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Inorganic glass electrolytes with polymer-like viscoelasticity

Nature Energy volume 8, pages 1221–1228 (2023)Cite this article

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Abstract

Solid-state batteries offer an alternative promising power source for electric vehicles. However, the interfacial mechanical stability of inorganic electrolytes is inferior to that of organic electrolytes. A high stack pressure (several to hundreds of megapascals) is often required to maintain intimate contact with electrodes. Here we report a class of viscoelastic inorganic glass (VIGLAS) to serve as solid electrolytes by simply replacing chlorine of tetrachloroaluminates with oxygen. The VIGLAS possesses high ionic conductivity (~1 mS cm−1 at 30 °C) for both Li+ and Na+, superior chemo-mechanical compatibility with 4.3 V cathodes and the ability to enable pressure-less Li- and Na-based solid-state batteries (<0.1 MPa). The low melting temperature (<160 °C) allows the electrolytes to efficiently infiltrate electrode materials, akin to a liquid battery. Additionally, the deformability of the electrolytes facilitates the feasibility of scale-up through the production of thin films via a rolling process.

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Fig. 1: Polymer-like characteristics of MACO.
Fig. 2: Li+ transport mechanism in LACO75 simulated by AIMD at 300 K.
Fig. 3: Electrochemical performance of MACO in SSBs.
Fig. 4: Processability and cost-effectiveness of MACO.

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Data availability

The data that support the findings of this study are available within this article and its Supplementary Information.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (52122214) and the Youth Innovation Promotion Association of the Chinese Academy of Sciences (2020006). We thank H. Chen and W. Yin at the Spallation Neutron Source Science Center (SNSSC), Dongguan, China for their great support with the neutron total scattering experiments.

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Authors and Affiliations

  1. Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Tao Dai, Siyuan Wu, Yaxiang Lu, Yang Yang, Yuan Liu, Chao Chang, Xiaohui Rong, Ruijuan Xiao, Yanhui Liu, Weihua Wang, Liquan Chen & Yong-Sheng Hu

  2. College of Materials Science and Optoelectronic Technology, University of Chinese Academy of Sciences, Beijing, China

    Yaxiang Lu & Yong-Sheng Hu

  3. Huairou Division, Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Yaxiang Lu, Xiaohui Rong & Yong-Sheng Hu

  4. Yangtze River Delta Physics Research Center Co. Ltd., Liyang, China

    Yaxiang Lu & Yong-Sheng Hu

  5. Institute of Process Engineering, Chinese Academy of Sciences, Beijing, China

    Junmei Zhao

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  1. Tao Dai
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Contributions

Y.S.H. and T.D. conceived the research. T.D. performed the experiments with Y.X.L. T.D. determined the composition with J.Z. S.W. carried out the simulation work with R.X. Y.Y. and Y.L. completed the XPS experiments and analysed the NPD data. C.C. conducted the DMA tests with Y.L. and W.W. T.D., Y.X.L. and Y.S.H. wrote the manuscript. All authors participated in analysing the experimental results and preparing the manuscript.

Corresponding authors

Correspondence to Yaxiang Lu, Junmei Zhao or Yong-Sheng Hu.

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Competing interests

Y.S.H. is employed by HiNa Battery Technology Co. Ltd. The other authors declare no competing interests.

Peer review

Peer review information

Nature Energy thanks Naoto Tanibata, Thomas A. Yersak and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Notes 1–7, Figs. 1–25 and Tables 1–4.

Supplementary Video 1

A video showing the physical characteristics of liquid and solid MAlCl4.

Supplementary Video 2

A video showing the physical characteristics of liquid MACO75.

Supplementary Video 3

A video showing that MACO75 can be rolled into thin films.

Supplementary Video 4

A video demonstrating the flexibility of LACO75 film at room temperature by repetitive bending.

Supplementary Video 5

A video demonstrating the viscoelasticity of hardened LACO75. Continuous films were produced by scraping a hardened LACO75 rod.

Supplementary Data 1

The predicted phase equilibria regions of LACO75.

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Dai, T., Wu, S., Lu, Y. et al. Inorganic glass electrolytes with polymer-like viscoelasticity. Nat Energy 8, 1221–1228 (2023). https://doi.org/10.1038/s41560-023-01356-y

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