Weakly coordinated Li ion in single-ion-conductor-based composite enabling low electrolyte content Li-metal batteries

Hyeokjin Kwon, Hyun-Ji Choi, Jung-kyu Jang, Jinhong Lee, Jinkwan Jung, Wonjun Lee, Youngil Roh, Jaewon Baek, Dong Jae Shin, Ju-Hyuk Lee, Nam-Soon Choi (), Ying Shirley Meng () and Hee-Tak Kim ()
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Hyeokjin Kwon: Korea Advanced Institute of Science and Technology (KAIST)
Hyun-Ji Choi: Korea Advanced Institute of Science and Technology (KAIST)
Jung-kyu Jang: Korea Research Institute of Chemical Technology (KRICT)
Jinhong Lee: Korea Advanced Institute of Science and Technology (KAIST)
Jinkwan Jung: Korea Advanced Institute of Science and Technology (KAIST)
Wonjun Lee: Ulsan National Institute of Science and Technology (UNIST)
Youngil Roh: Korea Advanced Institute of Science and Technology (KAIST)
Jaewon Baek: Korea Advanced Institute of Science and Technology (KAIST)
Dong Jae Shin: Korea Advanced Institute of Science and Technology (KAIST)
Ju-Hyuk Lee: Korea Advanced Institute of Science and Technology (KAIST)
Nam-Soon Choi: Korea Advanced Institute of Science and Technology (KAIST)
Ying Shirley Meng: University of California at San Diego
Hee-Tak Kim: Korea Advanced Institute of Science and Technology (KAIST)

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract The pulverization of lithium metal electrodes during cycling recently has been suppressed through various techniques, but the issue of irreversible consumption of the electrolyte remains a critical challenge, hindering the progress of energy-dense lithium metal batteries. Here, we design a single-ion-conductor-based composite layer on the lithium metal electrode, which significantly reduces the liquid electrolyte loss via adjusting the solvation environment of moving Li+ in the layer. A Li||Ni0.5Mn0.3Co0.2O2 pouch cell with a thin lithium metal (N/P of 2.15), high loading cathode (21.5 mg cm−2), and carbonate electrolyte achieves 400 cycles at the electrolyte to capacity ratio of 2.15 g Ah−1 (2.44 g Ah−1 including mass of composite layer) or 100 cycles at 1.28 g Ah−1 (1.57 g Ah−1 including mass of composite layer) under a stack pressure of 280 kPa (0.2 C charge with a constant voltage charge at 4.3 V to 0.05 C and 1.0 C discharge within a voltage window of 4.3 V to 3.0 V). The rational design of the single-ion-conductor-based composite layer demonstrated in this work provides a way forward for constructing energy-dense rechargeable lithium metal batteries with minimal electrolyte content.

Date: 2023
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DOI: 10.1038/s41467-023-39673-1

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