• Nano-Micro Letters
  • Vol. 15, Issue 1, 234 (2023)
Zhenglu Zhu1、2, Xiaohui Li3, Xiaoqun Qi1, Jie Ji1, Yongsheng Ji2, Ruining Jiang2, Chaofan Liang1, Dan Yang2, Ze Yang3、*, Long Qie1、**, and Yunhui Huang1
Author Affiliations
  • 1State Key Laboratory of Material Processing and Die and Mold Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074 Hubei, People’s Republic of China
  • 2Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai 201804, People’s Republic of China
  • 3Institute of Nanoscience and Nanotechnology, School of Physical Science and Technology, Central China Normal University, Wuhan 430079, People’s Republic of China
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    DOI: 10.1007/s40820-023-01205-3 Cite this Article
    Zhenglu Zhu, Xiaohui Li, Xiaoqun Qi, Jie Ji, Yongsheng Ji, Ruining Jiang, Chaofan Liang, Dan Yang, Ze Yang, Long Qie, Yunhui Huang. Demystifying the Salt-Induced Li Loss: A Universal Procedure for the Electrolyte Design of Lithium-Metal Batteries[J]. Nano-Micro Letters, 2023, 15(1): 234 Copy Citation Text show less

    Abstract

    Lithium (Li) metal electrodes show significantly different reversibility in the electrolytes with different salts. However, the understanding on how the salts impact on the Li loss remains unclear. Herein, using the electrolytes with different salts (e.g., lithium hexafluorophosphate (LiPF6), lithium difluoro(oxalato)borate (LiDFOB), and lithium bis(fluorosulfonyl)amide (LiFSI)) as examples, we decouple the irreversible Li loss (SEI Li+ and “dead” Li) during cycling. It is found that the accumulation of both SEI Li+ and “dead” Li may be responsible to the irreversible Li loss for the Li metal in the electrolyte with LiPF6 salt. While for the electrolytes with LiDFOB and LiFSI salts, the accumulation of “dead” Li predominates the Li loss. We also demonstrate that lithium nitrate and fluoroethylene carbonate additives could, respectively, function as the “dead” Li and SEI Li+ inhibitors. Inspired by the above understandings, we propose a universal procedure for the electrolyte design of Li metal batteries (LMBs): (i) decouple and find the main reason for the irreversible Li loss; (ii) add the corresponding electrolyte additive. With such a Li-loss-targeted strategy, the Li reversibility was significantly enhanced in the electrolytes with 1,2-dimethoxyethane, triethyl phosphate, and tetrahydrofuran solvents. Our strategy may broaden the scope of electrolyte design toward practical LMBs.
    Zhenglu Zhu, Xiaohui Li, Xiaoqun Qi, Jie Ji, Yongsheng Ji, Ruining Jiang, Chaofan Liang, Dan Yang, Ze Yang, Long Qie, Yunhui Huang. Demystifying the Salt-Induced Li Loss: A Universal Procedure for the Electrolyte Design of Lithium-Metal Batteries[J]. Nano-Micro Letters, 2023, 15(1): 234
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