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Tuning of Molecular Water Organization in Water-in-Salt Electrolytes by Addition of Chaotropic Ionic Liquids
KTH Royal Institute of Technology, Sweden.
Uppsala University, Sweden.
RISE Research Institutes of Sweden, Bioeconomy and Health, Chemical Process and Pharmaceutical Development.ORCID iD: 0000-0003-2410-7366
KTH Royal Institute of Technology, Sweden.
2023 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 127, no 50, p. 24065-24076Article in journal (Refereed) Published
Abstract [en]

Water-in-salt electrolytes (WISEs) have expanded the useful electrochemical stability of water, making the development of functional aqueous lithium-ion batteries more accessible. The implementation of additives in the formulation of WISEs can further improve the electrochemical stability of water and avoid potential lithium-ion salt solubility issues. Here, we have used Gemini-type ionic liquids to suppress water activity by designing the structure of ionic-liquid cations. The different water-organizing effects of ionic-liquid cations have been investigated and correlated to battery performance in LTO/LMO full cells. The champion device, containing the most chaotropic ionic liquid, retained at least 99% of its Coulombic efficiency after 500 charging cycles, associated with a final specific discharge capacity of 85 mA h·g-1. These results indicated that water-rich Li+ solvation shells significantly contribute to the excellent device performance and long-term stability of the LTO/LMO-based full battery cells. This work shows that the fine-tuning of the Li+ solvation shell and water structure by the addition of chaotropic cations represents a promising strategy for generating more stable and effective lithium-ion-containing rechargeable aqueous batteries. 

Place, publisher, year, edition, pages
American Chemical Society , 2023. Vol. 127, no 50, p. 24065-24076
Keywords [en]
Additives; Electric discharges; Electrolytes; Lithium-ion batteries; Positive ions; Solvation; Tuning; American Chemical Society; Battery performance; Electrochemical stabilities; Li +; Lithium ions; Molecular water; Salt electrolytes; Salt solubility; Solvation shell; Water activity; Ionic liquids
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:ri:diva-68772DOI: 10.1021/acs.jpcc.3c07164Scopus ID: 2-s2.0-85180106308OAI: oai:DiVA.org:ri-68772DiVA, id: diva2:1827698
Funder
Swedish Energy Agency, 50119-1Swedish Research Council, 2020-06701
Note

The work was supported by the Swedish Energy Agency contract no. 50119-1, entitled “Be WiSE─Robotic screening of water-in-salt electrolytes (WiSE) for environmental batteries” and the Swedish Research Council contract no. 2020-06701.

Available from: 2024-01-15 Created: 2024-01-15 Last updated: 2024-01-15Bibliographically approved

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Svensson, Per H.

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