Interfacial Atomistic Evolution in Sodium‐Ion Battery using a Graph‐Theoretic Approach

ABSTRACT Owing to the uneven distribution and high cost of lithium resources, sodium‐ion batteries are considered as an effective alternative and complement to lithium‐ion batteries. However, sodium‐ion batteries are confronted with challenges in forming a stable solid electrolyte interphase, which hinders their large‐scale commercialization. To overcome the limitations of traditional experimental characterization techniques in studying the solid electrolyte interphase formation, our study for the first time constructs the fully atomistic sodium‐ion battery models and explores advanced electrolyte designs. Additionally, we utilize a reaction network integrator based on graph theory to investigate a more realistic interphase formation process. By modeling ether‐ester hybrid electrolytes, our study investigates the evolution of interfacial products and solvation structures during the solid electrolyte interphase formation in sodium‐ion batteries. Our research not only deconstructs the atomistic mechanisms governing inorganic‐rich or organic‐rich SEI formation, but equally furnishes novel perspectives on electrochemical performance augmentation in sodium‐ion batteries.