Garnet-Polymer Composite Electrolytes with High Li+ Conductivity and Transference Number via Well-Fused Grain Boundaries in Microporous Frameworks

Xiang PENG, Kai HUANG, Shipai SONG, Fang WU, Yong XIANG, Xiaokun ZHANG*

*Corresponding author for this work

Research output: Journal PublicationsJournal Article (refereed)peer-review

21 Citations (Scopus)

Abstract

A garnet-polymer composite electrolyte with high Li+ conductivity and transference number is developed using microporous Li6.4La3Zr1.4Ta0.6O12 (LLZTO) framework as the matrix. The LLZTO framework, fabricated by a template-assisted gel-casting process, possesses micron-sized grains and well-fused grain boundaries, eliminating the low-conductive bottleneck at the interfaces between the ceramic blocks, and providing conductive and continuous networks for Li+ transport. As a result, the garnet-polymer composite electrolyte displays a high ionic conductivity (2.61×10−4 S cm−1 at 25 °C), an ultrahigh Li+ transference number of 0.71, as well as excellent thermal, structural, and electrochemical stabilities. Benefiting from the desired physical and chemical properties, the presented composite electrolyte enables a Li−Li cell to be cycled for more than 600 h at 25 °C. In addition, the integrated LiFePO4/CPCE/Li cells also show excellent cycling stability with a specific capacity of 133.2 mAh g−1 after 100 cycles under 50 °C. This study demonstrates a significant optimization on the microstructure of composite electrolytes that can be utilized for all-solid-state lithium batteries.

Original languageEnglish
Pages (from-to)2389-2394
Number of pages6
JournalChemElectroChem
Volume7
Issue number11
Early online date4 Mar 2020
DOIs
Publication statusPublished - 2 Jun 2020
Externally publishedYes

Bibliographical note

X.Z. acknowledges the support from National Science Funds of China (Grant No. 21905040) and the startup funds from the University of Electronic Science and Technology of China. X.P. acknowledges the support from Postdoctoral Research Foundation of China (contract No. 2018 M643444). X.P. would like to thank Prof. Wang Shi Wei (Shanghai Institute of Ceramics, Chinese Academy of Sciences) for introducing the copolymer of isobutylene and maleic anhydride.

Keywords

  • ceramic framework
  • composite electrolyte
  • ionic conductivity
  • transference number
  • well-fused grain boundary

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