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Title: A Localized High-Concentration Electrolyte with Optimized Solvents and Lithium Difluoro(oxalate)borate Additive for Stable Lithium Metal Batteries

Abstract

Lithium (Li) metal is considered as the ideal anode for high energy density rechargeable Li metal batteries (LMBs). However, the morphology instability of Li anode during electrochemical deposition/stripping leads to the uncontrolled growth of dendrites and the solid electrolyte interphase (SEI) layer which causes low Li Coulombic efficiency (CE) and rapid capacity fading in LMBs. Here, we report a carbonate-based localized high concentration electrolyte (LHCE) with a fluorinated ether as a diluent for 4-V class LMBs. This electrolyte consists of 1.2 M lithium bis(fluorosulfonyl)imide (LiFSI) in a co-solvent mixture of ethylene carbonate (EC)/ethyl methyl carbonate (EMC) with bis(2,2,2-trifluoroethyl) ether (BTFE) as diluent and 0.15 M lithium difluoro(oxalate)borate (LiDFOB) as additive. Using this electrolyte, dendrites-free Li deposition with a high Li CE (~98.5 %) is achieved. In addition, it offers much improved cycling stability of Li metal anode compared to previously reported dimethyl carbonate-based LHCEs. For example, a Li||NMC333 battery with a high areal loading of 3.8 mAh cm-2 maintains 84% of its initial capacity after 100 cycles. This is likely due to the highly robust SEI layer formed on the Li metal anode because of the decomposition of LiDFOB salt and EC solvent molecules. Therefore this novel electrolyte is promisingmore » for high energy density rechargeable LMBs.« less

Authors:
 [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [3];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, Washington 99354, United States
  2. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, Washington 99354, United States; Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei, Anhui 230026, People’s Republic of China
  3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 3335 Innovation Boulevard, Richland, Washington 99354, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1489905
Report Number(s):
PNNL-SA-134778
Journal ID: ISSN 2380-8195
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
lithium, lithium metal batteries, cycling stability

Citation Formats

Yu, Lu, Chen, Shuru, Lee, Hongkyung, Zhang, Linchao, Engelhard, Mark H., Li, Qiuyan, Jiao, Shuhong, Liu, Jun, Xu, Wu, and Zhang, Ji-Guang. A Localized High-Concentration Electrolyte with Optimized Solvents and Lithium Difluoro(oxalate)borate Additive for Stable Lithium Metal Batteries. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b00935.
Yu, Lu, Chen, Shuru, Lee, Hongkyung, Zhang, Linchao, Engelhard, Mark H., Li, Qiuyan, Jiao, Shuhong, Liu, Jun, Xu, Wu, & Zhang, Ji-Guang. A Localized High-Concentration Electrolyte with Optimized Solvents and Lithium Difluoro(oxalate)borate Additive for Stable Lithium Metal Batteries. United States. https://doi.org/10.1021/acsenergylett.8b00935
Yu, Lu, Chen, Shuru, Lee, Hongkyung, Zhang, Linchao, Engelhard, Mark H., Li, Qiuyan, Jiao, Shuhong, Liu, Jun, Xu, Wu, and Zhang, Ji-Guang. Tue . "A Localized High-Concentration Electrolyte with Optimized Solvents and Lithium Difluoro(oxalate)borate Additive for Stable Lithium Metal Batteries". United States. https://doi.org/10.1021/acsenergylett.8b00935.
@article{osti_1489905,
title = {A Localized High-Concentration Electrolyte with Optimized Solvents and Lithium Difluoro(oxalate)borate Additive for Stable Lithium Metal Batteries},
author = {Yu, Lu and Chen, Shuru and Lee, Hongkyung and Zhang, Linchao and Engelhard, Mark H. and Li, Qiuyan and Jiao, Shuhong and Liu, Jun and Xu, Wu and Zhang, Ji-Guang},
abstractNote = {Lithium (Li) metal is considered as the ideal anode for high energy density rechargeable Li metal batteries (LMBs). However, the morphology instability of Li anode during electrochemical deposition/stripping leads to the uncontrolled growth of dendrites and the solid electrolyte interphase (SEI) layer which causes low Li Coulombic efficiency (CE) and rapid capacity fading in LMBs. Here, we report a carbonate-based localized high concentration electrolyte (LHCE) with a fluorinated ether as a diluent for 4-V class LMBs. This electrolyte consists of 1.2 M lithium bis(fluorosulfonyl)imide (LiFSI) in a co-solvent mixture of ethylene carbonate (EC)/ethyl methyl carbonate (EMC) with bis(2,2,2-trifluoroethyl) ether (BTFE) as diluent and 0.15 M lithium difluoro(oxalate)borate (LiDFOB) as additive. Using this electrolyte, dendrites-free Li deposition with a high Li CE (~98.5 %) is achieved. In addition, it offers much improved cycling stability of Li metal anode compared to previously reported dimethyl carbonate-based LHCEs. For example, a Li||NMC333 battery with a high areal loading of 3.8 mAh cm-2 maintains 84% of its initial capacity after 100 cycles. This is likely due to the highly robust SEI layer formed on the Li metal anode because of the decomposition of LiDFOB salt and EC solvent molecules. Therefore this novel electrolyte is promising for high energy density rechargeable LMBs.},
doi = {10.1021/acsenergylett.8b00935},
url = {https://www.osti.gov/biblio/1489905}, journal = {ACS Energy Letters},
issn = {2380-8195},
number = 9,
volume = 3,
place = {United States},
year = {2018},
month = {7}
}