Ultra‐uniform Plating of Lithium on 10‐nm‐scale Ordered Carbon Grids for Long Lifespan Lithium Metal Batteries

Abstract Tailorable lithium (Li) nucleation and uniform early‐stage plating is essential for long‐lifespan Li metal batteries. Among factors influencing the early plating of Li anode, the substrate is critical, but a fine control of the substrate structure on a scale of ≈10 nm has been rarely achieved. Herein, a carbon consisting of ordered grids is prepared, as a model to investigate the effect of substrate structure on the Li nucleation. In contrast to the individual spherical Li nuclei formed on the flat graphene, an ultrauniform and nuclei‐free Li plating is obtained on the ordered carbon with a grid size smaller than the thermodynamical critical radius of Li nucleation (≈26 nm). Simultaneously, an inorganic‐rich solid‐electrolyte‐interphase is promoted by the cross‐sectional carbon layers of such ordered grids which are exposed to the electrolyte. Consequently, the carbon grids with a grid size of ≈10 nm show a favorable cycling stability for more than 1100 cycles measured at 2 mA cm −2 in a half cell. With LiNi 0.8 Co 0.1 Mn 0.1 O 2 as cathode, the assembled full cell with a cathode capacity of 3 mAh cm −2 and a negative/positive ratio of 1.67 demonstrates a stable cycling for over 130 cycles with a capacity retention of 88%.