Highly Stable Lithium Metal Batteries Enabled by Tuning the Molecular Polarity of Diluents in Localized High-Concentration Electrolytes.

Yang, Xin-Tao; Han, Chong; Xie, Yi-Meng; Fang, Rong; Zheng, Shisheng; Tian, Jing-Hua; Lin, Xiu-Mei; Zhang, Hua; Mao, Bing-Wei; Gu, Yu; Wang, Yao-Hui; Li, Jian-Feng

Yang, Xin-Tao; Han, Chong; Xie, Yi-Meng; Fang, Rong; Zheng, Shisheng; Tian, Jing-Hua; Lin, Xiu-Mei; Zhang, Hua; Mao, Bing-Wei; Gu, Yu; Wang, Yao-Hui; Li, Jian-Feng.

Affiliation

Yang XT; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Han C; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Xie YM; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Fang R; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Zheng S; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Tian JH; Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen, 361005, China.
Lin XM; Department of Chemistry and Environment Science, Fujian Province University Key Laboratory of Analytical Science, Minnan Normal University, Zhangzhou, 363000, China.
Zhang H; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Mao BW; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Gu Y; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Wang YH; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Li JF; College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Energy, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.

Small ; 20(28): e2311393, 2024 Jul.

Article in En | MEDLINE | ID: mdl-38287737

ABSTRACT

ABSTRACT

Electrolyte plays a crucial role in ensuring stable operation of lithium metal batteries (LMBs). Localized high-concentration electrolytes (LHCEs) have the potential to form a robust solid-electrolyte interphase (SEI) and mitigate Li dendrite growth, making them a highly promising electrolyte option. However, the principles governing the selection of diluents, a crucial component in LHCE, have not been clearly determined, hampering the advancement of such a type of electrolyte systems. Herein, the diluents from the perspective of molecular polarity are rationally designed and developed. A moderately fluorinated solvent, 1-(1,1,2,2-tetrafluoroethoxy)propane (TNE), is employed as a diluent to create a novel LHCE. The unique molecular structure of TNE enhances the intrinsic dipole moment, thereby altering solvent interactions and the coordination environment of Li-ions in LHCE. The achieved solvation structure not only enhances the bulk properties of LHCE, but also facilitates the formation of more stable anion-derived SEIs featured with a higher proportion of inorganic species. Consequently, the corresponding full cells of both Li||LiFePO4 and Li||LiNi0.8Co0.1Mn0.1O2 cells utilizing Li thin-film anodes exhibit extended long-term stability with significantly improved average Coulombic efficiency. This work offers new insights into the functions of diluents in LHCEs and provides direction for further optimizing the LHCEs for LMBs.

Key words

lithium metal batteries; localized highconcentration electrolyte; solidelectrolyte interphase; strongpolarity diluent

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