A Simple Composite Protective Layer Coating That Enhances the Cycling Stability of Lithium Metal Batteries

Metallic lithium is the most promising negative electrode for high-energy rechargeable batteries due to its extremely high specific capacity and its extremely low redox potential. However, the low cycle efficiency and lithium dendrite formation during the charge/discharge processes consistently hinder its practical application. In this report, we present a stabilized Li electrode on which a Li⁺ ion conductive inorganic/organic composite protective layer (CPL) is coated. With the introduction of the CPL, the Li dendrite growth and electrolyte decomposition are effectively suppressed; consequently, stable Li plating/stripping at high current densities up to 10 mA cm^-2 is possible. Nanoindentation tests demonstrate that the shear modulus of the CPL at narrow indentations is 1.8 times higher than that of the Li metal, which provides a theoretical understanding for its efficacy. Moreover, the LiCoO₂/Li cell incorporating CPL exhibits excellent cycling stability up to 400 cycles at 1 mA cm^-2 (1 C-rate), which demonstrates practical applicability in Li ion batteries through replacing the graphite anode with a CPL-coated Li metal anode.