Unlocking 4.9 V Quasi-Solid-State Lithium Metal Battery via Solvent Screening and Interfacial Manipulation.

Qiu, Bin; Xu, Feng; Huang, Jie; Wu, Ying; Huang, Kaiming; Gao, Jinyu; He, Chuanxin; Zhang, Peixin et al. · Nano Lett · 2024

basic_science · Level V

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Abstract

Parlous structure integrity of the cathode and erratic interfacial microdynamics under high potential take responsibility for the degradation of solid-state lithium metal batteries (LMBs). Here, high-voltage LMBs have been operated by modulating the polymer electrolyte intrinsic structure through an intermediate dielectric constant solvent and further inducing the gradient solid-state electrolyte interphase. Benefiting from the chemical adsorption between trimethyl phosphate (TMP) and the cathode, the gradient interphase rich in LiPF<sub><i>x</i></sub>O<sub><i>y</i></sub> and LiF is induced, thereby ensuring the structural integrity and interface compatibility of the commercial LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathode even at the 4.9 V cutoff voltage. Eventually, the specific capacity of NCM811|Li full cell based on TMP-modulated polymer electrolyte increased by 27.7% from 4.5 to 4.9 V. Such a universal screening method of electrolyte solvents and its derived electrode interfacial manipulation strategy opens fresh avenues for quasi-solid-state LMBs with high specific energy.