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Pressure-tailored lithium deposition and dissolution in lithium metal batteries

Abstract

Unregulated lithium (Li) growth is the major cause of low Coulombic efficiency, short cycle life and safety hazards for rechargeable Li metal batteries. Strategies that aim to achieve large granular Li deposits have been extensively explored, and yet it remains a challenge to achieve the ideal Li deposits, which consist of large Li particles that are seamlessly packed on the electrode and can be reversibly deposited and stripped. Here we report a dense Li deposition (99.49% electrode density) with an ideal columnar structure that is achieved by controlling the uniaxial stack pressure during battery operation. Using multiscale characterization and simulation, we elucidate the critical role of stack pressure on Li nucleation, growth and dissolution processes and propose a Li-reservoir-testing protocol to maintain the ideal Li morphology during extended cycling. The precise manipulation of Li deposition and dissolution is a critical step to enable fast charging and a low-temperature operation for Li metal batteries.

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Fig. 1: Quantifying the pressure effects on Li metal anode CE and plating morphology.
Fig. 2: MD simulation and schematic illustration of pressure effects on Li nucleation and growth.
Fig. 3: Pressure effects on SEI properties by cryo-TEM.
Fig. 4: Pressure effect on Li stripping process.

Data availability

All the data generated in this study are included in the published article and its supplementary information. Source data are provided with this paper.

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Acknowledgements

This work was supported by the Office of Vehicle Technologies of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) under contract DE-EE0007764. Cryo-FIB was performed at the San Diego Nanotechnology Infrastructure (SDNI), a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the National Science Foundation (grant ECCS-1542148). We acknowledge the UC Irvine Materials Research Institute (IMRI) for the use of the cryo-TEM, funded in part by the National Science Foundation Major Research Instrumentation Program under grant CHE-1338173. Idaho National Laboratory is operated by Battelle Energy Alliance under contract no. DE-AC07-05ID14517 for the US Department of Energy. The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US Government purposes. We thank J. K. Greene for the lithium surface coverage area data analysis, and Y. Lin for the simulation results discussion.

Author information

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Authors

Contributions

C.F. and Y.S.M. conceived the ideas. C.F. designed the experiments. B. Lu implemented the electrochemical tests. B. Lu, C.F. and D.C. performed the cryo-FIB experiments. G.P. and B. Liaw performed the MD simulations. M.Z. collected the cryo-TEM data. C.F. conducted TEM data interpretation. S.C. and M. Cai conducted the pouch cell tests. M. Ceja prepared the electrolytes. J.-M.D. conducted the load-cell design and calibration. C.F. wrote the manuscript. All the authors discussed the results and commented on the manuscript. All the authors gave approval to the final version of the manuscript.

Corresponding authors

Correspondence to Chengcheng Fang, Boryann Liaw or Ying Shirley Meng.

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Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature Energy thanks Venkatasubramanian Viswanathan for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Discussion, Figs. 1–17 and Table 1.

Supplementary Video 1

Cryo-FIB-SEM 3D reconstruction of deposited Li at 70 kPa, 2 mA cm2 for 0.333 mAh cm2.

Supplementary Video 2

Cryo-FIB-SEM 3D reconstruction of deposited Li at 350 kPa, 2 mA cm2 for 0.333 mAh cm2.

Source data

Source Data Fig. 1

Battery cycling data for each data point in Fig. 1b.

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Fang, C., Lu, B., Pawar, G. et al. Pressure-tailored lithium deposition and dissolution in lithium metal batteries. Nat Energy 6, 987–994 (2021). https://doi.org/10.1038/s41560-021-00917-3

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