Lithium Electrodeposition for Energy Storage: Filling the Gap Between Theory and Experiment

Lithium (Li) metal has been considered a promising anode material for high-energy-density rechargeable batteries, but its utilization is impeded by the nonuniform electrodeposition during the charging process which leads to poor cycling life and safety concerns. Thus, understanding the electrodeposition mech-anism of Li-metal anode is of great importance to develop practical engineering strategies for rechargeable Li-metal batteries. The electrodeposition of Li is controlled by both thermodynamic and kinetic factors, such as the solvation free energy of Li-ions, the Li nucleation, the surface diffusion of Li atom, and the strength of the interaction between Li-ion and the electrolyte anion. The scale of the whole process from the Li-ion reduction to the growth of a Li nucleus goes from sub-nanometer up to a few micrometers, which poses an outstanding challenge to both experiments and simulation. In this perspective, we discuss the top-down, the bottom-up, and the middle-way approaches to this challenge and the possible synergies between them.(c) 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).