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Electrolyte melt infiltration for scalable manufacturing of inorganic all-solid-state lithium-ion batteries

Nature Materials volume 20, pages 984–990 (2021)Cite this article

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Abstract

All-solid-state lithium (Li) metal and lithium-ion batteries (ASSLBs) with inorganic solid-state electrolytes offer improved safety for electric vehicles and other applications. However, current inorganic ASSLB manufacturing technology suffers from high cost, excessive amounts of solid-state electrolyte and conductive additives, and low attainable volumetric energy density. Such a fabrication method involves separate fabrications of sintered ceramic solid-state electrolyte membranes and ASSLB electrodes, which are then carefully stacked and sintered together in a precisely controlled environment. Here we report a disruptive manufacturing technology that offers reduced manufacturing costs and improved volumetric energy density in all solid cells. Our approach mimics the low-cost fabrication of commercial Li-ion cells with liquid electrolytes, except that we utilize solid-state electrolytes with low melting points that are infiltrated into dense, thermally stable electrodes at moderately elevated temperatures (~300 °C or below) in a liquid state, and which then solidify during cooling. Nearly the same commercial equipment could be used for electrode and cell manufacturing, which substantially reduces a barrier for industry adoption. This energy-efficient method was used to fabricate inorganic ASSLBs with LiNi0.33Mn0.33Co0.33O2 cathodes and both Li4Ti5O12 and graphite anodes. The promising performance characteristics of such cells open new opportunities for the accelerated adoption of ASSLBs for safer electric transportation.

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Fig. 1: Schematics of melt infiltration.
Fig. 2: Characterization of the electrodes’ morphology after the melt infiltration.
Fig. 3: Microstructural and thermal characterization of the SSE and the electrode materials before and after the melt infiltration.
Fig. 4: Electrochemical performance of NCM111/LTO ASSLBs fabricated by melt-infiltration technology.
Fig. 5: Electrochemical performance of NCM111/graphite ASSLBs fabricated by melt-infiltration technology.

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Data availability

The data used in this study are available from the authors upon reasonable request.

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Acknowledgements

This work was mostly supported by Sila Nanotechnologies. We thank the Materials Characterization Center (MCF) at Georgia Tech.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, USA

    Yiran Xiao, Kostiantyn Turcheniuk, Aashray Narla, Ah-Young Song, Xiaolei Ren, Alexandre Magasinski, Ayush Jain, Shirley Huang, Haewon Lee & Gleb Yushin

  2. College of Environment and Resources, Chongqing Technology and Business University, Chongqing, China

    Xiaolei Ren

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Contributions

Y.X. performed battery assembly and electrochemical tests; Y.X., K.T., A.N., A.S., X.R., A.M., A.J., S.H. and H.L. performed materials synthesis and characterization; Y.X., K.T., A.S. and G.Y. interpreted the experimental results and wrote the paper. G.Y. conceived the idea.

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Correspondence to Gleb Yushin.

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G.Y. is a stockholder of Sila Nanotechnologies.

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Supplementary Information

Supplementary Figs. 1–13 and caption of Video 1.

Supplementary Video 1

Melt-infiltration process of SSE into an NCM111 electrode.

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Xiao, Y., Turcheniuk, K., Narla, A. et al. Electrolyte melt infiltration for scalable manufacturing of inorganic all-solid-state lithium-ion batteries. Nat. Mater. 20, 984–990 (2021). https://doi.org/10.1038/s41563-021-00943-2

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