Quantitative Analysis and Prediction of Thermal Runaway Metrics of High-Nickel Oxide Cathodes by Machine Learning Models

Abstract The pursuit of higher energy density in lithium-ion batteries has made high-nickel (Ni) layered oxides leading cathode candidates for next-generation electric vehicles. However, their poor thermal stability, particularly at Ni contents ≥90%, increases the risk of cathode-initiated thermal runaway. Here, we present a data-driven framework combining linear and nonlinear machine learning models to predict key thermal runaway descriptors from a high-throughput differential scanning calorimetry database. With cathode composition and state of charge (SOC) as input features, the ensemble model accurately predicts peak temperature, heat release, and peak heat flow. SHAP analysis identifies Ni content and SOC as the dominant factors controlling thermal runaway temperature, while SOC primarily governs heat release and peak heat flow. Al, Mg, and Mn improve thermal stability by strengthening metal−oxygen bonding and delaying structural transformation, whereas B mainly reduces heat release through surface passivation. Validation with a new cathode composition confirms accurate prediction of SOC-dependent thermal runaway behavior and critical SOC.