SEI Formation and Lithium-Ion Electrodeposition Dynamics in Lithium Metal Batteries via First-Principles Kinetic Monte Carlo Modeling

Saul Perez-Beltran; Dacheng Kuai; Perla B Balbuena

doi:10.1021/acsenergylett.4c02019

SEI Formation and Lithium-Ion Electrodeposition Dynamics in Lithium Metal Batteries via First-Principles Kinetic Monte Carlo Modeling

ACS Energy Lett. 2024 Oct 7;9(11):5268-5278. doi: 10.1021/acsenergylett.4c02019. eCollection 2024 Nov 8.

Authors

Saul Perez-Beltran¹, Dacheng Kuai^{1

2}, Perla B Balbuena^{1

2

3}

Affiliations

¹ Department of Chemical Engineering, Texas A&M University, College Station, Texas 77843, United States.
² Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States.
³ Department of Materials Science and Engineering, Texas A&M University, College Station, Texas 77843, United States.

Abstract

The stabilization and enhanced performance of lithium metal batteries (LMBs) depend on the formation and evolution of the Solid Electrolyte Interphase (SEI) layer as a critical component for regulating the Li metal electrodeposition processes. This study employs a first-principles kinetic Monte Carlo (kMC) model to simulate the SEI formation and Li⁺ electrodeposition processes on a lithium metal anode, integrating both the electrochemical electrolyte reduction reactions and the diffusion events giving place to the SEI aggregation processes during battery charge and discharge processes. The model replicates the competitive interactions between organic and inorganic SEI components, emphasizing the influence of the cycling regime. Results indicate that grain boundaries within the SEI facilitate faster lithium-ion transport compared to crystalline regions, crucial for improving the performance and stability of LMBs. The findings underscore the importance of dynamic SEI modeling for further development of next-generation high-energy-density batteries.