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Constructing an anion-capturing interface to achieve Li+ cross-phase transport in composite solid electrolytes
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DOI：10.1038/s41467-025-67065-0.png)
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Abstract
En 中文
The ionic conductivity of solid electrolytes is still insufficient to approach performance promises of solid-state Li metal batteries, suffering from their charged interfaces among phase components and movable Li+ concentration. Herein, an anion-capturing interface based on FeF3 is established on Li6.5La3Zr1.5Ta0.5O12 surface through a sol-gel method. It promotes Li-salt dissociation and formation of anion aggregated layer before blending with polymer. Coulombic interaction of anion on grains boundary showcases multiple merits, including their weakened built-in electric field, restrained charge gradient layer, spontaneous Li+ cross-phase migration, and homogenized interfacial charge distribution. As such, the resulting composite solid electrolytes exhibits an ion conductivity of 1.1×10−4 S/cm2 and Li+ migration number of 0.75 at 25°C. Its resulting Li symmetrical batteries maintain Li plating/stripping behaviors for over 1300 h and low polarization at 0.1 mA/cm2 current density. When being assembled with LiFePO4 positive electrode in solid-state batteries, it performs a specific capacity of 152.8 mAh/g at 1.0 C (170 mA/g) with 96% retention after 600 cycles. This work prioritizes the promises of interface engineering for solid electrolytes in solid-state Li metal batteries. Composite solid electrolytes face sluggish inter-phase Li+ migration. Here, authors construct a FeF3-based anion-capturing layer onto Li6.5La3Zr1.5Ta0.5O12 nanofillers within PVdF solid electrolyte, where the charge gradient layer on the interface promotes Li+ cross-phase conductivity.
Keywords:
anion-capturing interface
Li+ cross-phase transport
composite solid electrolytes
ionic conductivity
solid-state Li metal batteries
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