Integrating First-Principle Calculation and Phase-Field Simulation for Lithium Dendritic Growth on the Anode of a Lithium-Ion Battery

Lithium (Li) dendrite formation compromises the reliability of Li-ion batteries, either because dendrite pieces lose electrical contractor or growing dendrite penetrates the separator and leads to internal short-circuiting. In this paper, a multi-scale computational approach integrating phase-field model and first-principles calculation is proposed to predict the Li dendrite formation at the anode/electrolyte interface of Li-ion batteries. The first-principles calculation is employed to atomically determine the interfacial energy, which is subsequently fed into the phase-field model at the micro-scale. 1D distribution of fields is first analyzed to validate the proposed model. An apparent 2D tree-type Li dendrite, widely observed in experiments during electrodeposition, is produced using the model. Finally, the 2D dendritic evolution under different electrochemical conditions specified by the applied current densities is discussed.