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Water-Ion Interaction Determines the Mobility of Ions in Highly Concentrated Aqueous Electrolytes

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Title
Water-Ion Interaction Determines the Mobility of Ions in Highly Concentrated Aqueous Electrolytes
Author(s)
Jungyu Kim; Koo, Bonhyeop; Anahita Khammari; Kwanghee Park; Lee, Hochun; Kyungwon Kwak; Minhaeng Cho
Publication Date
2024-02
Journal
ACS Applied Materials & Interfaces, v.16, no.8, pp.10033 - 10041
Publisher
American Chemical Society
Abstract
Solvation engineering plays a critical role in tailoring the performance of batteries, particularly through the use of highly concentrated electrolytes, which offer heterogeneous solvation structures of mobile ions with distinct electrochemical properties. In this study, we employed spectroscopic techniques and molecular dynamics simulations to investigate mixed-cation (Li+/K+) acetate aqueous electrolytes. Our research unravels the pivotal role of water in facilitating ion transport within a highly viscous medium. Notably, Li+ cations primarily form ion aggregates, predominantly interacting with acetate anions, while K+ cations emerge as the principal charge carriers, which is attributed to their strong interaction with water molecules. Intriguingly, even at a concentration as high as 40 m, a substantial amount of water molecules persistently engages in hydrogen bonding with one another, creating mobile regions rich in K+ ions. Our observations of a redshift of the OH stretching band of water suggest that the strength of the hydrogen bond alone cannot account for the expansion of the electrochemical stability window. These findings offer valuable insights into the cation transfer mechanism, shedding light on the contribution of water-bound cations to both the ion conductivity and the electrochemical stability window of aqueous electrolytes for rechargeable batteries. Our comprehensive molecular-level understanding of the interplay between cations and water provides a foundation for future advances in solvation engineering, leading to the development of high-performance batteries with improved energy storage and safety profiles.
URI
https://pr.ibs.re.kr/handle/8788114/14856
DOI
10.1021/acsami.3c15609
ISSN
1944-8244
Appears in Collections:
Center for Molecular Spectroscopy and Dynamics(분자 분광학 및 동력학 연구단) > 1. Journal Papers (저널논문)
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