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

被引:122
作者
Li, Zheng [1 ]
Rao, Harsha [1 ]
Atwi, Rasha [2 ]
Sivakumar, Bhuvaneswari M. [3 ]
Gwalani, Bharat [3 ,4 ]
Gray, Scott [5 ]
Han, Kee Sung [3 ,4 ]
Everett, Thomas A. [6 ]
Ajantiwalay, Tanvi A. [3 ]
Murugesan, Vijayakumar [3 ,4 ]
Rajput, Nav Nidhi [2 ]
Pol, Vilas G. [1 ]
机构
[1] Purdue Univ, Davidson Sch Chem Engn, W Lafayette, IN 47907 USA
[2] SUNY Stony Brook, Dept Mat Sci & Chem Engn, Stony Brook, NY 11794 USA
[3] Pacif Northwest Natl Lab, Richland, WA 99352 USA
[4] Pacif Northwest Natl Lab, Joint Ctr Energy Storage Res, Richland, WA 99352 USA
[5] Battery Innovat Ctr, Newberry, IN 47449 USA
[6] Purdue Univ, Discovery Pk, W Lafayette, IN 47907 USA
关键词
MOLECULAR-DYNAMICS; SOLVATION; MECHANISM; ANODE;
D O I
10.1038/s41467-023-36647-1
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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 mu m thick) and a LiNi0.8Co0.1Mn0.1O2-based positive electrode (3.3 mAh/cm(2)) in pouch cell configuration at 25 degrees C, a specific discharge capacity retention of about 74% after 150 cycles (0.33 and 1mA/cm(2) charge and discharge, respectively) is obtained. Ether solvents have poor anodic stabilities in lithium metal batteries. Here, the authors propose a non-aqueous electrolyte solution with a non-polar and non-fluorinated ether solvent. The electrolyte enables stable cycling of high-voltage Li metal batteries in pouch cell configuration.
引用
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页数:13
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