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Title: Stabilizing polymer electrolytes in high-voltage lithium batteries

Abstract

Electrochemical cells that utilize lithium and sodium anodes are under active study for their potential to enable high-energy batteries. Liquid and solid polymer electrolytes based on ether chemistry are among the most promising choices for rechargeable lithium and sodium batteries. However, uncontrolled anionic polymerization of these electrolytes at low anode potentials and oxidative degradation at working potentials of the most interesting cathode chemistries have led to a quite concession in the field that solid-state or flexible batteries based on polymer electrolytes can only be achieved in cells based on low- or moderate-voltage cathodes. Here, we show that cationic chain transfer agents can prevent degradation of ether electrolytes by arresting uncontrolled polymer growth at the anode. We also report that cathode electrolyte interphases composed of preformed anionic polymers and supramolecules provide a fundamental strategy for extending the high voltage stability of ether-based electrolytes to potentials well above conventionally accepted limits.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Cornell Univ., Ithaca, NY (United States)
  2. Florida State Univ., Tallahassee, FL (United States)
  3. Cornell Univ., Ithaca, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Beijing Institute of Collaboratory Innovation (BICI); Florida State University (FSU); State of Florida; Cornell Center for Materials Research (CCMR)
OSTI Identifier:
1624171
Grant/Contract Number:  
SC0001086; DMR-1609125; DMR-1644779; DMR-1654596; DMR-1719875
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Science & Technology - Other Topics

Citation Formats

Choudhury, Snehashis, Tu, Zhengyuan, Nijamudheen, A., Zachman, Michael J., Stalin, Sanjuna, Deng, Yue, Zhao, Qing, Vu, Duylinh, Kourkoutis, Lena F., Mendoza-Cortes, Jose L., and Archer, Lynden A. Stabilizing polymer electrolytes in high-voltage lithium batteries. United States: N. p., 2019. Web. https://doi.org/10.1038/s41467-019-11015-0.
Choudhury, Snehashis, Tu, Zhengyuan, Nijamudheen, A., Zachman, Michael J., Stalin, Sanjuna, Deng, Yue, Zhao, Qing, Vu, Duylinh, Kourkoutis, Lena F., Mendoza-Cortes, Jose L., & Archer, Lynden A. Stabilizing polymer electrolytes in high-voltage lithium batteries. United States. https://doi.org/10.1038/s41467-019-11015-0
Choudhury, Snehashis, Tu, Zhengyuan, Nijamudheen, A., Zachman, Michael J., Stalin, Sanjuna, Deng, Yue, Zhao, Qing, Vu, Duylinh, Kourkoutis, Lena F., Mendoza-Cortes, Jose L., and Archer, Lynden A. Fri . "Stabilizing polymer electrolytes in high-voltage lithium batteries". United States. https://doi.org/10.1038/s41467-019-11015-0. https://www.osti.gov/servlets/purl/1624171.
@article{osti_1624171,
title = {Stabilizing polymer electrolytes in high-voltage lithium batteries},
author = {Choudhury, Snehashis and Tu, Zhengyuan and Nijamudheen, A. and Zachman, Michael J. and Stalin, Sanjuna and Deng, Yue and Zhao, Qing and Vu, Duylinh and Kourkoutis, Lena F. and Mendoza-Cortes, Jose L. and Archer, Lynden A.},
abstractNote = {Electrochemical cells that utilize lithium and sodium anodes are under active study for their potential to enable high-energy batteries. Liquid and solid polymer electrolytes based on ether chemistry are among the most promising choices for rechargeable lithium and sodium batteries. However, uncontrolled anionic polymerization of these electrolytes at low anode potentials and oxidative degradation at working potentials of the most interesting cathode chemistries have led to a quite concession in the field that solid-state or flexible batteries based on polymer electrolytes can only be achieved in cells based on low- or moderate-voltage cathodes. Here, we show that cationic chain transfer agents can prevent degradation of ether electrolytes by arresting uncontrolled polymer growth at the anode. We also report that cathode electrolyte interphases composed of preformed anionic polymers and supramolecules provide a fundamental strategy for extending the high voltage stability of ether-based electrolytes to potentials well above conventionally accepted limits.},
doi = {10.1038/s41467-019-11015-0},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {7}
}

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