Balancing interfacial reactions to achieve long cycle life in high-energy lithium metal batteries

Chaojiang Niu, Dianying Liu, Joshua A. Lochala, Cassidy S. Anderson, Xia Cao, Mark E. Gross, Wu Xu, Ji-Guang Zhang, M. Stanley Whittingham, Jie Xiao () and Jun Liu ()
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Chaojiang Niu: Pacific Northwest National Laboratory
Dianying Liu: Pacific Northwest National Laboratory
Joshua A. Lochala: Pacific Northwest National Laboratory
Cassidy S. Anderson: Pacific Northwest National Laboratory
Xia Cao: Pacific Northwest National Laboratory
Mark E. Gross: Pacific Northwest National Laboratory
Wu Xu: Pacific Northwest National Laboratory
Ji-Guang Zhang: Pacific Northwest National Laboratory
M. Stanley Whittingham: Binghamton University
Jie Xiao: Pacific Northwest National Laboratory
Jun Liu: Pacific Northwest National Laboratory

Nature Energy, 2021, vol. 6, issue 7, 723-732

Abstract: Abstract The rechargeable lithium metal battery has attracted wide attention as a next-generation energy storage technology. However, simultaneously achieving high cell-level energy density and long cycle life in realistic batteries is still a great challenge. Here we investigate the degradation mechanisms of Li || LiNi0.6Mn0.2Co0.2O2 pouch cells and present fundamental linkages among Li thickness, electrolyte depletion and the structure evolution of solid–electrolyte interphase layers. Different cell failure processes are discovered when tuning the anode to cathode capacity ratio in compatible electrolytes. An optimal anode to cathode capacity ratio of 1:1 emerges because it balances well the rates of Li consumption, electrolyte depletion and solid–electrolyte interphase construction, thus decelerating the increase of cell polarization and extending cycle life. Contrary to conventional wisdom, long cycle life is observed by using ultra-thin Li (20 µm) in balanced cells. A prototype 350 Wh kg−1 pouch cell (2.0 Ah) achieves over 600 long stable cycles with 76% capacity retention without a sudden cell death.

Date: 2021
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DOI: 10.1038/s41560-021-00852-3

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