Suppressing electrolyte-lithium metal reactivity via Li<sup>+</sup>-desolvation in uniform nano-porous separator.

Sheng, Li; Wang, Qianqian; Liu, Xiang; Cui, Hao; Wang, Xiaolin; Xu, Yulong; Li, Zonglong; Wang, Li et al. · Nat Commun · 2022

basic_science · Level V

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Abstract

Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithium-metal anode in a reversible manner. Considerable attention has been focused on inhibiting dendrite via interface and electrolyte engineering, while admitting electrolyte-lithium metal reactivity as a thermodynamic inevitability. Here, we report the effective suppression of such reactivity through a nano-porous separator. Calculation assisted by diversified characterizations reveals that the separator partially desolvates Li<sup>+</sup> in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li<sup>0</sup>-deposition occurs. The consequence of such deactivation is realizing dendrite-free lithium-metal electrode, which even retaining its metallic lustre after long-term cycling in both Li-symmetric cell and high-voltage Li-metal battery with LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> as cathode. The discovery that a nano-structured separator alters both bulk and interfacial behaviors of electrolytes points us toward a new direction to harness lithium-metal as the most promising anode.