The Mechanism of Li Deposition on the Cu Substrates in the Anode‐Free Li Metal Batteries

Abstract Due to the rapid growth in the demand for high‐energy‐density Lithium (Li) batteries and insufficient global Li reserves, the anode‐free Li metal batteries are receiving increasing attention. Various strategies, such as surface modification and structural design of copper (Cu) current collectors, have been proposed to stabilize the anode‐free Li metal batteries. Unfortunately, the mechanism of Li deposition on the Cu surfaces with the different Miller indices is poorly understood, especially on the atomic scale. Here, the large‐scale molecular dynamics simulations of Li deposition on the Cu substrates are performed in the anode‐free Li metal batteries. The results show that the surface properties of the Li panel can be altered through the different Cu substrate surfaces. Through surface similarity analysis, potential energy distributions,and inhomogeneous deposition simulations, it is found that the Li atoms exhibit different potential energy variances and kinetic characteristics on the different Cu surfaces. Furthermore, a proposal to reduce the fraction of the (110) facet in commercial Cu foils is made to improve the reversibility and stability of Li plating/stripping in the anode‐free Li metal batteries.