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Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor

Author

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  • Cheng-Dong Fang

    (Xiamen University)

  • Ying Huang

    (Xiamen University)

  • Yi-Fan Sun

    (Chinese Academy of Sciences)

  • Peng-Fei Sun

    (Xiamen University)

  • Ke Li

    (Xiamen University)

  • Shu-Yang Yao

    (Chinese Academy of Sciences)

  • Min-Yi Zhang

    (Chinese Academy of Sciences)

  • Wei-Hui Fang

    (Chinese Academy of Sciences)

  • Jia-Jia Chen

    (Xiamen University)

Abstract

Understanding the Li-ions conduction network and transport dynamics in polymer electrolyte is crucial for developing reliable all-solid-state batteries. In this work, advanced nano- X-ray computed tomography combined with Raman spectroscopy and solid state nuclear magnetic resonance are used to multi-scale qualitatively and quantitatively reveal ion conduction network of poly(ethylene) oxide (PEO)-based electrolyte (from atomic, nano to macroscopic level). With the clear mapping of the microstructural heterogeneities of the polymer segments, aluminium-oxo molecular clusters (AlOC) are used to reconstruct a high-efficient conducting network with high available Li-ions (76.7%) and continuous amorphous domains via the strong supramolecular interactions. Such superionic PEO conductor (PEO-LiTFSI-AlOC) exhibites a molten-like Li-ion conduction behaviour among the whole temperature range and delivers an ionic conductivity of 1.87 × 10−4 S cm−1 at 35 °Ϲ. This further endows Li electrochemical plating/stripping stability under 50 μA cm−2 and 50 μAh cm−2 over 2000 h. The as-built Li|PEO-LiTFSI-AlOC|LiFePO4 full batteries show a high rate performance and a capacity retention more than 90% over 200 cycling at 250 μA cm−2, even enabling a high-loading LiFePO4 cathode of 16.8 mg cm−2 with a specific capacity of 150 mAh g−1 at 50 °Ϲ.

Suggested Citation

  • Cheng-Dong Fang & Ying Huang & Yi-Fan Sun & Peng-Fei Sun & Ke Li & Shu-Yang Yao & Min-Yi Zhang & Wei-Hui Fang & Jia-Jia Chen, 2024. "Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51191-2
    DOI: 10.1038/s41467-024-51191-2
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    1. Yun Su & Xiaohui Rong & Ang Gao & Yuan Liu & Jianwei Li & Minglei Mao & Xingguo Qi & Guoliang Chai & Qinghua Zhang & Liumin Suo & Lin Gu & Hong Li & Xuejie Huang & Liquan Chen & Binyuan Liu & Yong-She, 2022. "Rational design of a topological polymeric solid electrolyte for high-performance all-solid-state alkali metal batteries," Nature Communications, Nature, vol. 13(1), pages 1-15, December.
    2. Christoph Busche & Laia Vilà-Nadal & Jun Yan & Haralampos N. Miras & De-Liang Long & Vihar P. Georgiev & Asen Asenov & Rasmus H. Pedersen & Nikolaj Gadegaard & Muhammad M. Mirza & Douglas J. Paul & Jo, 2014. "Design and fabrication of memory devices based on nanoscale polyoxometalate clusters," Nature, Nature, vol. 515(7528), pages 545-549, November.
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