Stable Lithium Metal Anode Enabled by a Lithiophilic and Electron/Ion Conductive Framework

Abstract Li metal anode has been considered as the ideal anode for next-generation batteries due to its ultrahigh capacity and lowest electrochemical potential. However, its practical application is still impeded by low Coulombic efficiency, huge volume change, and safety hazards arising from Li dendrite growth. In this work, a three-dimensional (3D) structured highly stable Li metal anode is designed and easily preapred. Benefiting from the in situ reaction between Li metal and AlN, highly Li+ conductive Li3N and lithiophilic LiAl alloy have been simultaneously formed and homogeneously distributed in the framework, in which Li metal is finely dispersed and embedded. The outstanding electron/ion mixed conductivity of Li3N/LiAl and 3D composite structure with enhanced interfacial area significantly improve the electrode kinetics and suppress the volume change on cycling, while a lithiophilic effect of LiAl alloy and uniform distribution of Li ion flux inside the electrode avoid dendritic Li deposition. As a result, the proposed Li metal electrode exhibits exceptional electrochemical reversibility in both carbonate and ether-based electrolytes. Paired with LiFePO4 and sulfurized polyacrylonitrile (S@pPAN) cathodes, the full cells deliver highly stable and long-term cycling performance. Therefore, the proposed strategy to fabricate Li metal anodes could promote the practical application of Li metal batteries.