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In situ thermally polymerized solid composite electrolytes with a broad electrochemical window for all-solid-state lithium metal batteries

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Abstract

Solid composite electrolytes are prepared by polymerizing a liquid precursor containing Li6.25Ga0.25La3Zr2O12 (Ga-LLZO) nanoparticles. The composite electrolyte shows an ionic conductivity of 1.8 × 10−4 S cm−1 and a Li-ion transference number of 0.58 at 30 °C. Moreover, polymerized composite electrolytes (PCEs) are electrochemically stable up to 6.5 V versus Li/Li+ at room temperature. Li/PCEs/Li symmetric cells maintain stable cycling for more than 1000 h at 0.5 mA cm−2, and the dendrite formation is effectively inhibited, showing compatibility with lithium anodes. Using in situ polymerization, PCEs retain conformal interfacial contacts with all electrodes, and the interfacial resistance of solid-state batteries is decreased by half. Coupled with LiNi0.6Co0.2Mn0.2O2 (NCM622) and LiNi0.85Co0.05Al0.1O2 (NCA) cathodes, solid-state Li metal batteries with PCEs exhibit good cycling performances, including superior specific capacity, high coulombic efficiency and a long cycle lifetime at room temperature. This work offers an approach to meet both the bulk and interfacial requirements of solid-state Li metal batteries and extends the applications of solid composite electrolytes to high-voltage cathodes.

Graphical abstract: In situ thermally polymerized solid composite electrolytes with a broad electrochemical window for all-solid-state lithium metal batteries

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Supplementary files

Article information


Submitted
09 Sep 2019
Accepted
16 Jan 2020
First published
20 Jan 2020

J. Mater. Chem. A, 2020, Advance Article
Article type
Paper

In situ thermally polymerized solid composite electrolytes with a broad electrochemical window for all-solid-state lithium metal batteries

Z. Li, H. Xie, X. Zhang and X. Guo, J. Mater. Chem. A, 2020, Advance Article , DOI: 10.1039/C9TA09969G

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