  Due to the rapid growth in the demand for high-energy-density 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 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, a large-scale molecular
dynamics simulation of Li deposition on the Cu substrates was performed in the
anode-free Li metal batteries. The results show that the Li layers on the Cu
(100), Cu (110), and Cu (111) surfaces are closer to the structures of Li
(110), Li (100), and Li (110) surfaces, respectively. The mechanism was studied
through the surface similarity analysis, potential energy surfaces, and lattice
features. Finally, a proposal to reduce the fraction of the (110) facet in
commercial Cu foils was made to improve the reversibility and stability of Li
plating/stripping in the anode-free Li metal batteries.
