# Gel Polymer Electrolytes Based on Poly(vinylidene fluoride-<i>co</i>-hexafluoropropylene) and Salt-Concentrated Electrolytes for High-Voltage Lithium Metal Batteries

https://mdr.nims.go.jp/datasets/68fbd48d-b10e-4957-973f-4af4b72e60eb

## File

- [241018_MS_LiFSA-SL_PVDF-HFP_HVLMB_EndNote_ACSAPM.pdf](https://mdr.nims.go.jp/filesets/f19da965-737b-4807-9ab5-5fb154eac417/download) ([Detail](https://mdr.nims.go.jp/filesets/f19da965-737b-4807-9ab5-5fb154eac417.md))

## Id

68fbd48d-b10e-4957-973f-4af4b72e60eb

## Local identifier



## Visibility

open_to_public

## State

published

## Created at

2025-12-10T05:19:03.727392Z

## Updated at

2025-12-10T23:30:10.057747Z

## Published at

2025-12-10T23:24:20.370562Z

## Doi

https://doi.org/10.48505/nims.5989

## First published url

https://doi.org/10.1021/acsapm.4c03396

## Date published

2025-02-14

## Recorded date published

2025-2-14

## Resource type

journal_article

## Manuscript type

authors_original

## Collection



## Title

- title: Gel Polymer Electrolytes Based on Poly(vinylidene fluoride-<i>co</i>-hexafluoropropylene)
    and Salt-Concentrated Electrolytes for High-Voltage Lithium Metal Batteries
  title_type: original
  lang: en

## Description

- description: Although high-voltage lithium (Li) metal batteries are promising next-generation
    energy storage devices, their practical use is hindered by their poor cycling
    stability owing to low electrolyte compatibility with both Li metal anodes and
    5 Vclass cathodes. In this study, we report that the gelation of saltconcentrated
    electrolytes with weakly coordinating poly(vinylidene fluoride-co-hexafluoropropylene)
    (PVDF-HFP) effectively improves the cycling stability of high-voltage Li metal
    batteries. The PVDF-HFP-based gel polymer electrolyte with a saltconcentrated
    electrolyte comprising lithium bis(fluorosulfonyl)-amide (LiFSA) and sulfolane
    (SL) achieves a high Coulombic efficiency and dense deposition morphology of Li
    metal anodes, along with sufficient oxidation stability against 5 V-class cathodes.
    Experimental and computational analyses show that the solvation structures of
    SL−Li+−FSA−, similar to those in the original concentrated electrolyte, are maintained
    in the PVDF-HFP matrix, which leads to the formation of a low-resistance solid
    electrolyte interphase (SEI) rich in lithium fluoride and sulfur compounds. These
    findings indicate that the low-resistance SEI in the gel polymer electrolyte promotes
    dense Li deposits, which suppresses electrolyte decomposition and inactive Li
    formation, improving the Coulombic efficiency of Li metal anodes. We demonstrate
    that the stable cycling of a Li metal battery with a 5 V-class LiNi0.5Mn1.5O4
    cathode is enabled by the gel electrolyte, which inhibits the deposition of transition
    metals dissolved from the cathode onto the anode. This electrolyte and interface
    design is an effective strategy for developing 5 V-class Li metal batteries and
    can be applied to other high-energy-density metal batteries with high-voltage
    cathodes.
  description_type: abstract
  lang: und

## Creator

- name: Yuta Maeyoshi
  role: author
  orcid: https://orcid.org/0000-0002-4612-8283
- name: Kazuki Yoshii
  role: author
  orcid: https://orcid.org/0000-0001-8904-6790
- name: Hikaru Sano
  role: author
  orcid: https://orcid.org/0000-0002-7557-0767
- name: Hikari Sakaebe
  role: author
- name: Ryota Tamate
  role: author
  orcid: https://orcid.org/0000-0002-1704-1058
- name: Tomoaki Kaneko
  role: author
- name: Keitaro Sodeyama
  role: author
  orcid: https://orcid.org/0000-0002-9228-0729

## Contact agent



## Publisher

organization: American Chemical Society (ACS)

## Managing organization



## Keyword

- subject: Gel Polymer Electrolytes
  schema: not_defined
- subject: Salt-Concentrated Electrolytes
  schema: not_defined
- subject: Lithium Metal Batteries
  schema: not_defined

## Rights

- description: This document is the unedited Author’s version of a Submitted Work
    that was subsequently accepted for publication in ACS Applied Polymer Materials,
    copyright © 2025 American Chemical Society after peer review. To access the final
    edited and published work see https://doi.org/10.1021/acsapm.4c03396.
  identifier: http://rightsstatements.org/vocab/InC/1.0/

## Other identifier(s)



## Data origin



## Embargo



## Journal

- title: ACS Applied Polymer Materials
  issn: '26376105'
  volume: '7'
  issue: '3'
  start_page: 1629
  end_page: 1638

## Conference



## Related item



## Funding

- identifier: JP21K14731
  funder_name: Japan Society for the Promotion of Science
- identifier: JP22H04626
  funder_name: Japan Society for the Promotion of Science
- identifier: JP23K13833
  funder_name: Japan Society for the Promotion of Science
- identifier: '0331058-A'
  funder_name: Iketani Science and Technology Foundation
- identifier: JPMJGX23S3
  funder_name: GteX Program Japan

## Instrument



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## Chemical composition



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## Process for specimen treatment



## Computational method



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## Fileset

- id: f19da965-737b-4807-9ab5-5fb154eac417
  filename: 241018_MS_LiFSA-SL_PVDF-HFP_HVLMB_EndNote_ACSAPM.pdf
  content_type: application/pdf
  size: 1580710
  md5: b485a0159ec954c2688b3f9aa7ad95c8

## Thumbnail

fileset_id: f19da965-737b-4807-9ab5-5fb154eac417
filename: 241018_MS_LiFSA-SL_PVDF-HFP_HVLMB_EndNote_ACSAPM.pdf