Stabilizing polymer electrolytes in high-voltage lithium batteries

Snehashis Choudhury; Zhengyuan Tu; A. Nijamudheen; Michael J. Zachman; Sanjuna Stalin; Yue Deng; Qing Zhao; Duylinh Vu; Lena F. Kourkoutis; Jose L. Mendoza-Cortes; Lynden A. Archer

doi:10.1038/s41467-019-11015-0

Stabilizing polymer electrolytes in high-voltage lithium batteries

Snehashis Choudhury, Zhengyuan Tu, A. Nijamudheen, Michael J. Zachman, Sanjuna Stalin, Yue Deng, Qing Zhao, Duylinh Vu, Lena F. Kourkoutis, Jose L. Mendoza-Cortes, Lynden A. Archer

electron Microscopy and Microanalysis

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

114 Scopus citations

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.

Original language	English
Article number	3091
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-11015-0
State	Published - Dec 1 2019

Funding

The work was supported by the National Science Foundation, Division of Materials Research, through Award No. DMR-1609125. S.C., S.S. and Q.Z. acknowledge partial support from the Beijing Institute of Collaboratory Innovation (BICI). J.L.M.-C. and A. N. thank the High-Performance Computer cluster at the Research Computing Center (RCC) in Florida State University (FSU) for providing computational resources and support. J.L.M.-C. gratefully acknowledges the support from the Energy and Materials Initiative at FSU. A portion of this work was performed at the National High Magnetic Field Laboratory, which is supported by National Science Foundation Cooperative Agreement No. DMR-1644779 and the State of Florida. M.J.Z. and L.F.K. acknowledge support by the NSF (DMR-1654596). This work made use of the Cornell Center for Materials Research (CCMR) Shared Facilities with funding from the NSF MRSEC program (DMR-1719875). Additional support for the FIB/SEM cryo-stage and transfer system was provided by the Kavli Institute at Cornell and the Energy Materials Center at Cornell, DOE EFRC BES (DE-SC0001086).

Funders	Funder number
Beijing Institute of Collaboratory Innovation
DOE EFRC BES	DE-SC0001086
Kavli Institute at Cornell
State of Florida
National Science Foundation	DMR-1644779, DMR-1654596
National Science Foundation
Division of Materials Research	DMR-1609125
Division of Materials Research
Florida State University
Materials Research Science and Engineering Center, Harvard University	DMR-1719875
Materials Research Science and Engineering Center, Harvard University

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10.1038/s41467-019-11015-0

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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.",

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AU - Deng, Yue

AU - Zhao, Qing

AU - Vu, Duylinh

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AB - 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.

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Stabilizing polymer electrolytes in high-voltage lithium batteries

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