4.8 Article

Intrinsic Nonflammable Ether Electrolytes for Ultrahigh-Voltage Lithium Metal Batteries Enabled by Chlorine Functionality

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 32, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202203693

Keywords

Chlorine Functionality; Ether Electrolytes; High-Voltage Stability; Li Metal Batteries; Nonflammable

Funding

  1. National Key R&D Program of China [2017YFA0206703]
  2. National Natural Science Foundation of China [22179124, 21905265]
  3. Fundamental Research Funds for the Central Universities [WK3430000007, WK2060140026]

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A rationally designed ether-based electrolyte with chlorine functionality is reported to address the issues of low anodic stability and high flammability in high-voltage lithium metal batteries. The chloroether-based electrolyte shows high Li Coulombic efficiency and capacity retention, and possesses nonflammable safety feature due to the flame-retarding ability of chlorine functional groups. This study offers a new approach for enabling ether-based electrolytes in high energy density, long-life, and safe Li metal batteries.
The issues of inherent low anodic stability and high flammability hinder the deployment of the ether-based electrolytes in practical high-voltage lithium metal batteries. Here, we report a rationally designed ether-based electrolyte with chlorine functionality on ether molecular structure to address these critical challenges. The chloroether-based electrolyte demonstrates a high Li Coulombic efficiency of 99.2 % and a high capacity retention >88 % over 200 cycles for Ni-rich cathodes at an ultrahigh cut-off voltage of 4.6 V (stable even up to 4.7 V). The chloroether-based electrolyte not only greatly improves electrochemical stabilities of Ni-rich cathodes under ultrahigh voltages with interphases riched in LiF and LiCl, but possesses the intrinsic nonflammable safety feature owing to the flame-retarding ability of chlorine functional groups. This study offers a new approach to enable ether-based electrolytes for high energy density, long-life and safe Li metal batteries.

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