Review on Li Deposition in Working Batteries: From Nucleation to Early Growth.

Lithium (Li) metal is one of the most promising alternative anode materials of next-generation high-energy-density batteries demanded for advanced energy storage in the coming fourth industrial revolution. Nevertheless, disordered Li deposition easily causes short lifespan and safety concerns and thus severely hinders the practical applications of Li metal batteries. Tremendous efforts are devoted to understanding the mechanism for Li deposition, while the final deposition morphology tightly relies on the Li nucleation and early growth. Here, the recent progress in insightful and influential models proposed to understand the process of Li deposition from nucleation to early growth, including the heterogeneous model, surface diffusion model, crystallography model, space charge model, and Li-SEI model, are highlighted. Inspired by the abovementioned understanding on Li nucleation and early growth, diverse anode-design strategies, which contribute to better batteries with superior electrochemical performance and dendrite-free deposition behavior, are also summarized. This work broadens the horizon for practical Li metal batteries and also sheds light on more understanding of other important metal-based batteries involving the metal deposition process.