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Polymer electrolytes reinforced by 2D fluorinated filler for all-solid-state Li-Fe-F conversion-type lithium metal batteries

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Abstract

The polyethylene oxide (PEO) based solid-state batteries are considered as promising candidates for the next-generation Li metal batteries with high energy density and safety. However, the low Li-ion conductivity and high-voltage endurability hinder the further applications of PEO-based electrolytes. To overcome these issues, herein two-dimensional (2D) CeF3 nanoplates with maximally exposed [001] crystal faces are introduced into the PEO matrix to expand the electrochemical window and improve Li-ion conduction and transport. The optimized crystal shape and crystal face anisotropy of CeF3 nanoplate filler reduce the crystallinity of composite solid polymer electrolyte (CSPE) via its Lewis acid-base interaction with ether oxygen of PEO. The Li-affinity [100] and Li-repellent [001] crystal faces of CeF3 nanoplates synergistically realize the dissociation of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), fast Li-adsorption/desorption, and Li+ migration. The optimized CSPE-0.1CeF3 membrane enables the achievement of Li metal batteries with high endurability and stability, from the kinetically favorable Li/Li symmetric cells with long-term cycling over 8000 h. The highly reversible Li/LiFePO4 cells exhibit a capacity retention of 109.2 mAh·g−1 after 1000 cycles at 1 C, corresponding to a low capacity fading rate of 0.026% per cycle. The conversion-type all-solid-state Li/CSPE-0.1CeF3/FeF3 cells show a high reversible capacity of 201.9 mAh·g−1 after long-term 600 cycles and of 231.1 mAh·g−1 at an ultra-high rate of 5 C.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 21975276 and 52102329) and Shanghai Science and Technology Committee (No. 20520710800). C. L. appreciates the support by Program of Shanghai Academic Research Leader (No. 21XD1424400).

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Authors and Affiliations

  1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 201899, China

    Meng Lei, Xiaoxue Wu, Yangyang Liu, Keyi Chen, Jiulin Hu & Chilin Li

  2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China

    Yangyang Liu & Chilin Li

  3. CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 201899, China

    Meng Lei, Xiaoxue Wu, Yangyang Liu, Keyi Chen, Jiulin Hu & Chilin Li

  4. Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China

    Xiaoxue Wu

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  1. Meng Lei
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  2. Xiaoxue Wu
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Correspondence to Xiaoxue Wu or Chilin Li.

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12274_2023_5406_MOESM1_ESM.pdf

Polymer electrolytes reinforced by 2D fluorinated filler for all-solid-state Li-Fe-F conversion-type lithium metal batteries

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Lei, M., Wu, X., Liu, Y. et al. Polymer electrolytes reinforced by 2D fluorinated filler for all-solid-state Li-Fe-F conversion-type lithium metal batteries. Nano Res. 16, 8469–8477 (2023). https://doi.org/10.1007/s12274-023-5406-7

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