Sandwich-Model Cathode Electrolyte Interphase Facilitating All-Climate High-Voltage Nickel-Rich Cathode-Based Lithium Metal Batteries with LiBF<sub>4</sub>-Based Electrolyte.

Liu, Lei; Li, Yong; Su, Tao; Li, Chao; Hao, Zhimeng; Yang, Gaojing; Ma, Jianmin · Adv Mater · 2025

basic_science · Level V

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Abstract

All-climate lithium metal batteries are highly needed, but remains a huge challenge in cycling life due to the existence of unstable electrode electrolyte interphases, especially with nickel-rich layered oxide cathode at high cut-off voltage. To address this question, a functional and robust sandwich-model cathode electrolyte interphase (CEI) is proposed, derived from a LiBF<sub>4</sub>-based electrolyte modified with para-fluorobenzeneacetonitrile (P-FBCN) additive, to realize the stability of 4.8 V Li||LiNi<sub>0.94</sub>Co<sub>0.05</sub>Mn<sub>0.01</sub>O<sub>2</sub> (NCM94) battery operated from -60 to 60 °C. The LiF-rich sandwich-model CEI features an outer layer of LiB<sub>x</sub>O<sub>y</sub>-rich to enhance mechanical/thermal stability, and the inner -C≡N-rich anchoring layer to facilitate Li⁺ conduction and inhibit the dissolution of transition metal ions. Notably, the 7.6 Ah-grade Li||NCM94 pouch cell with such electrolyte can yield a high energy density of 544 Wh kg<sup>-1</sup> with a long lifespan of 158 cycles.