A quasi-solid polymer electrolyte initiated by two-dimensional functional nanosheets for stable lithium metal batteries

Abstract

Lithium-metal batteries (LMBs) are expected to serve as next-generation energy storage systems due to their high theoretical energy density. However, their practical application is largely impeded due to the safety risks that arise from the uncontrollable Li dendrite growth and the high reactivity between high flammability liquid organic electrolytes and metallic lithium. Here, we report a highly safe quasi-solid gel polymer electrolyte (GPE) to achieve stable cycling of lithium metal with high coulombic efficiency, and it is prepared by in situ polymerization of 1,3-dioxolane (DOL) assisted by multi-functional H₃Sb₃P₂O₁₄ sheets. H₃Sb₃P₂O₁₄ acts as an initiator and a functional additive simultaneously that promotes the formation of a stable solid electrolyte interface (SEI) layer, thereby regulating the uniform deposition of Li and improving the Li plating/stripping efficiency. The obtained quasi-solid GPE exhibits high ionic conductivity and enhanced oxidative stability, favoring a stabilized electrode/electrolyte interface. Using the GPE, the electrochemical performance of the quasi-solid-state LMB with a LiFePO₄ cathode and a lithium metal anode is significantly improved, delivering a discharge capacity of 125.7 mA h g⁻¹ even after 1000 cycles. Therefore, the high reversibility and remarkable battery cyclability suggest that such a GPE is a promising choice of electrolyte for LMBs, while its facile preparation makes its large-scale application possible in the future.