Suppressing electrolyte-lithium metal reactivity via Li+-desolvation in uniform nano-porous separator

• Published in: Nature communications Vol. 13; no. 1; p. 172
• Main Authors: Sheng, Li, Wang, Qianqian, Liu, Xiang, Cui, Hao, Wang, Xiaolin, Xu, Yulong, Li, Zonglong, Wang, Li, Chen, Zonghai, Xu, Gui-Liang, Wang, Jianlong, Tang, Yaping, Amine, Khalil, Xu, Hong, He, Xiangming
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 10.01.2022; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 147/135; 639/4077/4079/891; 639/638/161/891; 639/925/357/404; Anodes; Chemical reduction; Deactivation; Dendritic structure; Electrochemistry; Electrolytes; Humanities and Social Sciences; Lithium; Lithium ions; Metals; multidisciplinary; Reactivity; Science; Science (multidisciplinary); Separators
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-021-27841-0

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 + in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li 0 -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 0.6 Mn 0.2 Co 0.2 O 2 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. Lithium dendrite and parasitic reactions are two major challenges for lithium metal anode. Here, the authors show suppression of lithium-dendrite and elimination of continuous parasitic reactions by tuning the reduction kinetics of lithium-ion through a uniform nano-porous separator.