Solid electrolytes are revolutionizing the field of lithium–metal batteries; however, their practical implementation has been impeded by the interfacial instability between lithium metal electrodes and solid electrolytes. While various interlayers have been suggested to address this issue in recent years, long-term stability with repeated lithium deposition/stripping has been challenging to attain. Herein, we successfully operate a high-power lithium–metal battery by inducing the preferred directional lithium growth with a rationally designed interlayer, which employs (i) crystalline-direction-controlled carbon material providing isotropic lithium transports, with (ii) prelithium deposits that guide the lithium nucleation direction toward the current collector. This combination ensures that the morphology of the interlayer is mechanically robust while regulating the preferred lithium growth underneath the interlayer without disrupting the initial interlayer/electrolyte interface, enhancing the durability of the interface. We illustrate how these material/geometric optimizations are conducted from the thermodynamic considerations, and its applicability is demonstrated for the garnet-type Li_7–xLa_3–aZr_2–bO₁₂ (LLZO) solid electrolytes paired with the capacity cathode. It is shown that a lithium–metal cell with the optimized amorphous carbon interlayer with prelithium deposits exhibits outstanding room-temperature cycling performance (99. 6% capacity retention after 250 cycles), delivering 4.0 mAh cm^–2 at 2.5 mA cm^–2 without significant degradation of the capacity. The successful long-term operation of the hybrid solid-state cell at room temperature (approximately a cumulative deliverable capacity of over 1000 mAh cm^–2) is unprecedented and records the highest performance reported for lithium–metal batteries with LLZO electrolytes until date.

中文翻译：

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优先定向锂生长机制实现高功率混合固态锂金属电池

固体电解质正在彻底改变锂金属电池领域；然而，锂金属电极和固体电解质之间的界面不稳定性阻碍了它们的实际应用。近年来，虽然提出了各种中间层来解决这个问题，但要实现反复锂沉积/剥离的长期稳定性一直具有挑战性。在此，我们通过合理设计的夹层诱导首选的定向锂生长，成功运行了高功率锂金属电池，该夹层采用 (i) 结晶方向可控的碳材料提供各向同性锂传输，(ii) 预锂沉积引导锂成核方向朝向集电器。这种组合确保夹层的形态在机械上是稳健的，同时调节夹层下方优选的锂生长而不破坏初始夹层/电解质界面，从而增强界面的耐久性。我们说明了这些材料/几何优化是如何从热力学考虑进行的，并证明了它对石榴石型 Li 的适用性_{7– x} La _{3– a} Zr _{2– b} O ₁₂ (LLZO) 固体电解质与容量阴极配对。结果表明，具有优化的无定形碳中间层和预锂沉积物的锂金属电池表现出出色的室温循环性能（250 次循环后容量保持率为 99. 6%），在 2.5 mA cm ^{–2时提供 4.0 mAh cm –2}而无需能力的显着下降。混合固态电池在室温下成功长期运行（累计可提供容量约超过 1000 mAh cm ^–2) 是前所未有的，记录了迄今为止使用 LLZO 电解质的锂金属电池报告的最高性能。