Superlithiophilic, Ultrastable, and Ionic-Conductive Interface Enabled Long Lifespan All-Solid-State Lithium-Metal Batteries under High Mass Loading

Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) suffers from instability against moist air, poor interfacial contact with anode, and serious dendrite issue, which greatly impede its practical application in all-solid-state lithium batteries (ASSLBs). Herein, a superlithiophilic, moisture-resistant, and robust interlayer is demonstrated to overcome these obstacles by in situ forming an AlF3 interlayer on the LLZTO surface. Thanks to the unique property, the AlF3-modified LLZTO offers a significantly reduced interfacial resistance by more than two orders of magnitude (from 527.5 & omega; cm(2) for the pristine Li/LLZTO to 1.3 & omega; cm(2) for the surface-engineered interface), achieves a critical current density of 1.2 mA cm(-2) and long-term stability of over 4000-4700 h, and endows regulated Li plating/stripping behaviors. Specifically, ASSLBs coupled with LiFePO4 and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes can stably charge/discharge over 400 and 100 cycles at 0.5 and 0.2 C at 25 & DEG;C, with retentions of >80.0% and Coulombic efficiencies of >99.9%, respectively. Particularly, the NCM811-based full ASSLB with large mass loading of 8.3 mg cm(-2) also delivers a discharge-specific capacity as high as 199.1 mAh g(-1) with good rate capability, even approaching to the liquid cells. This study demonstrates a practical solution to address the interfacial challenges and paves the way for practical progress of ASSLBs.