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Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries

Hou, Xu LU orcid ; Pollard, Travis P. ; Zhao, Wenguang ; He, Xin ; Ju, Xiaokang ; Wang, Jun ; Du, Leilei ; Paillard, Elie ; Lin, Hai and Xu, Kang , et al. (2022) In Small 18(5).
Abstract

The formation of solid-electrolyte interphase (SEI) in “water-in-salt” electrolyte (WiSE) expands the electrochemical stability window of aqueous electrolytes beyond 3.0 V. However, the parasitic hydrogen evolution reaction that drives anode corrosion, cracking, and the subsequent reformation of SEI still occurs, compromising long-term cycling performance of the batteries. To improve cycling stability, an unsaturated monomer acrylamide (AM) is introduced as an electrolyte additive, whose presence in WiSE reduces its viscosity and improves ionic conductivity. Upon charging, AM electropolymerizes into polyacrylamide, as confirmed both experimentally and computationally. The in situ polymer constitutes effective protection layers at both... (More)

The formation of solid-electrolyte interphase (SEI) in “water-in-salt” electrolyte (WiSE) expands the electrochemical stability window of aqueous electrolytes beyond 3.0 V. However, the parasitic hydrogen evolution reaction that drives anode corrosion, cracking, and the subsequent reformation of SEI still occurs, compromising long-term cycling performance of the batteries. To improve cycling stability, an unsaturated monomer acrylamide (AM) is introduced as an electrolyte additive, whose presence in WiSE reduces its viscosity and improves ionic conductivity. Upon charging, AM electropolymerizes into polyacrylamide, as confirmed both experimentally and computationally. The in situ polymer constitutes effective protection layers at both anode and cathode surfaces, and enables LiMn2O4||L-TiO2 full cells with high specific capacity (157 mAh g−1 at 1 C), long-term cycling stability (80% capacity retention within 200 cycles at 1 C), and high rate capability (79 mAh g−1 at 30 C). The in situ electropolymerization found in this work provides an alternative and highly effective strategy to design protective interphases at the negative and positive electrodes for high-voltage aqueous batteries of lithium-ion or beyond.

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publishing date
type
Contribution to journal
publication status
published
in
Small
volume
18
issue
5
article number
2104986
publisher
John Wiley & Sons Inc.
external identifiers
  • pmid:34850544
  • scopus:85124056901
ISSN
1613-6810
DOI
10.1002/smll.202104986
language
English
LU publication?
no
additional info
Publisher Copyright: © 2021 The Authors. Small published by Wiley-VCH GmbH
id
a6bc71ad-768d-44e6-836f-e0ac2c3c861e
date added to LUP
2025-12-05 22:34:39
date last changed
2026-01-03 09:00:55
@article{a6bc71ad-768d-44e6-836f-e0ac2c3c861e,
  abstract     = {{<p>The formation of solid-electrolyte interphase (SEI) in “water-in-salt” electrolyte (WiSE) expands the electrochemical stability window of aqueous electrolytes beyond 3.0 V. However, the parasitic hydrogen evolution reaction that drives anode corrosion, cracking, and the subsequent reformation of SEI still occurs, compromising long-term cycling performance of the batteries. To improve cycling stability, an unsaturated monomer acrylamide (AM) is introduced as an electrolyte additive, whose presence in WiSE reduces its viscosity and improves ionic conductivity. Upon charging, AM electropolymerizes into polyacrylamide, as confirmed both experimentally and computationally. The in situ polymer constitutes effective protection layers at both anode and cathode surfaces, and enables LiMn<sub>2</sub>O<sub>4</sub>||L-TiO<sub>2</sub> full cells with high specific capacity (157 mAh g<sup>−1</sup> at 1 C), long-term cycling stability (80% capacity retention within 200 cycles at 1 C), and high rate capability (79 mAh g<sup>−1</sup> at 30 C). The in situ electropolymerization found in this work provides an alternative and highly effective strategy to design protective interphases at the negative and positive electrodes for high-voltage aqueous batteries of lithium-ion or beyond.</p>}},
  author       = {{Hou, Xu and Pollard, Travis P. and Zhao, Wenguang and He, Xin and Ju, Xiaokang and Wang, Jun and Du, Leilei and Paillard, Elie and Lin, Hai and Xu, Kang and Borodin, Oleg and Winter, Martin and Li, Jie}},
  issn         = {{1613-6810}},
  language     = {{eng}},
  month        = {{02}},
  number       = {{5}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Small}},
  title        = {{Simultaneous Formation of Interphases on both Positive and Negative Electrodes in High-Voltage Aqueous Lithium-Ion Batteries}},
  url          = {{http://dx.doi.org/10.1002/smll.202104986}},
  doi          = {{10.1002/smll.202104986}},
  volume       = {{18}},
  year         = {{2022}},
}