Stabilizing Li Growth Using Li/LLZO Composites for High‐Performance Li‐Metal‐Based Batteries

Abstract Lithium (Li) metal is widely acknowledged as the most promising anode material, owing to its high capacity and low potential. However, the practical implementation of Li faces challenges, including uncontrollable dendritic growth and a deficient solid electrolyte interphase (SEI). Here a straightforward method is provided for fabricating Li composites using Al‐doped Li 7 La 3 Zr 2 O 12 particles (Li/LLZO) with high Li‐ion conductivity achieved using a mechanical kneading process. The optimized composite, with 20% LLZO content (Li/LLZO‐20), effectively regulates the Li‐ion flux, successfully suppressing Li dendritic growth. Using a systematic investigation, it is demonstrated that incorporating LLZO particles significantly accelerates Li‐ion migration at the electrode–electrolyte interface, facilitating smooth transport through the LLZO particles. Consequently, Li‐metal battery and Li–S battery cells utilizing the Li/LLZO‐20 composite anode exhibit remarkable cycle stability compared to cells employing pure Li anodes.