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Research Article

Porous garnet as filler of solid polymer electrolytes to enhance the performance of solid-state lithium batteries

Yang Zhang1, Lei Zhang1, Peng Guo1, Chaoyan Zhang1, Xiaochuan Ren2(), Zhen Jiang3(), Jianjun Song1, Chuan Shi1()
College of Physics, Qingdao University, Qingdao 266071, China
Industrial Research Institute of Nonwovens and Technical Textiles, College of Textiles and Clothing, Qingdao University, Qingdao 266071, China
Department of Chemistry, University of Pennsylvania, Philadelphia, PA 19104, USA
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The unique porous structure of Li6.4La3Zr2Al0.2O12 (LLZO) facilitates the interaction between polymer and filler and provides sufficient entrance for Li+ migration into the LLZO phase. Meanwhile, it offers continuous ionic migration channels with the interlinked LLZO grains, which only permit cation migration, thus increasing the lithium-ion conductive and transference number of solid polymer electrolytes (SPEs).

Abstract

In order to enhance the ionic conductivity of solid polymer electrolytes (SPEs) and their structural rigidity against lithium dendrite during lithium-ion battery (LIB) cycling, we propose porous garnet Li6.4La3Zr2Al0.2O12 (LLZO), as the filler to SPEs. The porous LLZO with interlinked grains was synthesized via a resol-assisted cationic coordinative co-assembly approach. The porous structure of LLZO with high specific surface area facilitates the interaction between polymer and filler and provides sufficient entrance for Li+ migration into the LLZO phase. Furthermore, the interconnection of LLZO grains forms continuous inorganic pathways for fast Li+ migration, which avoid the multiple diffusion for Li+ in interface. As a result, the SPEs with porous LLZO (SPE-PL) show a high ionic conductive of 0.73 mS·cm−1 at 30 °C and lithium-ion transference number of 0.40. The porous LLZO with uniformly dispersed pores also acts as an ion distributor to regulate ionic flux. The lithium-symmetrical batteries assembled with SPE-PL show a highly stable Li plating/stripping cycling for nearly 3000 h at 0.1 mA·cm−2. The corresponding Li/LiFePO4 batteries also exhibit excellent cyclic performance with capacity retention of 75% after nearly 500 cycles. This work brings new insights into the design of conductive fillers and the optimization of SPEs.

Keywords

solid polymer electrolyteslithium metal batteryporous conductive fillersolid state battery

Electronic Supplementary Material

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Nano Research
Volume 17 Issue 4,
April 2024
Pages 2663-2670
DOI: 10.1007/s12274-023-6065-4
Cite this article:
Zhang Y, Zhang L, Guo P, et al. Porous garnet as filler of solid polymer electrolytes to enhance the performance of solid-state lithium batteries. Nano Research, 2024, 17(4): 2663-2670. https://doi.org/10.1007/s12274-023-6065-4
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