Lithium hexamethyldisilazide as electrolyte additive for efficient cycling of high-voltage non-aqueous lithium metal batteries

Danfeng Zhang, Ming Liu, Jiabin Ma, Ke Yang, Zhen Chen, Kaikai Li, Chen Zhang, Yinping Wei, Min Zhou, Peng Wang, Yuanbiao He, Wei Lv, Quan-Hong Yang, Feiyu Kang and Yan-Bing He ()
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Danfeng Zhang: Tsinghua University
Ming Liu: Tsinghua University
Jiabin Ma: Tsinghua University
Ke Yang: Tsinghua University
Zhen Chen: Tsinghua University
Kaikai Li: School of Materials Science and Engineering, Harbin Institute of Technology
Chen Zhang: Tsinghua University
Yinping Wei: Tsinghua University
Min Zhou: East China University of Science and Technology
Peng Wang: Tsinghua University
Yuanbiao He: Tsinghua University
Wei Lv: Tsinghua University
Quan-Hong Yang: Tianjin University
Feiyu Kang: Tsinghua University
Yan-Bing He: Tsinghua University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract High-voltage lithium metal batteries suffer from poor cycling stability caused by the detrimental effect on the cathode of the water moisture present in the non-aqueous liquid electrolyte solution, especially at high operating temperatures (e.g., ≥60 °C). To circumvent this issue, here we report lithium hexamethyldisilazide (LiHMDS) as an electrolyte additive. We demonstrate that the addition of a 0.6 wt% of LiHMDS in a typical fluorine-containing carbonate-based non-aqueous electrolyte solution enables a stable Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) coin cell operation up to 1000 or 500 cycles applying a high cut-off cell voltage of 4.5 V in the 25 °C−60 °C temperature range. The LiHMDS acts as a scavenger for hydrofluoric acid and water and facilitates the formation of an (electro)chemical robust cathode|electrolyte interphase (CEI). The LiHMDS-derived CEI prevents the Ni dissolution of NCM811, mitigates the irreversible phase transformation from layered structure to rock-salt phase and suppresses the side reactions with the electrolyte solution.

Date: 2022
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DOI: 10.1038/s41467-022-34717-4

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