High-Voltage and Wide-Temperature Lithium Metal Batteries Enabled by Ultrathin MOF-Derived Solid Polymer Electrolytes...

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 μm with a satisfactory ionic conductivity and lithium-ion transference number (1.1 mS cm^-1 at 30 °C, 0.72). The optimized SLMBs with high-voltage LiMn_0.75Fe_0.25PO₄ (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 °C, and their capacity remains 143.3 mA h g^-1 after being cycled 300 times at 10 C at 100 °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 °C. From the above analysis, these MMSEs present new opportunities for the development of SLMBs with good electrochemical properties.