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

Cheng-Dong Fang, Ying Huang, Yi-Fan Sun, Peng-Fei Sun, Ke Li, Shu-Yang Yao, Min-Yi Zhang, Wei-Hui Fang () and Jia-Jia Chen ()
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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

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-51191-2

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