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Title: 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 » of other electrochemical systems.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [1]
+ Show Author Affiliations
  1. 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
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  4. 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.
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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
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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.
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@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}
}
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https://doi.org/10.1038/ncomms7362
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    journal, November 2015

    Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy
    journal, October 2016

    High-Purity Lithium Metal Films from Aqueous Mineral Solutions
    journal, January 2018

    A reversible dendrite-free high-areal-capacity lithium metal electrode
    journal, April 2017

    • Wang, Hui; Matsui, Masaki; Kuwata, Hiroko
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15106

    Accommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes
    journal, August 2015

    • Yang, Chun-Peng; Yin, Ya-Xia; Zhang, Shuai-Feng
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms9058

    Designing solid-liquid interphases for sodium batteries
    journal, October 2017

    Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode
    journal, September 2018

    High-energy-density dual-ion battery for stationary storage of electricity using concentrated potassium fluorosulfonylimide
    journal, October 2018

    • Kravchyk, Kostiantyn V.; Bhauriyal, Preeti; Piveteau, Laura
    • Nature Communications, Vol. 9, Issue 1
    • DOI: 10.1038/s41467-018-06923-6

    Achieving three-dimensional lithium sulfide growth in lithium-sulfur batteries using high-donor-number anions
    journal, January 2019

    Publisher Correction: Aligning academia and industry for unified battery performance metrics
    journal, January 2019

    Stabilizing polymer electrolytes in high-voltage lithium batteries
    journal, July 2019

    A new ether-based electrolyte for dendrite-free lithium-metal based rechargeable batteries
    journal, February 2016

    • Miao, Rongrong; Yang, Jun; Xu, Zhixin
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep21771

    Structural modulation of lithium metal-electrolyte interface with three-dimensional metallic interlayer for high-performance lithium metal batteries
    journal, August 2016

    • Lee, Hongkyung; Song, Jongchan; Kim, Yun-Jung
    • Scientific Reports, Vol. 6, Issue 1
    • DOI: 10.1038/srep30830

    Towards high energy density lithium battery anodes: silicon and lithium
    journal, January 2019

    • Zhu, Bin; Wang, Xinyu; Yao, Pengcheng
    • Chemical Science, Vol. 10, Issue 30
    • DOI: 10.1039/c9sc01201j

    Composite lithium electrode with mesoscale skeleton via simple mechanical deformation
    journal, March 2019

    Fluorinated solid electrolyte interphase enables highly reversible solid-state Li metal battery
    journal, December 2018

    Concentrated LiODFB Electrolyte for Lithium Metal Batteries
    journal, July 2019

    The Effect of Concentration of Lithium Salt on the Structural and Transport Properties of Ionic Liquid-Based Electrolytes
    journal, February 2020

    Lithiophilic Silver Coating on Lithium Metal Surface for Inhibiting Lithium Dendrites
    journal, February 2020

    Synergistic Effects of Salt Concentration and Working Temperature towards Dendrite-Free Lithium Deposition
    journal, October 2019

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