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Localized high-concentration electrolytes get more localized through micelle-like structures

delete2023-11-06
delete63
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OA
AI
C
Corey M. Efaw
Q
Qisheng Wu
N
Ningshengjie Gao
Y
Yugang Zhang
H
Haoyu Zhu
K
Kevin L. Gering
M
Michael F. Hurley
H
Hui Xiong
E
Enyuan Hu
X
Xia Cao
W
Wu Xu
J
Ji‐Guang Zhang
E
Eric J. Dufek
J
Jie Xiao
X
Xiao‐Qing Yang
刘俊 cover
刘俊 (Jun Liu)
Y
Yue Qi *
B
Bin Li *
DOI:10.1038/s41563-023-01700-3delete
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Abstract

Abstract

En 中文
Liquid electrolytes in batteries are typically treated as macroscopically homogeneous ionic transport media despite having a complex chemical composition and atomistic solvation structures, leaving a knowledge gap of the microstructural characteristics. Here, we reveal a unique micelle-like structure in a localized high-concentration electrolyte, in which the solvent acts as a surfactant between an insoluble salt in a diluent. The miscibility of the solvent with the diluent and simultaneous solubility of the salt results in a micelle-like structure with a smeared interface and an increased salt concentration at the centre of the salt-solvent clusters that extends the salt solubility. These intermingling miscibility effects have temperature dependencies, wherein a typical localized high-concentration electrolyte peaks in localized cluster salt concentration near room temperature and is used to form a stable solid-electrolyte interphase on a Li metal anode. These findings serve as a guide to predicting a stable ternary phase diagram and connecting the electrolyte microstructure with electrolyte formulation and formation protocols of solid-electrolyte interphases for enhanced battery cyclability. Liquid electrolytes in batteries are considered to be macroscopically homogeneous ionic transport media despite having a complex chemical composition and atomistic solvation structures. A micelle-like structure in a localized high-concentration electrolyte for which the solvent acts as a surfactant is reported.
Keywords:
ORTHOFORMATE-BASED ELECTROLYTES
MOLECULAR-DYNAMICS
METAL BATTERIES
LITHIUM
CONDUCTIVITY
INTERPHASE
SOLVATION
CARBONATE
SODIUM

Journal

Nature Materials cover
Nature Materials
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38.5
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Citations:
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Brown University
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Boise State University
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Idaho National Laboratory
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united states department of energy (doe)
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Brookhaven National Laboratory
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