High-Voltage And Wide-Temperature Lithium Metal Batteries Enabled By Ultrathin Mof-Derived Solid Polymer Electrolytes With Modulated Ion Transport

Solid polymer electrolytes (SPEs) of superior ionic conductivity, long-term cycling stability, and good interface compatibility are regarded as promising candidates to enable the practical applications of solid lithium metal batteries (SLMBs). Here, a mixed-matrix SPE (MMSE) with incorporated metal-organic frameworks (MOFs) and ionic liquid is prepared. The dissociation of Li salt in MMSE can be promoted effectively due to the introduction of MOF via the Fourier-transform infrared spectroscopy (FT-IR) analysis, density functional theory calculation, and molecular dynamics simulation. The as-formed MMSE exhibits an ultralow thickness of 20 mu m with a satisfactory ionic conductivity and lithium-ion transference number (1.1 mS cm(-1) at 30 degrees C, 0.72). The optimized SLMBs with high-voltage LiMn0.75Fe0.25PO4 (LMFP) exhibit an excellent cyclability at 4.2 V under room temperature. Moreover, Li/MMSE/LiFePO4 cells have desirable cycle performance from -20 to 100 degrees C, and their capacity remains 143.3 mA h g(-1) after being cycled 300 times at 10 C at 100 degrees C. The Li/LiFePO4 pouch cells also show excellent safety under extreme conditions. The Li symmetric cells can work steadily even at a supreme current density of 4 mA cm(-2) at 100 degrees C. From the above analysis, these MMSEs present new opportunities for the development of SLMBs with good electrochemical properties.