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


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.

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The data that support the plots within this paper and other findings of this study are available from the corresponding author on reasonable request.

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This research was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy (DoE) through the Advanced Battery Materials Research Program (Battery500 Consortium). SEM and XRD analyses were conducted in the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DoE's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated by Battelle for the DoE under contract DE-AC05-76RLO1830. We thank L. Luo, Y. He and C. Wang of the PNNL for TEM characterizations.

Author information

J.X. and J.L. proposed the research. C.N. assembled the pouch cells, performed the electrochemical measurements and carried out the characterizations with assistance from H.L. The compatible electrolyte was developed by S.C., W.X. and J.-G.Z. Q.L. and J.D. helped with cell assembly. M.S.W. participated in data analyses and discussion. C.N., H.L., J.X. and J.L. co-wrote the manuscript with input from all authors.

Competing interests

The authors declare no competing interests.

Correspondence to Jie Xiao or Jun Liu.

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Fig. 1: 300 Wh kg−1 Li metal pouch cell at 1.0 Ah level.
Fig. 2: Characterization of 300 Wh kg−1 Li||NMC622 pouch cells with two different electrolytes.
Fig. 3: Cycling of the 300 Wh kg−1 Li||NMC622 pouch cell with uniform external pressure in a compatible electrolyte.
Fig. 4: Post-cycling characterization of Li metal anodes in the 300 Wh kg−1 Li||NMC622 pouch cell, with a compatible electrolyte and uniform external pressure.
Fig. 5: Structural evolution of the Li metal anode in high-energy Li metal pouch cells.