Constructing an anion-capturing interface to achieve Li(+) cross-phase transport in composite solid electrolytes #MMPMID41381567
Lan J; Zhong Y; Peng H; Meng ZD; He NX; Lan SZ; Huang L; Sun SG; Deng YP
Nat Commun 2025[Dec]; ? (?): ? PMID41381567show ga
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 FeF(3) is established on Li(6.5)La(3)Zr(1.5)Ta(0.5)O(12) 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 1.1x10(-4) S/cm(2) and Li(+) migration number of 0.75 at 25 degrees C. Its resulting Li symmetrical batteries maintain Li plating/stripping behaviors for over 1300 h and low polarization at 0.1 mA/cm(2) current density. When being assembled with LiFePO(4) 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.