Research on Calendar Aging Modeling of Sulfide All-Solid-State Batteries Based on the Electron Tunneling Mechanism

To address ambiguous aging mechanisms and inadequate predictive accuracy of traditional empirical models for sulfide-based all-solid-state batteries (ASSBs) during long-term storage, this study develops an innovative multiscale coupled aging model based on electron tunneling dynamics.From a quantum mechanical perspective, electron tunneling across the cathode-electrolyte interphase (CEI) energy barrier is the microscopic origin of calendar capacity degradation, with a quantitative logarithmic correlation between capacity loss and time.Integrating an equivalent circuit model (ECM) to reconstruct interfacial overpotentials, the model couples macroscopic electrochemical kinetics with microscopic interfacial reactions.Calibrated via experimental data at 25°C/45°C (varied SOC) and validated at 5°C, 35°C, and 55°C, it exhibits low root-mean-square error (RMSE) for precise aging prediction over a wide temperature and full SOC range.This study provides a physically grounded framework for interfacial degradation and a robust basis for BMS lifespan prediction.