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.

中文翻译：

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负载阳离子的多孔 Mg2+-沸石层直接无枝晶沉积长寿命锂金属阳极

锂金属具有超高的理论比容量，被认为是锂离子电池的理想负极材料。然而，其实际应用受到枝晶锂不受控制形成的严重困扰。这里，负载阳离子的多孔镁2+‐沸石层旨在实现锂金属阳极表面的无枝晶沉积。沸石的骨架通道提供了低配位的Li+‐溶剂化基团，导致界面处更快的去溶剂化过程。同时，涉及阴离子的溶剂化鞘层会诱导形成稳定的、富含无机物的SEI，从而有助于均匀的Li+通过界面的通量。此外，缓释镁的共沉积2+实现了一种新的更快迁移途径，主动促进锂在锂基板上的均匀扩散。这些动力学过程的协同调节促进了均匀的锂沉积/剥离行为。基于这种协同机制，在含镁的对称Li/Li电池中观察到了循环寿命超过2100小时的高效沉积2+‐1 mA cm 时的沸石改性阳极−2。与LiFePO配套的软包电池4在1 C充电/放电的严格电流密度下，正极在100次循环后容量保持率为88.4%。这种协同保护机制可以为实现安全、高性能的锂金属电池提供新的指导。