The Influence of Surface Chemistry on Critical Current Density for Garnet Electrolyte

Abstract Garnet‐based solid state lithium batteries have attracted a lot of attention due to their potential advantages in safety and energy density. However, the high electrode–electrolyte interfacial resistance and low critical current density (CCD) related with lithium dendrite penetration have seriously hindered their further development and practical application. Here, for garnet‐type solid electrolyte, the surface Li 2 CO 3 , interlayer species, lithium wettability, interfacial impedance, and CCD are systematically investigated. It turns out that Li 2 CO 3 ‐free garnet electrolyte is intrinsically lithiophilic, and the interfacial impedance is mainly affected by the amount of surface Li 2 CO 3 . In addition, the CCD values are manipulated by the interfacial impedance rather than the apparent Li wettability. This study provides a comprehensive understanding about the interrelationships among surface chemistry, lithium wettability, interfacial impedance, and critical current density for garnet‐type solid electrolytes.