Cation‐Loaded Porous Mg2+‐Zeolite Layer Direct Dendrite‐Free Deposition toward Long‐Life Lithium Metal Anodes

Abstract Lithium metal, with ultrahigh theoretical specific capacity, is considered as an ideal anode material for the lithium‐ion batteries. However, its practical application is severely plagued by the uncontrolled formation of dendritic Li. Here, a cation‐loaded porous Mg2+‐Zeolite layer is proposed to enable the dendrite‐free deposition on the surface of Li metal anode. The skeleton channels of zeolite provide the low coordinated Li+‐solvation groups, leading to the faster desolvation process at the interface. Meanwhile, anions‐involved solvation sheath induces a stable, inorganic‐rich SEI, contributing to the uniform Li+ flux through the interface. Furthermore, the co‐deposition of sustained release Mg2+ realizes a new faster migration pathway, which proactively facilitates the uniform diffusion of Li on the lithium substrate. The synergistic modulation of these kinetic processes facilitates the homogeneous Li plating/stripping behavior. Based on this synergistic mechanism, the high‐efficiency deposition with cyclic longevity exceeding 2100 h is observed in the symmetric Li/Li cell with Mg2+‐Zeolite modified anode at 1 mA cm−2. The pouch cell matched with LiFePO4 cathode fulfills a capacity retention of 88.4% after 100 cycles at a severe current density of 1 C charge/discharge. This synergistic protective mechanism can give new guidance for realizing the safe and high‐performance Li metal batteries.