the stabilitymore »
- Authors:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- U.S. Army Research Lab., Adelphi, MD (United States). Sensor & Electron Devices Directorate
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1184948
- Report Number(s):
- PNNL-SA-107989
Journal ID: ISSN 2041-1723; 48379; 48316; KC0208010
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, and Zhang, Jiguang. High rate and stable cycling of lithium metal anode. United States: N. p., 2015.
Web. doi:10.1038/ncomms7362.
Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, & Zhang, Jiguang. High rate and stable cycling of lithium metal anode. United States. https://doi.org/10.1038/ncomms7362
Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, and Zhang, Jiguang. Fri .
"High rate and stable cycling of lithium metal anode". United States. https://doi.org/10.1038/ncomms7362. https://www.osti.gov/servlets/purl/1184948.
@article{osti_1184948,
title = {High rate and stable cycling of lithium metal anode},
author = {Qian, Jiangfeng and Henderson, Wesley A. and Xu, Wu and Bhattacharya, Priyanka and Engelhard, Mark H. and Borodin, Oleg and Zhang, Jiguang},
abstractNote = {Lithium (Li) metal is an ideal anode material for rechargeable batteries. However, dendritic Li growth and limited Coulombic efficiency (CE) during repeated Li deposition/stripping processes have prevented the application of this anode in rechargeable Li metal batteries, especially for use at high current densities. Here, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide (LiFSI) salt enables the high rate cycling of a Li metal anode at high CE (up to 99.1 %) without dendrite growth. With 4 M LiFSI in 1,2-dimethoxyethane (DME) as the electrolyte, a Li|Li cell can be cycled at high rates (10 mA cm-2) for more than 6000 cycles with no increase in the cell impedance, and a Cu|Li cell can be cycled at 4 mA cm-2 for more than 1000 cycles with an average CE of 98.4%. These excellent high rate performances can be attributed to the increased solvent coordination and increased availability of Li+ concentration in the electrolyte. Lastly, further development of this electrolyte may lead to practical applications for Li metal anode in rechargeable batteries. The fundamental mechanisms behind the high rate ion exchange and stability of the electrolytes also shine light on the stability of other electrochemical systems.},
doi = {10.1038/ncomms7362},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Fri Feb 20 00:00:00 EST 2015},
month = {Fri Feb 20 00:00:00 EST 2015}
}
Web of Science
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- Zhu, Bin; Wang, Xinyu; Yao, Pengcheng
- Chemical Science, Vol. 10, Issue 30
Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface
journal, April 2017
- Fu, Kun (Kelvin); Gong, Yunhui; Liu, Boyang
- Science Advances, Vol. 3, Issue 4
Composite lithium electrode with mesoscale skeleton via simple mechanical deformation
journal, March 2019
- Liang, Zheng; Yan, Kai; Zhou, Guangmin
- Science Advances, Vol. 5, Issue 3
Fluorinated solid electrolyte interphase enables highly reversible solid-state Li metal battery
journal, December 2018
- Fan, Xiulin; Ji, Xiao; Han, Fudong
- Science Advances, Vol. 4, Issue 12
Concentrated LiODFB Electrolyte for Lithium Metal Batteries
journal, July 2019
- Yu, Juan; Gao, Na; Peng, Jiaxin
- Frontiers in Chemistry, Vol. 7
The Effect of Concentration of Lithium Salt on the Structural and Transport Properties of Ionic Liquid-Based Electrolytes
journal, February 2020
- Tong, Jiahuan; Wu, Shengli; von Solms, Nicolas
- Frontiers in Chemistry, Vol. 7
Lithiophilic Silver Coating on Lithium Metal Surface for Inhibiting Lithium Dendrites
journal, February 2020
- Zuo, Zefu; Zhuang, Libin; Xu, Jinzhuo
- Frontiers in Chemistry, Vol. 8
Synergistic Effects of Salt Concentration and Working Temperature towards Dendrite-Free Lithium Deposition
journal, October 2019
- Li, Panlong; Li, Chao; Yang, Yang
- Research, Vol. 2019