Enabling Stable Lithium Metal Anode via 3D Inorganic Skeleton with Superlithiophilic Interphase

The lithium metal battery (LMB) is among the most sought-after battery chemistries for high-energy storage devices. However, LMBs usually undergo uncontrollable lithium deposition and severe side reactions, which significantly impede their practical applications. Herein, a stable Al₂O₃-based inorganic framework with superlithiophilic lithium aluminum oxide (Li-Al-O) interphase is created via reacting Li with Al₂O₃ nanoparticles. The Al₂O₃-based inorganic framework can serve as a stable Li “host,” reducing the volume expansion during cell cycling. Moreover, the strong interaction between Li-Al-O interphase and Li⁺ can redistribute Li⁺ and reduce the ion concentration gradient near surface protrusion, thus reducing uneven lithium electrodeposition. From galvanostatic measurements, symmetric cells with the 3D Al₂O₃-hybrid electrode can operate under an ultrahigh current density of 8 mA cm⁻² over 480 cycles. When used in full cells, it improves the capacity retention of Li/LiFePO₄ from 78.4% to 93.6% after 200 cycles and enables long-term operation of Li/Li₄Ti₅O₁₂ for over 1200 cycles.