Non-polar Ether-based Electrolyte Solutions for Stable High-voltage Non-aqueous Lithium Metal Batteries (original) (raw)

• Zheng Li, Purdue University
• Harsha Rao, Purdue University
• Rasha Atwi, Stony Brook University
• Bhuvaneswari M. Sivakumar, Pacific Northwest National Laboratory
• Bharat Gwalani, Pacific Northwest National Laboratory
• Scott Gray, Battery Innovation Center
• Kee Sung Han, Pacific Northwest National Laboratory
• Thomas A. Everett, Purdue University
• Tanvi A. Ajantiwalay, Pacific Northwest National Laboratory
• Vijayakumar Murugesan, Pacific Northwest National Laboratory
• Nav Nidhi Rajput, Stony Brook University
• Vilas G. Pol, Purdue University

Abstract

The electrochemical instability of ether-based electrolyte solutions hinders their practical applications in high-voltage Li metal batteries. To circumvent this issue, here, we propose a dilution strategy to lose the Li+/solvent interaction and use the dilute non-aqueous electrolyte solution in high-voltage lithium metal batteries. We demonstrate that in a non-polar dipropyl ether (DPE)-based electrolyte solution with lithium bis(fluorosulfonyl) imide salt, the decomposition order of solvated species can be adjusted to promote the Li+/salt-derived anion clusters decomposition over free ether solvent molecules. This selective mechanism favors the formation of a robust cathode electrolyte interphase (CEI) and a solvent-deficient electric double-layer structure at the positive electrode interface. When the DPE-based electrolyte is tested in combination with a Li metal negative electrode (50 μm thick) and a LiNi0.8Co0.1Mn0.1O2-based positive electrode (3.3 mAh/cm2) in pouch cell configuration at 25 °C, a specific discharge capacity retention of about 74% after 150 cycles (0.33 and 1 mA/cm2 charge and discharge, respectively) is obtained.

DOI

10.1038/s41467-023-36647-1

Date of this Version

2-16-2023

Recommended Citation

Li, Z., Rao, H., Atwi, R. et al. Non-polar ether-based electrolyte solutions for stable high-voltage non-aqueous lithium metal batteries. Nat Commun 14, 868 (2023). https://doi.org/10.1038/s41467-023-36647-1

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