Pseudo-concentrated electrolytes for lithium metal batteries

Wang Huaping; Liu Jiandong; He Jian; Qi Shihan; Wu Mingguang; Li Fang; Huang Junda; Huang Yun; Ma Jianmin

doi:10.1016/j.esci.2022.06.005

Volume 2 Issue 5

Sep. 2022

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Wang Huaping, Liu Jiandong, He Jian, Qi Shihan, Wu Mingguang, Li Fang, Huang Junda, Huang Yun, Ma Jianmin. Pseudo-concentrated electrolytes for lithium metal batteries[J]. eScience, 2022, 2(5): 557-565. doi: 10.1016/j.esci.2022.06.005

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Wang Huaping, Liu Jiandong, He Jian, Qi Shihan, Wu Mingguang, Li Fang, Huang Junda, Huang Yun, Ma Jianmin. Pseudo-concentrated electrolytes for lithium metal batteries[J]. eScience, 2022, 2(5): 557-565. doi: 10.1016/j.esci.2022.06.005

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Pseudo-concentrated electrolytes for lithium metal batteries

doi: 10.1016/j.esci.2022.06.005

School of Physics and Electronics, Hunan University, Changsha, 410082, China

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Corresponding author: E-mail address: nanoelechem@hnu.edu.cn (J. Ma)
Received Date: 2022-04-11
Revised Date: 2022-06-08
Accepted Date: 2022-06-21

Available Online: 2022-06-28

Abstract

Abstract

Lithium metal batteries suffer from short lifespans and low Coulombic efficiency (CE) due to the high reactivity of Li and the poor stability of the solid electrolyte interphase (SEI). Herein, we propose the concept of a pseudo-concentrated electrolyte (PCE) induced by an electron-deficient additive (4-pyridylboronic acid; 4-PBA) to form a robust, LiF-rich SEI, thus addressing the above issues. Molecular dynamics simulations confirm that 4-PBA can increase the coordination number of anions in the Li⁺ solvation sheath to achieve pseudo-concentrated LiPF₆ in the electrolyte. Moreover, the 4-PBA can scavenge harmful PF₅ decomposed from LiPF₆ to stabilize the LiF-rich SEI. The resulting robust LiF-rich SEI promotes Li growth along the SEI/Li interface and represses the growth of Li dendrites. Thus, excellent performance is achieved, with a high CE of 97.1% for a Li||Cu cell at 1.0 mA cm⁻², and over 950 cycles at 0.5 mA cm⁻² for Li||Li symmetric cells with 1.0 wt% 4-PBA electrolyte. Meanwhile, the resulting stable boron-containing cathode electrolyte interphase enables Li||LiNi₀_·₆Co₀_·₂Mn₀_·₂O₂ (NCM622) cells to achieve excellent stability, with a capacity retention of 86.9% after 200 cycles.
- Lithium metal batteries,
- Pseudo-concentrated electrolyte,
- Solid electrolyte interphase,
- Solvation structure,
- 4-Pyridylboronic acid

● 4-pyridylboronic acid can scavenge harmful PF₅ in the electrolyte.
● As an additive, 4-pyridylboronic acid can have a pseudo-concentrated effect on electrolytes.
● The concept of a pseudo-concentrated electrolyte is presented.
● 4-pyridylboronic acid can increase the coordination number of PF₆^– anions in the Li⁺ solvation sheath.
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Supplementary data to this article can be found online at https://doi.org/10.1016/j.esci.2022.06.005.
Appendix A. Supplementary data

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