Three-Dimensional Interpenetrated Metal-Organic Frameworks for Stabilizing Lithium Metal Interfaces: Structural...

Rechargeable lithium metal batteries (LMBs) are hindered by uncontrolled dendrite growth and interfacial instability driven by erratic ion migration and unstable electrochemical dynamics at the anode interface. In this study, a multifunctional three-dimensional interpenetrating Co-DPBB metal-organic framework (MOF) coating as an artificial solid electrolyte interphase was introduced to homogenize ion migration and expedite transport behaviors across the electrode-electrolyte interface. Through synergistic density functional theory (DFT) calculations and comprehensive in situ/ex situ characterizations, the relationship of orchestrated lithium-ion desolvation kinetics, charge transfer efficiency, and deposition topography with Co-DPBB's nanoarchitectural channels and lithiophilic anchoring moieties were decoupled. Co-DPBB-modified electrodes exhibit exceptional electrochemical performance, with reduced polarization, extended cycle life (>8000 h), and stable lithium deposition. This work introduces a transformative interfacial engineering approach, laying the groundwork for high-energy-density LMBs.