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

Li Sheng, Qianqian Wang, Xiang Liu, Hao Cui, Xiaolin Wang, Yulong Xu, Zonglong Li, Li Wang, Zonghai Chen, Gui-Liang Xu, Jianlong Wang, Yaping Tang, Khalil Amine, Hong Xu () and Xiangming He ()
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Li Sheng: Institute of Nuclear and New Energy Technology, Tsinghua University
Qianqian Wang: Institute of Nuclear and New Energy Technology, Tsinghua University
Xiang Liu: Argonne National Laboratory
Hao Cui: Institute of Nuclear and New Energy Technology, Tsinghua University
Xiaolin Wang: Institute of Nuclear and New Energy Technology, Tsinghua University
Yulong Xu: Institute of Nuclear and New Energy Technology, Tsinghua University
Zonglong Li: Institute of Nuclear and New Energy Technology, Tsinghua University
Li Wang: Institute of Nuclear and New Energy Technology, Tsinghua University
Zonghai Chen: Argonne National Laboratory
Gui-Liang Xu: Argonne National Laboratory
Jianlong Wang: Institute of Nuclear and New Energy Technology, Tsinghua University
Yaping Tang: Institute of Nuclear and New Energy Technology, Tsinghua University
Khalil Amine: Argonne National Laboratory
Hong Xu: Institute of Nuclear and New Energy Technology, Tsinghua University
Xiangming He: Institute of Nuclear and New Energy Technology, Tsinghua University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: 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+ in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li0-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 LiNi0.6Mn0.2Co0.2O2 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.

Date: 2022
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DOI: 10.1038/s41467-021-27841-0

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