Lithium metal is the only anode material that can enable the Li−O₂ battery to realize its high theoretical energy density (≈3500 Wh kg⁻¹). However, the inherent uncontrolled dendrite growth and serious corrosion limitations of lithium metal anodes make it experience fast degradation and impede the practical application of Li−O₂ batteries. Herein, a multifunctional complementary LiF/F‐doped carbon gradient protection layer on a lithium metal anode by one‐step in situ reaction of molten Li with poly(tetrafluoroethylene) (PTFE) is developed. The abundant strong polar C‐F bonds in the upper carbon can not only act as Li⁺ capture site to pre‐uniform Li⁺ flux but also regulate the electron configuration of LiF to make Li⁺ quasi‐spontaneously diffuse from carbon to LiF surface, avoiding the strong Li⁺‐adhesion‐induced Li aggregation. For LiF, it can behave as fast Li⁺ conductor and homogenize the nucleation sites on lithium, as well as ensure firm connection with lithium. As a result, this well‐designed protection layer endows the Li metal anode with dendrite‐free plating/stripping and anticorrosion behavior both in ether‐based and carbonate ester‐based electrolytes. Even applied protected Li anodes in Li−O₂ batteries, its superiority can still be maintained, making the cell achieve stable cycling performance (180 cycles).

中文翻译：

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针对长寿命Li-O2电池的原位设计梯度Li +捕获和准自发扩散阳极保护层。

锂金属是可使Li-O ₂电池实现其较高的理论能量密度（约3500 Wh kg ^-1）的唯一阳极材料。但是，锂金属阳极固有的不受控制的枝晶生长和严重的腐蚀限制使其经历快速降解，并阻碍了Li-O ₂电池的实际应用。本文通过熔融锂与聚四氟乙烯（PTFE）的一步原位反应，开发了锂金属阳极上的多功能互补LiF / F掺杂碳梯度保护层。上部碳原子中丰富的强极性C-F键不仅可以充当Li ^+的捕获位点，使Li ⁺预先均匀通量，但也调节LiF的电子构型，使Li ⁺准自发地从碳扩散到LiF表面，避免了强烈的Li ⁺粘附诱导的Li聚集。对于LiF，它可以充当快速的Li ⁺导体，并使锂上的成核位置均匀化，并确保与锂的牢固连接。因此，这种精心设计的保护层使锂金属阳极在醚基和碳酸酯基电解质中均具有无枝晶的镀层/剥落和抗腐蚀性能。即使在Li-O ₂电池中使用受保护的Li阳极，也仍然可以保持其优越性，从而使电池达到稳定的循环性能（180次循环）。