Interface engineering is an effective approach to solving the difficult Li-dendrite issues in lithium–metal batteries, and yet a robust large-capacity Li anode (≥20 mA h cm⁻²) working at an ultrahigh rate density (≥20 mA cm⁻²) is still rarely achieved. Herein, an integrated Li–metal-based anode with a top-down composition gradient (Li₂O–LiOH–Li₃Sb/Li) is constructed through a thermal-induced reaction of molten Li with polyantimonic acid (PAA). Unexpectedly, the lattice-water-containing PAA is found in favor of a mild but homogeneous lithiation reaction, whilst accompanied by a spontaneous phase separation between the resulting Li₂O, LiOH, and Li₃Sb components due to their significant interfacial energy discrepancy. The consequent Li₂O-enriched top layer affording a high Young's modulus (>10 GPa) and electron-shielding ability can effectually suppress the Li-dendrite growth, while the underlying LiOH–Li₃Sb interphase as ionic-channels homogenize Li⁺-flux distribution, in turn enabling dendrite-free Li deposition in a lithiophilic Li₃Sb/Li bottom layer. With this free-standing integrated electrode, large-areal-capacity symmetrical cells (25 mA h cm⁻²) can maintain over 1280 h Li plating/stripping cycles at an ultrahigh-current-density of 50 mA cm⁻², and the full-cells paired with high-capacity LiCoO₂ (3.5 mA h cm⁻²) exhibit improved cycling stability under a practical low N/P ratio (1.33). Importantly, this robust integrated anode also showcases decent compatibility with gel-polymer/Li₇La₃Zr₂O₁₂ solid-state electrolytes, signifying the application potential in safe Li–metal batteries.

中文翻译：

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一种由聚锑酸实现自上而下成分梯度的大容量、超高倍率集成锂金属负极

界面工程是解决锂金属电池中锂枝晶问题的有效方法，并且是在超高倍率密度（≥20 mA cm ^{-2 ）下工作的坚固的大容量锂负极（≥20 mA h cm -2 ） 2} ) 仍然很少实现。在此，通过熔融锂与聚锑酸（PAA）的热诱导反应构建了具有自上而下成分梯度（Li ₂ O-LiOH-Li ₃ Sb/Li）的集成锂金属基阳极。出乎意料的是，含有晶格水的PAA有利于温和但均匀的锂化反应，同时由于其显着的界面能差异，所产生的Li ₂ O、LiOH和Li ₃ Sb组分之间会发生自发相分离。由此产生的富含 Li ₂ O 的顶层具有高杨氏模量 (>10 GPa) 和电子屏蔽能力，可以有效抑制锂枝晶的生长，而下面的 LiOH-Li ₃ Sb 界面作为离子通道使 Li ⁺ -均质化。通量分布，进而能够在亲锂的 Li ₃ Sb/Li 底层中实现无枝晶的 Li 沉积。借助这种独立式集成电极，大面积容量对称电池（25 mA h cm ^{-2 ）可以在50 mA cm -2}的超高电流密度下维持超过1280小时的锂沉积/剥离循环，并且-与高容量LiCoO ₂ (3.5 mA h cm ^-2 )配对的电池在实际低N/P比(1.33)下表现出改善的循环稳定性。重要的是，这种坚固的集成阳极还表现出与凝胶聚合物/Li ₇ La ₃ Zr ₂ O ₁₂固态电解质良好的兼容性，这表明其在安全锂金属电池中的应用潜力。