SEI Formation\nand Lithium-Ion Electrodeposition Dynamics\nin Lithium Metal Batteries via First-Principles Kinetic Monte Carlo\nModeling

The stabilization and enhanced performance of lithium\nmetal batteries\n(LMBs) depend on the formation and evolution of the Solid Electrolyte\nInterphase (SEI) layer as a critical component for regulating the\nLi metal electrodeposition processes. This study employs a first-principles\nkinetic Monte Carlo (kMC) model to simulate the SEI formation and\nLi<sup>+</sup> electrodeposition processes on a lithium metal anode,\nintegrating both the electrochemical electrolyte reduction reactions\nand the diffusion events giving place to the SEI aggregation processes\nduring battery charge and discharge processes. The model replicates\nthe competitive interactions between organic and inorganic SEI components,\nemphasizing the influence of the cycling regime. Results indicate\nthat grain boundaries within the SEI facilitate faster lithium-ion\ntransport compared to crystalline regions, crucial for improving the\nperformance and stability of LMBs. The findings underscore the importance\nof dynamic SEI modeling for further development of next-generation\nhigh-energy-density batteries.