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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, Vilas G. Pol

2023Nature Communications274 citationsDOIOpen Access PDF

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 LiNi 0.8 Co 0.1 Mn 0.1 O 2 -based positive electrode (3.3 mAh/cm 2 ) in pouch cell configuration at 25 °C, a specific discharge capacity retention of about 74% after 150 cycles (0.33 and 1 mA/cm 2 charge and discharge, respectively) is obtained.

Topics & Concepts

ElectrolyteElectrochemistryLithium (medication)SolventEtherInorganic chemistryElectrodeAqueous solutionChemistryMaterials scienceSalt (chemistry)Chemical engineeringOrganic chemistryPhysical chemistryEndocrinologyMedicineEngineeringAdvanced Battery Materials and TechnologiesAdvancements in Battery MaterialsAdvanced Battery Technologies Research
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