Low-Temperature In Situ Lithiation Construction of a Lithiophilic Particle-Selective Interlayer for Solid-State...

Unexpected interface resistance and lithium dendrite puncture hinder the application of garnet-type solid-state electrolytes in high-energy-density systems. Different from the previous high-temperature (>180 °C) molten lithium that promotes the alloying reaction between the coating layer and Li to enhance the interface contact, herein, we introduce liquid-metal-like SbCl₃ to construct a three-dimensional Li⁺ directional-selection interlayer by in situ low-temperature lithiation (80 °C). An interlayer with a more negative interface energy composed of SbLi₃ and LiCl exhibits a superior affinity with Li and LGLZO, which reduces the interface resistance and suppresses the growth of Li dendrites by an insulated electron. The introduction of the SbCl₃ modification layer into Li/Li symmetric cells enables charge/discharge at a current density of 6.0 mA cm^-2 and operation for more than 1000 h under 2.0 mA cm^-2 at room temperature. The full cells with the LiFePO₄ cathode exhibit a high residual capacity of 144.8 mAh g^-1 at 0.5 C after 1000 cycles and excellent cycling stability with a retention ratio of 94.7% at 1 C after 600 cycles. The low-temperature lithiation method based on an energy-saving perspective should be applied to other types of solid-state electrolyte modification strategies.