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Title: Cyclic carbonate for highly stable cycling of high voltage lithium metal batteries

Abstract

The lithium metal battery (LMB) is one of the most promising next-generation battery systems due to its ultrahigh energy density. However, problematic dendrite formation and low Coulombic efficiency (CE) greatly limit its practical application. Carbonate electrolyte solvents are still indispensable for the operation of LMBs using a transition metal oxide cathode. We determined the impact of different cyclic carbonates, which actively participate in the formation of the solid-electrolyte interface (SEI), on the stable cycling of LMBs using a nickel-rich layered cathode LiN i0.6Mn 0.2Co 0.2O 2 (NMC622). The substitution of fluorine atoms in the cyclic carbonate profoundly enhances the stability of the lithium metal anode while fluoroalkyl and alkoxy substituents are detrimental. Cyclic carbonate trans-difluoroethylene carbonate (DFEC) was identified as a novel SEI enabler on the lithium metal anode, facilitating the formation of a protective SEI with relatively high lithium fluoride content. A Li/NMC622 cell utilizing DFEC electrolyte solvent as SEI enabler displayed a capacity retention larger than 82% after 400 cycles and an average CE of 99.95%. In contrast, the cycling retention after 400 cycles for a Li/NMC622 cell using monofluoroethylene carbonate was only 31% with an average CE of 99.73 %. Other fluoroalkyl or alkoxy cyclic carbonates domore » not provide improved stabilization of the lithium metal anode over ethylene carbonate. The fundamental studies in this work provide critical insight for the further development of advanced electrolytes in LMBs« less

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Stanford Univ., CA (United States). Dept. of Material Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1493894
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Energy Storage Materials
Additional Journal Information:
Journal Volume: 17; Journal Issue: C; Journal ID: ISSN 2405-8297
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrolyte optimization; fluorinated cyclic carbonates; high voltage electrolytes; lithium metal batteries; lithium stabilization

Citation Formats

Su, Chi-Cheung, He, Meinan, Amine, Rachid, Chen, Zonghai, Sahore, Ritu, Dietz Rago, Nancy, and Amine, Khalil. Cyclic carbonate for highly stable cycling of high voltage lithium metal batteries. United States: N. p., 2018. Web. doi:10.1016/j.ensm.2018.11.003.
Su, Chi-Cheung, He, Meinan, Amine, Rachid, Chen, Zonghai, Sahore, Ritu, Dietz Rago, Nancy, & Amine, Khalil. Cyclic carbonate for highly stable cycling of high voltage lithium metal batteries. United States. doi:10.1016/j.ensm.2018.11.003.
Su, Chi-Cheung, He, Meinan, Amine, Rachid, Chen, Zonghai, Sahore, Ritu, Dietz Rago, Nancy, and Amine, Khalil. Thu . "Cyclic carbonate for highly stable cycling of high voltage lithium metal batteries". United States. doi:10.1016/j.ensm.2018.11.003. https://www.osti.gov/servlets/purl/1493894.
@article{osti_1493894,
title = {Cyclic carbonate for highly stable cycling of high voltage lithium metal batteries},
author = {Su, Chi-Cheung and He, Meinan and Amine, Rachid and Chen, Zonghai and Sahore, Ritu and Dietz Rago, Nancy and Amine, Khalil},
abstractNote = {The lithium metal battery (LMB) is one of the most promising next-generation battery systems due to its ultrahigh energy density. However, problematic dendrite formation and low Coulombic efficiency (CE) greatly limit its practical application. Carbonate electrolyte solvents are still indispensable for the operation of LMBs using a transition metal oxide cathode. We determined the impact of different cyclic carbonates, which actively participate in the formation of the solid-electrolyte interface (SEI), on the stable cycling of LMBs using a nickel-rich layered cathode LiNi0.6Mn0.2Co0.2O2 (NMC622). The substitution of fluorine atoms in the cyclic carbonate profoundly enhances the stability of the lithium metal anode while fluoroalkyl and alkoxy substituents are detrimental. Cyclic carbonate trans-difluoroethylene carbonate (DFEC) was identified as a novel SEI enabler on the lithium metal anode, facilitating the formation of a protective SEI with relatively high lithium fluoride content. A Li/NMC622 cell utilizing DFEC electrolyte solvent as SEI enabler displayed a capacity retention larger than 82% after 400 cycles and an average CE of 99.95%. In contrast, the cycling retention after 400 cycles for a Li/NMC622 cell using monofluoroethylene carbonate was only 31% with an average CE of 99.73 %. Other fluoroalkyl or alkoxy cyclic carbonates do not provide improved stabilization of the lithium metal anode over ethylene carbonate. The fundamental studies in this work provide critical insight for the further development of advanced electrolytes in LMBs},
doi = {10.1016/j.ensm.2018.11.003},
journal = {Energy Storage Materials},
number = C,
volume = 17,
place = {United States},
year = {2018},
month = {11}
}

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