Issue 15, 2024

Trace ethylene carbonate-mediated low-concentration ether-based electrolytes for high-voltage lithium metal batteries

Abstract

Ether-based electrolytes have been extensively utilized in lithium metal batteries due to their superior compatibility with lithium metal. Nevertheless, the inferior high-voltage oxidation stability (>4.0 V) hampers their practical implementation and proves challenging to rectify without resorting to high-concentration strategies or the inclusion of specific additives. Herein, it was discovered that the ether-based electrolytes can be well-stabilized by adding a trace amount of ethylene carbonate (EC) at a low concentration (i.e., 0.63 M). This strategy can not only improve the solubility of LiPF6 in dimethoxyethane (DME) solvent significantly, but also improve the high-voltage oxidation stability of the electrolyte, enabling the 80 μm Li‖LiNi0.8Co0.1Mn0.1O2 full-cell to operate stably at 4.5 V. We demonstrated that the EC can preferentially dissociate the insoluble LiPF6 by entering the first solvation layer, which further regulates the molecule–ion interaction on the cathode interface to improve the oxidation stability of the electrolyte. A novel solvation structure and interfacial model were proposed to elucidate the solubilization effect and interpret the superior battery performance at the molecular scale. This work not only sheds light on the electrolyte's microstructures in their formulation but also offers a promising strategy to overcome the challenges associated with high-energy-density lithium (ion) batteries.

Graphical abstract: Trace ethylene carbonate-mediated low-concentration ether-based electrolytes for high-voltage lithium metal batteries

Supplementary files

Article information

Article type
Paper
Submitted
26 Apr 2024
Accepted
21 Jun 2024
First published
24 Jun 2024

Energy Environ. Sci., 2024,17, 5613-5626

Trace ethylene carbonate-mediated low-concentration ether-based electrolytes for high-voltage lithium metal batteries

Y. Chen, Z. Ma, Y. Wang, P. Kumar, F. Zhao, T. Cai, Z. Cao, L. Cavallo, H. Cheng, Q. Li and J. Ming, Energy Environ. Sci., 2024, 17, 5613 DOI: 10.1039/D4EE01831A

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