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

Efaw, Corey M.; Wu, Qisheng; Gao, Ningshengjie; Zhang, Yugang; Zhu, Haoyu; Gering, Kevin; Hurley, Michael F.; Xiong, Hui; Hu, Enyuan; Cao, Xia; Xu, Wu; Zhang, Ji-Guang; Dufek, Eric J.; Xiao, Jie; Yang, Xiao-Qing; Liu, Jun; Qi, Yue; Li, Bin

doi:10.1038/s41563-023-01700-3

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

Journal Article · Mon Nov 06 00:00:00 EST 2023 · Nature Materials

DOI:https://doi.org/10.1038/s41563-023-01700-3· OSTI ID:2205647

^[1]; ^[2]; ^[3]; ^[4]; Zhu, Haoyu ^[5]; Gering, Kevin ^[3]; Hurley, Michael F. ^[5]; ^[5]; ^[6]; ^[7]; ^[7]; ^[7]; ^[3]; ^[7]; ^[6]; ^[7]; ^[2]; ^[8]

Idaho National Laboratory (INL), Idaho Falls, ID (United States); Boise State Univ., ID (United States)
Brown Univ., Providence, RI (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Boise State Univ., ID (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States); Boise State Univ., ID (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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. Importantly, 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Idaho National Laboratory (INL), Idaho Falls, ID (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Aeronautics and Space Administration (NASA); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO). Batteries for Advanced Transportation Technologies (BATT) Program

Grant/Contract Number:: AC05-00OR22725; AC05-76RL01830; AC07-05ID14517; SC0012704

OSTI ID:: 2205647

Alternate ID(s):: OSTI ID: 2328511
OSTI ID: 2386883
OSTI ID: 2251586

Report Number(s):: BNL--224993-2023-JAAM; INL/JOU-24-78659-Rev000; PNNL-SA-178219

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 12 Vol. 22; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
Lithium battery
Performance
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batteries
electrolyte
high voltage
lithium-ion battery
low temperature
molecular dynamics

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

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