Dynamic Evolution and Degradation of Silicon–Electrolyte Interfaces under Cycling via Chemical Potential–Controlled Molecular Dynamics

and forming carbonate fragments that bond with Si. Repeated cycling promotes detachment of Si-C-O species into the electrolyte, linking interfacial decomposition with mechanical failure. This study provides a direct atomistic picture of coupled electrode-electrolyte degradation in Si-based batteries and introduces a transferable simulation approach for exploring charge-discharge processes in alloying and intercalation materials.