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

Sung Ju Cho; Dae Eun Yu; Travis P. Pollard; Hyunseok Moon; Minchul Jang; Oleg Borodin; Sang Young Lee

doi:10.1016/j.isci.2020.100844

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

Sung Ju Cho, Dae Eun Yu, Travis P. Pollard, Hyunseok Moon, Minchul Jang, Oleg Borodin, Sang Young Lee

Department of Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

51 Citations (Scopus)

Abstract

Coupling thin Li metal anodes with high-capacity/high-voltage cathodes such as LiNi_0.8Co_0.1Mn_0.1O₂ (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 kg_cell ⁻¹/1,024 Wh L_cell ⁻¹) coupled with nonflammability.

Original language	English
Article number	100844
Journal	iScience
Volume	23
Issue number	2
DOIs	https://doi.org/10.1016/j.isci.2020.100844
Publication status	Published - 2020 Feb 21

Bibliographical note

Funding Information:
This work was supported by US Army Research Office (ARO) ( W911NF-18-1-0016 ), Basic Science Research Program ( 2017M1A2A2087810 , 2018R1A2A1A05019733 , 2018M3D1A1058624 , and 2019R1I1A1A0144168 ), Wearable Platform Materials Technology Center ( 2016R1A5A1009926 ) through a National Research Foundation of Korea (NRF) grant by the Korean Government ( MSIT ), and Corporate R&D of LG Chem. The computation modeling work at ARL was supported by a Department of Energy Program (Peter Faguy).

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© 2020 The Author(s)

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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 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.",

author = "Cho, {Sung Ju} and Yu, {Dae Eun} and Pollard, {Travis P.} and Hyunseok Moon and Minchul Jang and Oleg Borodin and Lee, {Sang Young}",

note = "Funding Information: This work was supported by US Army Research Office (ARO) ( W911NF-18-1-0016 ), Basic Science Research Program ( 2017M1A2A2087810 , 2018R1A2A1A05019733 , 2018M3D1A1058624 , and 2019R1I1A1A0144168 ), Wearable Platform Materials Technology Center ( 2016R1A5A1009926 ) through a National Research Foundation of Korea (NRF) grant by the Korean Government ( MSIT ), and Corporate R&D of LG Chem. The computation modeling work at ARL was supported by a Department of Energy Program (Peter Faguy). Publisher Copyright: {\textcopyright} 2020 The Author(s)",

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AU - Moon, Hyunseok

AU - Jang, Minchul

AU - Borodin, Oleg

AU - Lee, Sang Young

N1 - Funding Information: This work was supported by US Army Research Office (ARO) ( W911NF-18-1-0016 ), Basic Science Research Program ( 2017M1A2A2087810 , 2018R1A2A1A05019733 , 2018M3D1A1058624 , and 2019R1I1A1A0144168 ), Wearable Platform Materials Technology Center ( 2016R1A5A1009926 ) through a National Research Foundation of Korea (NRF) grant by the Korean Government ( MSIT ), and Corporate R&D of LG Chem. The computation modeling work at ARL was supported by a Department of Energy Program (Peter Faguy). Publisher Copyright: © 2020 The Author(s)

PY - 2020/2/21

Y1 - 2020/2/21

N2 - 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.

AB - 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.

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

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