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External-pressure–electrochemistry coupling in solid-state lithium metal batteries

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Abstract

Solid-state lithium metal batteries (SSLBs) using inorganic solid-state electrolytes (SSEs) have attracted extensive scientific and commercial interest owing to their potential to provide higher energy density and safety than conventional Li-ion batteries. These batteries are subject to external pressure during both their manufacturing processes (fabrication pressure) and their operation (stack pressure). This pressure not only affects the intrinsic properties of both the electrolytes (such as ionic conductivity and electrochemical voltage window) and the electrodes (such as ion transport and structural variation) but also determines the cyclability and safety of the whole battery. Hence, understanding the effect of pressure is essential when designing high-performance SSLBs. This Review aims to elucidate the coupling between external pressure and electrochemistry in these batteries. We summarize the effects of external pressure on SSEs and electrodes, and on the interfaces between the components. We analyse the overall electrochemical performance and safety of the batteries under external pressure. Finally, we clarify the dominant challenges in achieving pressure-proof and low-pressure SSLBs, laying out a perspective for future breakthroughs.

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Fig. 1: Sources of external pressure in solid-state lithium metal batteries.
Fig. 2: External-pressure-derived deformation and contact.
Fig. 3: Effect of external pressure on Li creep.
Fig. 4: Effects of external pressure on the deposition morphology and dendrite growth of Li metal anode.
Fig. 5: Structural changes under external pressure.
Fig. 6: Effects of external pressure on electrode–electrolyte interfacial reactions.
Fig. 7: Effects of external pressures on the performance of SSEs and SSLBs.

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Acknowledgements

B.L. acknowledges support by National Nature Science Foundation of China (no. 52072208 and no. 52261160384), the Shenzhen Science and Technology Program (KCXFZ20211020163810015), the Fundamental Research Project of Shenzhen (no. JCYJ20220818101004009), Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01N111) and Shenzhen Outstanding Talents Training Fund. G.W. acknowledges support by the Australian Research Council through the ARC Discovery projects (DP210101389 and DP230101579), ARC Linkage project (LP200200926) and ARC Research Hub for Integrated Energy Storage Solutions (IH180100020).

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  1. These authors contributed equally: Xia Hu, Zhijia Zhang.

Authors and Affiliations

  1. Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China

    Xia Hu, Zhijia Zhang, Xiang Zhang, Yao Wang, Dong Zhou & Baohua Li

  2. School of Materials Science and Engineering, Tsinghua University, Beijing, China

    Xia Hu

  3. Centre for Clean Energy Technology, School of Mathematical and Physical Sciences, Faculty of Science, University of Technology Sydney, Sydney, New South Wales, Australia

    Zhijia Zhang, Xu Yang, Steven Langford & Guoxiu Wang

  4. Max Planck Institute for Chemical Physics of Solids, Topological Catalysis Group, Dresden, Germany

    Xia Wang

  5. Department of Chemistry and Bar-Ilan Institute of Nanotechnology and Advanced Materials, Bar-Ilan University, Ramat-Gan, Israel

    Miryam Fayena-Greenstein, Hadas Alon Yehezkel & Doron Aurbach

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All authors contributed to the discussion of content and writing of the manuscript, added substantial thoughts and revised the manuscript in a collaborative manner.

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Hu, X., Zhang, Z., Zhang, X. et al. External-pressure–electrochemistry coupling in solid-state lithium metal batteries. Nat Rev Mater (2024). https://doi.org/10.1038/s41578-024-00669-y

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