Novel Organophosphate‐Derived Dual‐Layered Interface Enabling Air‐Stable and Dendrite‐Free Lithium Metal Anode

Lithium (Li) metal, as a promising candidate for next-generation energy storage systems, suffers from an extremely unstable interface that is prone to crack, causing serious corrosion of Li metal and dendrite growth. To address this, a novel dual-layered interface on the Li metal anode is reported, which is featured with organics (COPO3 , (CO)2 PO2 , and (CO)3 PO) on the top and inorganics (Li3 PO4 ) at the bottom. The flexible organic layer with reduced Young's modulus (≈550 MPa) contributes to maintain structural integrity, while the rigid inorganic layer with improved Young's modulus of ≈12 GPa is beneficial to suppress the Li dendrite growth. Accordingly, the protected Li is stabilized to maintain successive electrodeposition over 800 cycles of plating/stripping process at a current density of 2 mA cm-2 . Furthermore, the uniform dual-layered interface tends to prevent the corrosion of air to Li metal, exhibiting almost the same performance as the Li metal treated in the inert atmosphere.