AI‐Driven Big Data Frameworks for Electrode–Electrolyte Interphases in Batteries

This review presents a comprehensive perspective on how AI and big data strategies can transform the understanding and design of the electrode-electrolyte interphases (EEI) in rechargeable batteries, highlighting their pivotal role in battery performance and longevity. Through uniting high-throughput experimentation and high-throughput computation (HTC), which includes automated cell fabrication, advanced characterization, large-scale HTC screening, and reaction network modeling, diverse datasets can be generated to reveal the mechanistic foundations of interfacial processes. The integration of these datasets with artificial intelligence-orchestrated workflows and machine learning models, such as closed-loop optimization and large language model-assisted hypothesis generation, enables the prediction of interphase behavior, linking molecular-level EEI understanding and macroscale device performance, and data-driven discovery of optimal material combinations. Critically, the review identifies persistent challenges, including limited data standardization, a shortage of high-quality interoperable datasets, the gap between optimization and generalizable understanding, the limits of currently available self-driving labs, and outlines mitigation strategies for building intelligent, data-centric frameworks for rational engineering of next-generation battery systems.