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All-solid-state lithium–sulfur batteries through a reaction engineering lens

Nature Chemical Engineering volume 1, pages 400–410 (2024)Cite this article

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Abstract

All-solid-state lithium–sulfur (Li–S) batteries have emerged as a promising energy storage solution due to their potential high energy density, cost effectiveness and safe operation. Gaining a deeper understanding of sulfur redox in the solid state is critical for advancing all-solid-state Li–S battery technology. In particular, the key electrochemical reactions of solid-state sulfur are distinct from those in the liquid state, yet discussion of such aspects remains lacking thus far. This Perspective provides a fundamental overview of all-solid-state Li–S batteries by delving into the underlying redox mechanisms of solid-state sulfur, placing a specific emphasis on key reaction engineering principles, such as mass transport, electrochemical kinetics and thermodynamics. The dimensionless Damköhler number is underscored to elucidate transport and kinetics limitations in solid-state sulfur. Furthermore, advanced characterization techniques, such as cryogenic electron microscopy, are highlighted as powerful tools to bridge the current gaps in understanding that limit the deployment of all-solid-state Li–S batteries.

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Fig. 1: Comparing liquid Li–S batteries with all-solid-state Li–S batteries.
Fig. 2: Comparing the conversion mechanism of sulfur during discharge in liquid and solid-state electrolytes.
Fig. 3: Mapping the conversion pathway of sulfur in liquid and all-solid-state configurations.
Fig. 4: Schematic illustrations highlighting various unresolved questions concerning the discharge/charge products of all-solid-state Li–S batteries.
Fig. 5: Characterization tools for all-solid-state Li–S batteries.

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Acknowledgements

J.T.K. thanks J. Peterson, S. Srivastava and J. B. Jang for fruitful discussions regarding the Damköhler number.

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  1. These authors contributed equally: Jung Tae Kim, Han Su, Yu Zhong.

Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA, USA

    Jung Tae Kim, Chongzhen Wang, Haoyang Wu, Dingyi Zhao & Yuzhang Li

  2. Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada

    Han Su, Changhong Wang & Xueliang Sun

  3. State Key Laboratory of Silicon and Advanced Semiconductor Materials, Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, School of Materials Science and Engineering, Zhejiang University, Hangzhou, People’s Republic of China

    Han Su & Yu Zhong

  4. Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo, People’s Republic of China

    Changhong Wang & Xueliang Sun

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Contributions

J.T.K., Y.L. and Changhong Wang. conceived the Perspective. J.T.K. wrote the paper. Changhong Wang. conducted the gravimetric energy density calculations. Y.Z. drew the schematic illustrations. Y.L., Changhong Wang. and X.S. supervised the project. All authors reviewed, edited and enriched each section of the paper.

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Correspondence to Changhong Wang, Xueliang Sun or Yuzhang Li.

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Supplementary Fig. 1, Notes 1–3, Table 1 and refs. 1–19.

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Kim, J.T., Su, H., Zhong, Y. et al. All-solid-state lithium–sulfur batteries through a reaction engineering lens. Nat Chem Eng 1, 400–410 (2024). https://doi.org/10.1038/s44286-024-00079-5

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