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Stabilizing the Solid-Electrolyte Interphase with Polyacrylamide for High-Voltage Aqueous Lithium-Ion Batteries

Hou, Xu LU orcid ; Wang, Rui ; He, Xin ; Pollard, Travis P. ; Ju, Xiaokang ; Du, Leilei ; Paillard, Elie ; Frielinghaus, Henrich ; Barnsley, Lester C. and Borodin, Oleg , et al. (2021) In Angewandte Chemie - International Edition 60(42). p.22812-22817
Abstract

The introduction of “water-in-salt” electrolyte (WiSE) concept opens a new horizon to aqueous electrochemistry that is benefited from the formation of a solid-electrolyte interphase (SEI). However, such SEI still faces multiple challenges, including dissolution, mechanical damaging, and incessant reforming, which result in poor cycling stability. Here, we report a polymeric additive, polyacrylamide (PAM) that effectively stabilizes the interphase in WiSE. With the addition of 5 molar % PAM to 21 mol kg−1 LiTFSI electrolyte, a LiMn2O4∥L-TiO2 full cell exhibits enhanced cycling stability with 86 % capacity retention after 100 cycles at 1 C. The formation mechanism and evolution of PAM-assisted... (More)

The introduction of “water-in-salt” electrolyte (WiSE) concept opens a new horizon to aqueous electrochemistry that is benefited from the formation of a solid-electrolyte interphase (SEI). However, such SEI still faces multiple challenges, including dissolution, mechanical damaging, and incessant reforming, which result in poor cycling stability. Here, we report a polymeric additive, polyacrylamide (PAM) that effectively stabilizes the interphase in WiSE. With the addition of 5 molar % PAM to 21 mol kg−1 LiTFSI electrolyte, a LiMn2O4∥L-TiO2 full cell exhibits enhanced cycling stability with 86 % capacity retention after 100 cycles at 1 C. The formation mechanism and evolution of PAM-assisted SEI was investigated using operando small angle neutron scattering and density functional theory (DFT) calculations, which reveal that PAM minimizes the presence of free water molecules at the anode/electrolyte interface, accelerates the TFSI− anion decomposition, and densifies the SEI.

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publishing date
type
Contribution to journal
publication status
published
keywords
lithium-ion batteries, polymer additive, small-angle neutron scattering, solid-electrolyte interphase, “water-in-salt” electrolyte
in
Angewandte Chemie - International Edition
volume
60
issue
42
pages
6 pages
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85114685729
  • pmid:34379346
ISSN
1433-7851
DOI
10.1002/anie.202107252
language
English
LU publication?
no
additional info
Publisher Copyright: © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
id
ed857b9d-4f42-4680-8ca0-8ee71146aad8
date added to LUP
2025-12-05 22:35:15
date last changed
2025-12-12 03:52:31
@article{ed857b9d-4f42-4680-8ca0-8ee71146aad8,
  abstract     = {{<p>The introduction of “water-in-salt” electrolyte (WiSE) concept opens a new horizon to aqueous electrochemistry that is benefited from the formation of a solid-electrolyte interphase (SEI). However, such SEI still faces multiple challenges, including dissolution, mechanical damaging, and incessant reforming, which result in poor cycling stability. Here, we report a polymeric additive, polyacrylamide (PAM) that effectively stabilizes the interphase in WiSE. With the addition of 5 molar % PAM to 21 mol kg<sup>−1</sup> LiTFSI electrolyte, a LiMn<sub>2</sub>O<sub>4</sub>∥L-TiO<sub>2</sub> full cell exhibits enhanced cycling stability with 86 % capacity retention after 100 cycles at 1 C. The formation mechanism and evolution of PAM-assisted SEI was investigated using operando small angle neutron scattering and density functional theory (DFT) calculations, which reveal that PAM minimizes the presence of free water molecules at the anode/electrolyte interface, accelerates the TFSI<sup>−</sup> anion decomposition, and densifies the SEI.</p>}},
  author       = {{Hou, Xu and Wang, Rui and He, Xin and Pollard, Travis P. and Ju, Xiaokang and Du, Leilei and Paillard, Elie and Frielinghaus, Henrich and Barnsley, Lester C. and Borodin, Oleg and Xu, Kang and Winter, Martin and Li, Jie}},
  issn         = {{1433-7851}},
  keywords     = {{lithium-ion batteries; polymer additive; small-angle neutron scattering; solid-electrolyte interphase; “water-in-salt” electrolyte}},
  language     = {{eng}},
  month        = {{10}},
  number       = {{42}},
  pages        = {{22812--22817}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Angewandte Chemie - International Edition}},
  title        = {{Stabilizing the Solid-Electrolyte Interphase with Polyacrylamide for High-Voltage Aqueous Lithium-Ion Batteries}},
  url          = {{http://dx.doi.org/10.1002/anie.202107252}},
  doi          = {{10.1002/anie.202107252}},
  volume       = {{60}},
  year         = {{2021}},
}