First-principles studies on the atomistic properties of metallic magnesium as anode material in magnesium-based batteries

Rechargeable magnesium-ion batteries (MIBs) are a promising alternative to commercial lithium-ion batteries (LIBs). They are safer to handle, environmentally more friendly, and provide a five-time higher volumetric capacity (3832 mAh·cm-3) than commercialized LIBs. However, the formation of a passivation layer on metallic Mg electrodes is still a major challenge towards their commercialization. Using density functional theory, the atomistic properties of metallic magnesium, such as bulk, surface, and adsorption properties, were examined. Well-selected self-diffusion processes on perfect and imperfect Mg surfaces were investigated to better understand the initial surface growth phenomena. Subsequently, rate constants and activation temperatures of crucial diffusion processes on Mg(0001) and Mg(101m1) were determined, providing preliminary insights into the surface kinetics of metallic Mg electrodes.