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An in-situ generated composite solid-state electrolyte towards high-voltage lithium metal batteries

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Abstract

The solid-state electrolyte (SSE) has promising applications in next-generation lithium (Li) metal batteries (LMBs) because of its significantly enhanced safety and more compatible interface characteristics than flammable traditional liquid electrolytes. However, only a few attempts have achieved high-performance high-voltage LMBs, which is attributed to the fact that both high ionic conductivity and good compatibility with electrodes can hardly be achieved simultaneously. Herein, a composite solid-state electrolyte (CSE) based on star-shaped siloxane-based polymer electrolyte coupled with Li6.75La3Zr1.75Ta0.25O12 (LLZTO) ceramic fillers is designed and prepared through a facile in-situ polymerization method. The obtained CSE exhibits high ionic conductivity (i.e., 1.68 × 10−4 S cm−1 at a temperature of 60 °C), superior anodic stability, and high Li-ion transference number (i.e., 0.53) because of the multifunctional synergistic effect of the polymer electrolyte with LLZTO ceramic fillers. Moreover, the as-developed CSE shows excellent compatibility with Li anodes. As a result, the as-developed CSE enables the development of long-life 4.4-V-class solid-state LMBs with a LiCoO2 cathode, with 79.7% capacity retention and 99.74% average Coulombic efficiency after 500 cycles at a 0.5 C rate. Postmortem analysis of cycled batteries confirms that such superior battery performance can be mainly ascribed to the formation of a compatible electrode/electrolyte interface. Furthermore, excellent safety features can be observed in LiCoO2/Li pouch batteries. This work provides an important guide for the rational design of SSEs for high-voltage LMBs.

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Acknowledgements

This work was supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21070304), the National Natural Science Foundation of China (51502319, 51803230, 52003285, 21901248), the Natural Science Foundation of Shandong Province (ZR2021QE039, ZR2021QE149, ZR2020MB082), the Key Scientific and Technological Innovation Project of Shandong (2020CXGC010401), and the Taishan Scholars of Shandong Province (ts201511063).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266100, China

    Qinglei Wang, Tiantian Dong, Qian Zhou, Zili Cui, Chenglong Lu, Zhaolin Lv, Kai Chen, Lang Huang, Huanrui Zhang & Guanglei Cui

  2. School of Materials Science and Engineering, Ocean University of China, Qingdao, 266042, China

    Tiantian Dong

  3. School of Materials Science and Engineering, Linyi University, Linyi, 276000, China

    Qinglei Wang & Xuehui Shangguan

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  1. Qinglei Wang
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  2. Tiantian Dong
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Correspondence to Huanrui Zhang or Guanglei Cui.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Wang, Q., Dong, T., Zhou, Q. et al. An in-situ generated composite solid-state electrolyte towards high-voltage lithium metal batteries. Sci. China Chem. 65, 934–942 (2022). https://doi.org/10.1007/s11426-022-1221-4

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  • DOI: https://doi.org/10.1007/s11426-022-1221-4

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