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Title: Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes

Abstract

Coupling thin Li metal anodes with high-capacity/high-voltage cathodes such as LiNi 0.8Co 0.1Mn 0.1O 2 (NCM811) is a promising way to increase lithium battery energy density. Yet, the realization of high-performance full cells remains a formidable challenge. Here, we demonstrate a new class of highly coordinated, nonflammable carbonate electrolytes based on lithium bis(fluorosulfonyl)imide (LiFSI) in propylene carbonate/fluoroethylene carbonate mixtures. Utilizing an optimal salt concentration (4 M LiFSI) of the electrolyte results in a unique coordination structure of Li +-FSI --solvent cluster, which is critical for enabling the formation of stable interfaces on both the thin Li metal anode and high-voltage NCM811 cathode. Under highly demanding cell configuration and operating conditions (Li metal anode = 35 μm, areal capacity/charge voltage of NCM811 cathode = 4.8 mAh cm -2/4.6 V, and anode excess capacity [relative to the cathode] = 0.83), the Li metal-based full cell provides exceptional electrochemical performance (energy densities = 679 Wh kg cell -1/1,024 Wh L cell -1) coupled with nonflammability.

Authors:
 [1];  [1];  [2];  [1];  [3];  [2];  [1]
  1. Ulsan National Institute of Science and Technology, Ulsan (Korea, Republic of). School of Energy and Chemical Engineering. Dept. of Energy Engineering
  2. Army Research Lab., Adelphi, MD (United States). Sensor and Electron Devices Directorate. Energy and Biomaterials Division. Battery Science Branch
  3. LG Chem., Daejeon (Korea, Republic of). Battery R&D Center
Publication Date:
Research Org.:
Army Research Lab., Adelphi, MD (United States). Sensor and Electron Devices Directorate. Energy and Biomaterials Division. Battery Science Branch
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1623688
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
iScience
Additional Journal Information:
Journal Volume: 23; Journal Issue: 2; Journal ID: ISSN 2589-0042
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Science & Technology - Other Topics

Citation Formats

Cho, Sung-Ju, Yu, Dae-Eun, Pollard, Travis P., Moon, Hyunseok, Jang, Minchul, Borodin, Oleg, and Lee, Sang-Young. Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes. United States: N. p., 2020. Web. doi:10.1016/j.isci.2020.100844.
Cho, Sung-Ju, Yu, Dae-Eun, Pollard, Travis P., Moon, Hyunseok, Jang, Minchul, Borodin, Oleg, & Lee, Sang-Young. Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes. United States. doi:10.1016/j.isci.2020.100844.
Cho, Sung-Ju, Yu, Dae-Eun, Pollard, Travis P., Moon, Hyunseok, Jang, Minchul, Borodin, Oleg, and Lee, Sang-Young. Sat . "Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes". United States. doi:10.1016/j.isci.2020.100844. https://www.osti.gov/servlets/purl/1623688.
@article{osti_1623688,
title = {Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes},
author = {Cho, Sung-Ju and Yu, Dae-Eun and Pollard, Travis P. and Moon, Hyunseok and Jang, Minchul and Borodin, Oleg and Lee, Sang-Young},
abstractNote = {Coupling thin Li metal anodes with high-capacity/high-voltage cathodes such as LiNi0.8Co0.1Mn0.1O2 (NCM811) is a promising way to increase lithium battery energy density. Yet, the realization of high-performance full cells remains a formidable challenge. Here, we demonstrate a new class of highly coordinated, nonflammable carbonate electrolytes based on lithium bis(fluorosulfonyl)imide (LiFSI) in propylene carbonate/fluoroethylene carbonate mixtures. Utilizing an optimal salt concentration (4 M LiFSI) of the electrolyte results in a unique coordination structure of Li+-FSI--solvent cluster, which is critical for enabling the formation of stable interfaces on both the thin Li metal anode and high-voltage NCM811 cathode. Under highly demanding cell configuration and operating conditions (Li metal anode = 35 μm, areal capacity/charge voltage of NCM811 cathode = 4.8 mAh cm-2/4.6 V, and anode excess capacity [relative to the cathode] = 0.83), the Li metal-based full cell provides exceptional electrochemical performance (energy densities = 679 Wh kgcell-1/1,024 Wh Lcell-1) coupled with nonflammability.},
doi = {10.1016/j.isci.2020.100844},
journal = {iScience},
issn = {2589-0042},
number = 2,
volume = 23,
place = {United States},
year = {2020},
month = {2}
}

Journal Article:
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