Interface chemistry of an amide electrolyte for highly reversible lithium metal batteries

Qidi Wang, Zhenpeng Yao, Chenglong Zhao, Tomas Verhallen, Daniel P. Tabor, Ming Liu, Frans Ooms, Feiyu Kang, Alán Aspuru-Guzik, Yong-Sheng Hu, Marnix Wagemaker () and Baohua Li ()
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Qidi Wang: Tsinghua University
Zhenpeng Yao: Harvard University
Chenglong Zhao: Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Tomas Verhallen: Delft University of Technology
Daniel P. Tabor: Harvard University
Ming Liu: Delft University of Technology
Frans Ooms: Delft University of Technology
Feiyu Kang: Tsinghua University
Alán Aspuru-Guzik: Harvard University
Yong-Sheng Hu: Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
Marnix Wagemaker: Delft University of Technology
Baohua Li: Tsinghua University

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: Abstract Metallic lithium is a promising anode to increase the energy density of rechargeable lithium batteries. Despite extensive efforts, detrimental reactivity of lithium metal with electrolytes and uncontrolled dendrite growth remain challenging interconnected issues hindering highly reversible Li-metal batteries. Herein, we report a rationally designed amide-based electrolyte based on the desired interface products. This amide electrolyte achieves a high average Coulombic efficiency during cycling, resulting in an outstanding capacity retention with a 3.5 mAh cm−2 high-mass-loaded LiNi0.8Co0.1Mn0.1O2 cathode. The interface reactions with the amide electrolyte lead to the predicted solid electrolyte interface species, having favorable properties such as high ionic conductivity and high stability. Operando monitoring the lithium spatial distribution reveals that the highly reversible behavior is related to denser deposition as well as top-down stripping, which decreases the formation of porous deposits and inactive lithium, providing new insights for the development of interface chemistries for metal batteries.

Date: 2020
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DOI: 10.1038/s41467-020-17976-x

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