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Formation of hierarchically ordered structures in conductive polymers to enhance the performances of lithium-ion batteries

Nature Energy volume 8, pages 129–137 (2023)Cite this article

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Abstract

Electrically conductive polymers have found increasing applications in energy conversion and storage devices. In the conventional design of conductive polymers, organic functionalities are introduced via bottom-up synthetic approaches to enhance specific properties by modification of the individual polymers. Unfortunately, the addition of functional groups leads to conflicting effects, limiting their scaled synthesis and broad applications. Here we show a conductive polymer with simple primary building blocks that can be thermally processed to develop hierarchically ordered structures (HOS) with well-defined nanocrystalline morphologies. Our approach to constructing permanent HOS in conductive polymers leads to substantial enhancement of charge transport properties and mechanical robustness, which are critical for practical lithium-ion batteries. Finally, we demonstrate that conductive polymers with HOS enable exceptional cycling performance of full cells with high-loading micron-size SiOx-based anodes, delivering areal capacities of more than 3.0 mAh cm−2 over 300 cycles and average Coulombic efficiency of >99.95%.

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Fig. 1: Proposed chemical and morphological evolution of conductive polymers.
Fig. 2: The chemical and morphological evolution of multifunctional conductive polymers based on a controlled thermal process.
Fig. 3: Transport properties enhanced by HOS.
Fig. 4: Conductive polymers with HOS function in practical lithium-ion batteries.

Data availability

All datasets analysed and generated during the current study are available in the paper or Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work is primarily funded by the assistant secretary of energy efficiency in the Vehicle Technologies Office of the US Department of Energy under the I4-Lab programme. T.Z., C.F., Y.L., Y.F. and G.L. were supported by the Vehicle Technologies Office. H.S. and B.H.S. were supported by the Toyota Research Institute. Y.H., D.L., X.Z., C.O., C.Z., W.Y., A.M.M. and the Molecular Foundry and the Advanced Light Source were supported by the director of the Office of Science, Office of Basic Energy Sciences of the US Department of Energy under contract number DE-AC02-05CH11231.

Author information

Authors and Affiliations

  1. Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Tianyu Zhu, Chen Fang, Yanying Lu, Yanbao Fu & Gao Liu

  2. National Center for Electron Microscopy, The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Hadas Sternlicht, Dongye Liu, Benjamin H. Savitzky, Colin Ophus & Andrew M. Minor

  3. Department of Materials Science and Engineering, University of California, Berkeley, CA, USA

    Hadas Sternlicht, Dongye Liu, Xiao Zhao & Andrew M. Minor

  4. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Yang Ha, Chenhui Zhu & Wanli Yang

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  1. Tianyu Zhu
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Contributions

T.Z. and G.L. conceived and designed the experiments. C.O., C.Z., W.Y., A.M.M. and G.L. provided critical guidance on the experiments. H.S. provided important guidance on the TEM analysis and sample preparation. H.S. conducted the TEM experiments and 4D-STEM data collection. H.S. and B.H.S. conducted analysis of the 4D-STEM data. T.Z., Y.H., C.Z. and W.Y. performed the synchrotron-based measurements. D.L. performed mechanical testing. C.F. performed MALDI-TOF analysis. X.Z. performed atomic force microscopy and Raman spectroscopy for polymers. T.Z., Y.L and Y.F. performed battery fabrication and electrochemical testing. T.Z. performed all other experiments. T.Z. and G.L. wrote the first draft of the manuscript, and all the authors revised and approved the manuscript.

Corresponding author

Correspondence to Gao Liu.

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Nature Energy thanks Ali Coskun, Rafael Verduzco and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

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Additional experimental details and Supplementary Notes 1–10, Figs. 1–39 and Tables 1–6.

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Source Data Fig. 1

Unprocessed western blots.

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Zhu, T., Sternlicht, H., Ha, Y. et al. Formation of hierarchically ordered structures in conductive polymers to enhance the performances of lithium-ion batteries. Nat Energy 8, 129–137 (2023). https://doi.org/10.1038/s41560-022-01176-6

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