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.
Publications
Article type
Year
Research Article
Issue
Nano Research 2024, 17(4): 2663-2670
Published: 02 September 2023
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