Poly(Ionic Liquid) Electrolytes at an Extreme Salt Concentration for Solid-State Batteries
Polymer-in-salt electrolytes were introduced three decades ago as an innovative solution to the challenge of low Li-ion conductivity in solvent-free solid polymer electrolytes. Despite significant progress, the approach still faces considerable challenges, ranging from a fundamental understanding to the development of suitable polymers and salts. A critical issue is maintaining both the stability and high conductivity of molten salts within a polymer matrix, which has constrained their further exploration. This research offers a promising solution by integrating cationic poly(ionic liquids) (polyIL) with a crystallization-resistive salt consisting of asymmetric anions. A stable polymer-in-salt electrolyte with an exceptionally high Li-salt content of up to 90 mol % was achieved, providing a valuable opportunity for the in-depth understanding of these electrolytes at an extremely high salt concentration. This work explicates how increased salt concentration affects coordination structures, glass transitions, ionic conductivity, and the decoupling and coupling of ion transport from structural dynamics in a polymer electrolyte, ultimately enhancing electrolyte performance. These findings provide significant knowledge advancement in the field, guiding the future design of polymer-in-salt electrolytes.
Authors
- Heng Zhang (ORCID: https://orcid.org/0000-0002-8811-6336)
- Shinji Kondou (ORCID: https://orcid.org/0000-0002-7782-7431)
- Azusa Nakanishi
- Taku Sudoh (ORCID: https://orcid.org/0009-0007-7265-3288)
- Hiroyuki Ueda (ORCID: https://orcid.org/0000-0002-1278-8734)
- Luke A. O’Dell (ORCID: https://orcid.org/0000-0002-7760-5417)
- Faezeh Makhlooghiazad (ORCID: https://orcid.org/0000-0002-8002-9668)
- Ivan I. Popov (ORCID: https://orcid.org/0000-0002-7235-2043)
- Alexei P. Sokolov (ORCID: https://orcid.org/0000-0002-8187-9445)
- Masayoshi Watanabe (ORCID: https://orcid.org/0000-0003-4092-6150)
- Michel B. Armand (ORCID: https://orcid.org/0000-0002-1303-9233)
- Murillo L. Martins (ORCID: https://orcid.org/0000-0002-3883-9114)
- Mohanad Abdullah
- Patrick C. Howlett (ORCID: https://orcid.org/0000-0002-2151-2932)
- Kazuhide Ueno (ORCID: https://orcid.org/0000-0002-4684-5717)
- Maria Forsyth (ORCID: https://orcid.org/0000-0002-4273-8105)
- Fangfang Chen (ORCID: https://orcid.org/0000-0002-8004-1720)
Institutions
- Oak Ridge National Laboratory (US)
- Deakin University (AU)
- Yokohama National University (JP)
- Boeing (Spain) (ES)
- ARC Centre of Excellence in Future Low-Energy Electronics Technologies (AU)
- NOAA Chemical Sciences Laboratory (US)
- CIC energiGUNE (ES)
- Digital Research Alliance of Canada
- Huazhong University of Science and Technology (CN)
- University of Tennessee at Knoxville (US)
- The University of Osaka (JP)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-11-19
- DOI
- https://doi.org/10.1021/jacs.4c12616
- Citations
- 43
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 8.97
Funders
- Australian Research Council
- Japan Society for the Promotion of Science
- National Cancer Institute