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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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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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.
The authors declare no competing interests.
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Additional experimental details and Supplementary Notes 1–10, Figs. 1–39 and Tables 1–6.
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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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