Non-polar ether-based electrolyte solutions for stable high-voltage non-aqueous lithium metal batteries

Zheng Li (), Harsha Rao, Rasha Atwi, Bhuvaneswari M. Sivakumar, Bharat Gwalani, Scott Gray, Kee Sung Han, Thomas A. Everett, Tanvi A. Ajantiwalay, Vijayakumar Murugesan, Nav Nidhi Rajput and Vilas G. Pol ()
Additional contact information
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

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-36647-1

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