In Situ Polymerized Hybrid Nanofiber Membranes Boost High-Voltage Stability of Solid-State Lithium Metal Batteries

Solid-state lithium metal batteries, particularly those with solid polymer electrolytes, are regarded as promising solutions to achieve both higher energy density and safety. However, their development has been hampered by limited high-voltage tolerance. To overcome this challenge, we propose integrating a multifunctional hybrid nanofiber membrane with <i>in situ</i> polymerization of vinylene carbonate to create a solid electrolyte with exceptional high-voltage stability and efficient room-temperature performance. The improved compatibility and ionic conductivity arise from dipole-dipole interactions between polar groups and vinylene carbonate. Our approach delivers LiFePO₄//Li cells with marvelous cycling stability, surpassing 1000 cycles at 1C, and especially shows excellent compatibility with high-voltage Li₃V₂(PO₄)₃ (4.8 V vs Li/Li⁺) and LiNi_0.8Co_0.1Mn_0.1O₂ (4.7 V vs Li/Li⁺). This straightforward yet effective strategy contributes to energy storage with safer and higher-energy-density solid-state lithium metal batteries.