Anion-enrichment interface enables high-voltage anode-free lithium metal batteries

Minglei Mao, Xiao Ji, Qiyu Wang, Zejing Lin, Meiying Li, Tao Liu, Chengliang Wang, Yong-Sheng Hu, Hong Li, Xuejie Huang, Liquan Chen and Liumin Suo ()
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Minglei Mao: Beijing National Laboratory for Condensed Matter Physics
Xiao Ji: Huazhong University of Science and Technology
Qiyu Wang: Beijing National Laboratory for Condensed Matter Physics
Zejing Lin: Beijing National Laboratory for Condensed Matter Physics
Meiying Li: Beijing National Laboratory for Condensed Matter Physics
Tao Liu: Beijing National Laboratory for Condensed Matter Physics
Chengliang Wang: Huazhong University of Science and Technology
Yong-Sheng Hu: Beijing National Laboratory for Condensed Matter Physics
Hong Li: Beijing National Laboratory for Condensed Matter Physics
Xuejie Huang: Beijing National Laboratory for Condensed Matter Physics
Liquan Chen: Beijing National Laboratory for Condensed Matter Physics
Liumin Suo: Beijing National Laboratory for Condensed Matter Physics

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Aggressive chemistry involving Li metal anode (LMA) and high-voltage LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode is deemed as a pragmatic approach to pursue the desperate 400 Wh kg−1. Yet, their implementation is plagued by low Coulombic efficiency and inferior cycling stability. Herein, we propose an optimally fluorinated linear carboxylic ester (ethyl 3,3,3-trifluoropropanoate, FEP) paired with weakly solvating fluoroethylene carbonate and dissociated lithium salts (LiBF4 and LiDFOB) to prepare a weakly solvating and dissociated electrolyte. An anion-enrichment interface prompts more anions’ decomposition in the inner Helmholtz plane and higher reduction potential of anions. Consequently, the anion-derived interface chemistry contributes to the compact and columnar-structure Li deposits with a high CE of 98.7% and stable cycling of 4.6 V NCM811 and LiCoO2 cathode. Accordingly, industrial anode-free pouch cells under harsh testing conditions deliver a high energy of 442.5 Wh kg−1 with 80% capacity retention after 100 cycles.

Date: 2023
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DOI: 10.1038/s41467-023-36853-x

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