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Sequencing polymers to enable solid-state lithium batteries

Nature Materials volume 22, pages 1515–1522 (2023)Cite this article

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Abstract

Rational designs of solid polymer electrolytes with high ion conduction are critical in enabling the creation of advanced lithium batteries. However, known polymer electrolytes have much lower ionic conductivity than liquid/ceramics at room temperature, which limits their practical use in batteries. Here we show that precise positioning of designed repeating units in alternating polymer sequences lays the foundation for homogenized Li+ distribution, non-aggregated Li+-anion solvation and sequence-assisted site-to-site ion migration, facilitating the tuning of Li+ conductivity by up to three orders of magnitude. The assembled all-solid-state batteries facilitate reversible and dendrite-mitigated cycling against Li metal from ambient to elevated temperatures. This work demonstrates a powerful molecular engineering means to access highly ion-conductive solid-state materials for next-generation energy devices.

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Fig. 1: Illustration of Li+ transport patterns during battery charging in different polymer electrolyte systems.
Fig. 2: Synthesis of alter-SIPE.
Fig. 3: Analysis of Li+ dissociation in different polymer sequences.
Fig. 4: Tailoring polymer structures and characterizations of thermal, Li+ transport and mechanical properties.
Fig. 5: Investigation of transport pathway and Li+ conduction.
Fig. 6: Dendrite-suppression behaviour and battery performance from ambient to elevated temperatures.

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Source data are provided with this paper. Additional data supporting the findings of this study are included in the Supplementary Information.

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Acknowledgements

This research was financially supported by the National Natural Science Foundation of China (no. 21971044 to M.C. and 52003231 to X.L.), the Shanghai Pilot Program for Basic Research-Fudan University 21TQ1400100 (no. 21TQ007 to M.C.) and the State Key Laboratory of Molecular Engineering of Polymers and Duke Kunshan University. We thank J. A. Johnson for helpful discussions.

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Authors and Affiliations

  1. State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai, China

    Shantao Han, Peng Wen, Huaijiao Wang, Yang Zhou, Yu Gu, Lu Zhang & Mao Chen

  2. Department of Materials Science and Engineering, Research Laboratory of Electronics, Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Yang Shao-Horn

  3. Division of Natural and Applied Sciences, Duke Kunshan University, Kunshan, China

    Xinrong Lin

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  1. Shantao Han
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Contributions

S.H., X.L. and M.C. conceived the idea and designed the experiments. S.H. conducted major experiments and prepared the draft article. S.H. and X.L. contributed molecular dynamic simulations. P.W. and Y.Z. contributed DFT calculations. S.H., H.W., Y.G. and L.Z. conducted materials characterizations. S.H., Y.S.-H., X.L. and M.C. interpreted the data and completed the final manuscript writing.

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Correspondence to Yang Shao-Horn, Xinrong Lin or Mao Chen.

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Nature Materials thanks Renaud Bouchet and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Han, S., Wen, P., Wang, H. et al. Sequencing polymers to enable solid-state lithium batteries. Nat. Mater. 22, 1515–1522 (2023). https://doi.org/10.1038/s41563-023-01693-z

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