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

Zhang, Danfeng; Liu, Ming; Ma, Jiabin; Yang, Ke; Chen, Zhen; Li, Kaikai; Zhang, Chen; Wei, Yinping et al. · Nat Commun · 2022

basic_science · Level V

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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||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (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.