Rational solvent molecule tuning for high-performance lithium metal battery electrolytes

Zhiao Yu, Paul E. Rudnicki, Zewen Zhang, Zhuojun Huang, Hasan Celik, Solomon T. Oyakhire, Yuelang Chen, Xian Kong, Sang Cheol Kim, Xin Xiao, Hansen Wang, Yu Zheng, Gaurav A. Kamat, Mun Sek Kim, Stacey F. Bent, Jian Qin (), Yi Cui () and Zhenan Bao ()
Additional contact information
Zhiao Yu: Stanford University
Paul E. Rudnicki: Stanford University
Zewen Zhang: Stanford University
Zhuojun Huang: Stanford University
Hasan Celik: University of California
Solomon T. Oyakhire: Stanford University
Yuelang Chen: Stanford University
Xian Kong: Stanford University
Sang Cheol Kim: Stanford University
Xin Xiao: Stanford University
Hansen Wang: Stanford University
Yu Zheng: Stanford University
Gaurav A. Kamat: Stanford University
Mun Sek Kim: Stanford University
Stacey F. Bent: Stanford University
Jian Qin: Stanford University
Yi Cui: Stanford University
Zhenan Bao: Stanford University

Nature Energy, 2022, vol. 7, issue 1, 94-106

Abstract: Abstract Electrolyte engineering improved cycling of Li metal batteries and anode-free cells at low current densities; however, high-rate capability and tuning of ionic conduction in electrolytes are desirable yet less-studied. Here, we design and synthesize a family of fluorinated-1,2-diethoxyethanes as electrolyte solvents. The position and amount of F atoms functionalized on 1,2-diethoxyethane were found to greatly affect electrolyte performance. Partially fluorinated, locally polar –CHF2 is identified as the optimal group rather than fully fluorinated –CF3 in common designs. Paired with 1.2 M lithium bis(fluorosulfonyl)imide, these developed single-salt-single-solvent electrolytes simultaneously enable high conductivity, low and stable overpotential, >99.5% Li||Cu half-cell efficiency (up to 99.9%, ±0.1% fluctuation) and fast activation (Li efficiency >99.3% within two cycles). Combined with high-voltage stability, these electrolytes achieve roughly 270 cycles in 50-μm-thin Li||high-loading-NMC811 full batteries and >140 cycles in fast-cycling Cu||microparticle-LiFePO4 industrial pouch cells under realistic testing conditions. The correlation of Li+–solvent coordination, solvation environments and battery performance is investigated to understand structure–property relationships.

Date: 2022
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DOI: 10.1038/s41560-021-00962-y

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