High‐Performance Dendrite‐Free Lithium Metal Anode Based on Metal‐Organic Framework Glass

Abstract The performance of lithium metal batteries is severely hampered by uncontrollable dendrite growth and volume change within the anode. This work addresses these obstacles by introducing a novel strategy: applying an isotropic and internal grain‐boundary‐free layer, specifically, a metal‐organic framework (MOF) glass layer with nano‐porosity onto the electrochemically plated lithium metal anode. Both ab initio and classical molecular dynamics simulations indicate that the MOF glass layer makes the lithium transport smooth and uniform via its internal monolithic and interfacial advantages. This MOF glass layer with the fast and more uniform lithium diffusion in the monolithic interior and its interface enables dendrite‐free lithium plating and stripping through surface confinement effect and interfacial effect. When employed in symmetric batteries, the achieved Li metal anode can operate over 300 h at 1 mA cm⁻². The full batteries matched with LiFePO₄ exhibit high capacity (148 mAh g⁻¹), excellent rate performance (61 mAh g⁻¹ at 5 C), and outstanding cycling stability (with capacity retention of ≈90% after 1000 cycles). The full batteries matched with high‐voltage LiCoO₂ also show superior performances. Therefore, the strategy of utilizing a MOF glass layer enables the development of high‐performance lithium metal anodes.