A Metal-Organic Framework Based Quasi-Solid-State Electrolyte Enabling Continuous Ion Transport for High-Safety and High-Energy-Density Lithium Metal Batteries

Solid-state lithium metal batteries are promising next-generation rechargeable energy storage systems. However, the poor compatibility of the electrode/electrolyte interface and the low lithium ion conductivity of solid-state electrolytes are key issues hindering the practicality of solid-state electrolytes. Herein, rational designed metal-organic frameworks (MOFs) with the incorporation of two types of ionic liquids (ILs) are fabricated as quasi-solid electrolytes. The obtained MOF-IL electrolytes offer continuous ion transport channels with the functional sulfonic acid groups serving as lithium ion hopping sites, which accelerate the Li⁺ transport both in the bulk and at the interfaces. The quasi-solid MOF-IL electrolytes exhibit competitive ionic conductivities of over 3.0 × 10^-4 S cm^-1 at room temperature, wide electrochemical windows over 5.2 V, and good interfacial compatibility, together with greatly enhanced Li⁺ transference numbers compared to the bare IL electrolyte. Consequently, the assembled quasi-solid Li metal batteries show either superior stability at low C rates or improved rate performance, related to the species of ILs. Overall, the quasi-solid MOF-IL electrolytes possess great application potential in high-safety and high-energy-density lithium metal batteries.