Homogenous lithium plating/stripping regulation by a mass-producible Zn particles modified Li-metal composite anode

A stable lithium-metal anode is critical for high performance lithium-metal batteries. However, heterogeneous Li plating/stripping may induce lithium dendrites formation on bare lithium-metal anode, which lowers the cell Coulombic efficiency and weakens battery safety. We found that bare Li metal surface becomes bumpy and cratered with numerous pits formation during Li stripping. These pits enhance electric field distortion and heterogeneous ion distribution during plating. Li plating preferentially happens on the edge of the pits, intensifying the voltage variation and Li dendrites growth, which leads to the cell rapid death or separator piercing. Herein, we propose a facile and mass-producible method to homogenize Li plating/stripping via adding lithiophilic particles into Li metal. Zinc particles were uniformly pressed in Li metal by a facile and scalable physical strategy of “rolling”, and transformed into LiZn alloy in situ through Li-Zn alloying at room temperature in a few minutes. The critical role of modified LiZn/Li composite anode in stabilizing electrode surface was revealed by both electrochemical test and simulation. Compared with bare Li anode, the evenly dispersed LiZn alloy particles in Li metal can effectively regulate the Li plating/stripping on electrode surface, reducing deepness of pits during stripping and directionally inducing Li plating to maintain electrode surface stability. On this basis, the pits depth of LiZn/Li composite during Li stripping is reduced to ∼ 15 μm, which is much shallower than that of bare Li metal of ∼ 40 μm. The LiZn/Li composite electrode can stably cycle for 600 h under Li plating/stripping capacity of 1 mAh·cm−2 and current density of 1 mA·cm−2 without any short circuit. Furthermore, assembled LiZn/Li||LiFePO4 full cell presents better cycling stability and rate performances than that of based on bare Li anode.