High-energy lithium metal pouch cells with limited anode swelling and long stable cycles

Chaojiang Niu, Hongkyung Lee, Shuru Chen, Qiuyan Li, Jason Du, Wu Xu, Ji-Guang Zhang, M. Stanley Whittingham, Jie Xiao () and Jun Liu ()
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Chaojiang Niu: Pacific Northwest National Laboratory
Hongkyung Lee: Pacific Northwest National Laboratory
Shuru Chen: Pacific Northwest National Laboratory
Qiuyan Li: Pacific Northwest National Laboratory
Jason Du: 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, 2019, vol. 4, issue 7, 551-559

Abstract: Abstract Lithium metal anodes have attracted much attention as candidates for high-energy batteries, but there have been few reports of long cycling behaviour, and the degradation mechanism of realistic high-energy Li metal cells remains unclear. Here, we develop a prototypical 300 Wh kg−1 (1.0 Ah) pouch cell by integrating a Li metal anode, a LiNi0.6Mn0.2Co0.2O2 cathode and a compatible electrolyte. Under small uniform external pressure, the cell undergoes 200 cycles with 86% capacity retention and 83% energy retention. In the initial 50 cycles, flat Li foil converts into large Li particles that are entangled in the solid-electrolyte interphase, which leads to rapid volume expansion of the anode (cell thickening of 48%). As cycling continues, the external pressure helps the Li anode maintain good contact between the Li particles, which ensures a conducting percolation pathway for both ions and electrons, and thus the electrochemical reactions continue to occur. Accordingly, the solid Li particles evolve into a porous structure, which manifests in substantially reduced cell swelling by 19% in the subsequent 150 cycles.

Date: 2019
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DOI: 10.1038/s41560-019-0390-6

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