Abstract

Inducing uniform nucleation and unidirectional growth of lithium (Li) electrodeposition is of vital significance to achieve dendrite-free lithium metal batteries. Herein, a lateral growth model of Li electrodeposition on the single crystal Cu with (110) crystallographic plane is realized. The influence of grain boundaries and crystal grains on the electrodeposition of Li metal and related mechanisms are further explained from the perspective of thermodynamics. The combined simulation and experiment results reveal that the electrodeposited Li grows along (110) crystallographic plane of single crystal Cu foil due to the homogeneous physical and chemical properties surfaces, indicating a typical lateral growth model. With the achieved smooth and flat Li metal electrodeposition layer on the single crystal Cu substrate, the Li|Cu half cell exhibits a high initial Coulombic efficiency of ~98% under different current densities of 0.5 and 1.0 mA cm−2, and Li|NCM523 full cell displays remarkable cycle stability with a high cycle retention of 76.71% even after 300 cycles at the current density of 1 C. This work not only proposes the electrocrystalline growth model of Li metal, but also provides guidance for the commercialization of safe and stable LMBs.

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