Citation: Li-Heng ZHANG, Hai-Tao GU, Ying LUO, Qing-Yu DONG, Yan-Bin SHEN, Jing-Ying XIE. Tris(trimethylsilyl)-Based Additives Enables Practical 5 V LiNi_0.5Mn_1.5O₄ Batteries[J]. Chinese Journal of Inorganic Chemistry, ;2022, 38(10): 2091-2102. doi: 10.11862/CJIC.2022.215 shu

Tris(trimethylsilyl)-Based Additives Enables Practical 5 V LiNi_0.5Mn_1.5O₄ Batteries

Li-Heng ZHANG ¹ ,
Hai-Tao GU ² ,
Ying LUO ² ,
Qing-Yu DONG ³ ,
Yan-Bin SHEN ^3,, ,
Jing-Ying XIE ^{1, 2,,}

1.
School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China
2.
State Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, China
3.
i-Lab, CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, Jiangsu 215123, China

Corresponding author: Yan-Bin SHEN, ybshen2017@sinano.ac.cn Jing-Ying XIE, jyxie@hit.edu.cn
Received Date: 9 July 2022
Revised Date: 29 August 2022

Figures(10)

LiNi_0.5Mn_1.5O₄ cathode materials have been considered promising candidates for high energy density Li-ion batteries due to their high operation potential. However, to develop 5 V LiNi_0.5Mn_1.5O₄-based batteries, practical electrolytes with high electrochemical stability are yet to be realized. In this work, tris(trimethylsilyl)-based additives, including tris(trimethylsilyl)borate (TMSB) and tris(trimethylsilyl)phosphite (TMSPi), were selected as electrolyte additives for typical ethylene carbonate (EC)-LiPF₆ based electrolyte to develop practical LiNi_0.5Mn_1.5O₄-based batteries. Combining theoretical calculations, physicochemical characterization, and electrochemical measurements, we found that both TMSB and TMSPi can improve the Coulombic efficiency and cycling stability of 5 V LiNi_0.5Mn_1.5O₄-based cells. Specifically, TMSB can act as the stabilizer for PF₆^- due to its electron deficiency nature, thereby suppressing the increase of cell impedance. In addition, thanks to its high highest occupied molecule orbital (HOMO) energy level, TMSPi can be preferentially oxidized on the surface of charged LiNi_0.5Mn_1.5O₄ electrodes, resulting in a decent rate capacity and high discharge platform. In addition, TMSPi is conducive to the formation of robust solid electrolyte interphase (SEI) on graphite anode through the nucleophilic attack, resulting in enhanced cycle performance. As a result, Graphite||LiNi_0.5Mn_1.5O₄ pouch cells with TMSPi - containing electrolyte displayed capacity retention of 88.9% after 100 cycles at 1C, superior to that in the blank (60.5%) and TMSB - containing (77.4%) electrolytes.
- electrolyte additive,
- LiNi_0.5Mn_1.5O₄,
- tris(trimethylsilyl)borate,
- tris(trimethylsilyl)phosphite
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沈阳化工大学材料科学与工程学院沈阳 110142

Tris(trimethylsilyl)-Based Additives Enables Practical 5 V LiNi0.5Mn1.5O4 Batteries

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通讯作者: 陈斌, bchen63@163.com

Tris(trimethylsilyl)-Based Additives Enables Practical 5 V LiNi_0.5Mn_1.5O₄ Batteries