Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries

Zhiao Yu, Hansen Wang, Xian Kong, William Huang, Yuchi Tsao, David G. Mackanic, Kecheng Wang, Xinchang Wang, Wenxiao Huang, Snehashis Choudhury, Yu Zheng, Chibueze V. Amanchukwu, Samantha T. Hung, Yuting Ma, Eder G. Lomeli, Jian Qin, Yi Cui () and Zhenan Bao ()
Additional contact information
Zhiao Yu: Stanford University
Hansen Wang: Stanford University
Xian Kong: Stanford University
William Huang: Stanford University
Yuchi Tsao: Stanford University
David G. Mackanic: Stanford University
Kecheng Wang: Stanford University
Xinchang Wang: Xiamen University
Wenxiao Huang: Stanford University
Snehashis Choudhury: Stanford University
Yu Zheng: Stanford University
Chibueze V. Amanchukwu: Stanford University
Samantha T. Hung: Stanford University
Yuting Ma: Stanford University
Eder G. Lomeli: Stanford University
Jian Qin: Stanford University
Yi Cui: Stanford University
Zhenan Bao: Stanford University

Nature Energy, 2020, vol. 5, issue 7, 526-533

Abstract: Abstract Electrolyte engineering is critical for developing Li metal batteries. While recent works improved Li metal cyclability, a methodology for rational electrolyte design remains lacking. Herein, we propose a design strategy for electrolytes that enable anode-free Li metal batteries with single-solvent single-salt formations at standard concentrations. Rational incorporation of –CF2– units yields fluorinated 1,4-dimethoxylbutane as the electrolyte solvent. Paired with 1 M lithium bis(fluorosulfonyl)imide, this electrolyte possesses unique Li–F binding and high anion/solvent ratio in the solvation sheath, leading to excellent compatibility with both Li metal anodes (Coulombic efficiency ~ 99.52% and fast activation within five cycles) and high-voltage cathodes (~6 V stability). Fifty-μm-thick Li|NMC batteries retain 90% capacity after 420 cycles with an average Coulombic efficiency of 99.98%. Industrial anode-free pouch cells achieve ~325 Wh kg−1 single-cell energy density and 80% capacity retention after 100 cycles. Our design concept for electrolytes provides a promising path to high-energy, long-cycling Li metal batteries.

Date: 2020
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DOI: 10.1038/s41560-020-0634-5

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