Active-Oxygen-Enhanced Homogeneous Nucleation of Lithium Metal on Ultrathin Layered Double Hydroxide.

The development of safe lithium-metal anodes is crucial for the next-generation rechargeable batteries. To stabilize Li metal anodes, pre-planting Li nucleation seeds on lithiophilic substrates is an efficient strategy to regulate initial nucleation process of Li metal. Now, activated ultrathin layered double hydroxide (U-LDHs) are reported as a promising lithiophilic 2D material to realize the uniform deposition of Li metal. The experimental studies and DFT calculations reveal that the active oxygen on U-LDHs provides abundant atomic-scale active sites for Li homogeneous nucleation and plating. Moreover, the lithiophilic properties of active oxygen is also related to its coordination environments. This work opens up an opportunity to more accurate regulation and understanding of Li nucleation from atomic-scale based on 2D ultrathin materials.