A nonflammable electrolyte for ultrahigh-voltage (4.8 V-class) Li||NCM811 cells with a wide temperature range of 100 °C

被引:193
作者
Xiao, Peitao [1 ,2 ]
Zhao, Yun [3 ,4 ]
Piao, Zhihong [1 ]
Li, Baohua [3 ,4 ]
Zhou, Guangmin [1 ]
Cheng, Hui-Ming [1 ,5 ,6 ]
机构
[1] Tsinghua Univ, Shenzhen Geim Graphene Ctr, Shenzhen Int Grad Sch, Tsinghua Berkeley Shenzhen Inst & Tsinghua, Shenzhen 518055, Peoples R China
[2] Natl Univ Def Technol, Coll Aerosp Sci & Engn, Changsha 410073, Peoples R China
[3] Tsinghua Shenzhen Int Grad Sch SIGS, Shenzhen Key Lab Power Battery Safety, Shenzhen 518055, Peoples R China
[4] Tsinghua Shenzhen Int Grad Sch SIGS, Shenzhen Geim Graphene Ctr, Shenzhen 518055, Peoples R China
[5] Chinese Acad Sci, Inst Technol Carbon Neutral, Shenzhen Inst Adv Technol, Shenzhen 518055, Peoples R China
[6] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
基金
中国国家自然科学基金;
关键词
METAL ANODES; LITHIUM; BATTERIES;
D O I
10.1039/d1ee02959b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of ultrahigh-voltage lithium metal batteries is one of the most promising ways to increase the energy density. However, commercial ethylene carbonate (EC)-based electrolytes have poor compatibility with both lithium metal anodes and cathodes at ultrahigh voltages. We report a high-voltage resistant electrolyte (HV electrolyte) produced by the fluorination of commercial solvents with the guidance of theoretical calculations. These designed solvents, with low energy levels of the lowest unoccupied molecular orbital (LUMO), can be preferably reduced at the lithium metal anode, suppressing lithium dendrite growth because of the formation of a LiF-rich solid-electrolyte interphase (SEI). Fluorination also decreases the energy levels of the highest occupied molecular orbital (HOMO), resulting in improved anodic stability at ultrahigh voltages. The low binding energies between fluorinated solvents in the HV electrolyte and Li+ accelerate the desolvation of Li+, leading to excellent electrochemical kinetics. As a result, Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) cells, which can work in a wide operating temperature range from -30 to 70 degrees C, have capacity retentions of 95.1% after 160 cycles and 85.7% after 100 cycles at ultrahigh cut-off voltages of 4.7 and 4.8 V, respectively. Li||NCM811 cells with a thin (50 mu m) lithium metal anode and a lean electrolyte were constructed, and had a capacity retention of 89.2% after 150 cycles, demonstrating high potential in practical use as high energy density batteries.
引用
收藏
页码:2435 / 2444
页数:10
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