首页|Unique double-layer solid electrolyte interphase formed with fluorinated ether-based electrolytes for high-voltage lithium metal batteries

Unique double-layer solid electrolyte interphase formed with fluorinated ether-based electrolytes for high-voltage lithium metal batteries

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Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attrib-uted to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both high-voltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a co-solvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based elec-trolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic com-ponents for enhanced flexibility.The Li‖Cu cells display a noticeably high Coulombic efficiency of 99.28％after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm2 and 1.0 mAh/cm2.In addition,lithium metal cells using LiNi0.8Co0.1Mn0.1O2 and LiCoO2 cathodes(both load-ings～3.0 mAh/cm2)realize capacity retentions of＞85％over 240 cycles with a charge cut-off voltage of 4.4 V and 90％for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries.

Lithium metal batteriesHigh-voltage layered oxidesFluorinated ether-based electrolytesSolid electrolyte interphaseCathode electrolyte interphase

Ruo Wang、Jiawei Li、Bing Han、Qingrong Wang、Ruohong Ke、Tong Zhang、Xiaohu Ao、Guangzhao Zhang、Zhongbo Liu、Yunxian Qian、Fangfang Pan、Iseult Lynch、Jun Wang、Yonghong Deng

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Department of Materials Science & Engineering,School of Innovation and Entrepreneurship,Southern University of Science and Technology,Shenzhen 518055,Guangdong,China

School of Geography,Earth and Environmental Sciences,University of Birmingham,Edgbaston,Birmingham B15 2TT,UK

Key Laboratory of Marine Environmental Corrosion and Bio-Fouling,Institute of Oceanology,Chinese Academy of Sciences,Qingdao 266071,Shandong,China

Shenzhen CAPCHEM Technology Co.,Ltd.,Shenzhen 518118,Guangdong,China

CALB Group Co.,Ltd.,Changzhou 213200,Jiangsu,China

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Key-Area Research and Development Program of Guangdong ProvinceNational Natural Science Foundation of ChinaGuangdong Natural Science Foundation for Basic and Applied Basic ResearchGuangdong Natural Science Foundation for Basic and Applied Basic Research

2020B090919001220781442021A15150101382023A1515010686

2024

10.1016/j.jechem.2023.10.002

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.88(1)
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