First-principles study of the adsorption and diffusion mechanisms of lithium dendrite growth

Lithium dendrite growth is an important issue in the design of lithium metal batteries (LMBs), and most relevant experimental studies lack theoretical guidance. We employ density functional theory to study the adsorption and diffusion of lithium atoms, which are two dominating factors for dendrite growth, by calculating the binding energy and potential map. Perfect, dislocation defective and heteroatom defective surfaces are considered. For a perfect surface, dendrite growth on the (110) face compared to the (200) face is dominated more by the adsorption mechanism. For dislocation defects, an extra potential barrier is found on the section of the dislocation, which might lead to uncontrolled dendrite growth. For heteroatom defects, the influence is correlated with the face direction due to the correlation between the chemical bond and cell parameters; it seems that Si, P and B are unfavourable, while F, Cl and alkali metal atoms are favourable for dendrite-free LMBs.