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

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Garnet‐Polymer Composite Electrolytes with High Li+ Conductivity and Transference Number via Well‐Fused Grain Boundaries in Microporous Frameworks
ChemElectroChem ( IF 3.5 ) Pub Date : 2020-03-04 , DOI: 10.1002/celc.202000202
Xiang Peng ₁ , Kai Huang ₁ , Shipai Song ₁ , Fang Wu ₁ , Yong Xiang ₁ , Xiaokun Zhang ₁

Affiliation

A garnet‐polymer composite electrolyte with high Li⁺ conductivity and transference number is developed using microporous Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (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.

中文翻译：

石榴石-聚合物复合电解质通过微孔骨架中充分融合的晶界具有高Li +电导率和转移数

以微孔Li _6.4 La ₃ Zr _1.4 Ta _0.6 O ₁₂（LLZTO）为骨架，开发了具有高Li ⁺电导率和转移数的石榴石-聚合物复合电解质。LLZTO框架由模板辅助的凝胶浇铸工艺制造，具有微米级的晶粒和良好融合的晶界，消除了陶瓷块之间界面处的低导电瓶颈，并为Li ⁺提供了导电和连续的网络运输。结果，石榴石-聚合物复合电解质显示出高的离子电导率（在25°C下为2.61×10 ^-4 S cm ^-1），超高的Li⁺转移数为0.71，以及出色的热，结构和电化学稳定性。得益于所需的物理和化学性能，本发明的复合电解质使Li-Li电池在25°C下循环600小时以上。此外，集成的LiFePO ₄ / CPCE / Li电池还显示出出色的循环稳定性，在50°C下100次循环后的比容量为133.2 mAh g ^-1。这项研究证明了可用于全固态锂电池的复合电解质微观结构的重大优化。

更新日期：2020-03-04

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