Leveraging Machine Learning for Accelerated Electrode–Electrolyte Interface Design in Rechargeable Li‐Based Batteries

Due to their high specific energy, lithium-metal batteries (LMBs) are widely regarded as the promising next-generation energy storage devices. Nevertheless, their practical applications are plagued by the challenges of irregular deposition and dissolution, coupled with the high chemical reactivity of lithium electrodes. Extensive research has focused on the stabilization of electrode-electrolyte interfaces as the key strategy to achieve improved battery performance. However, the exploration process via traditional "trial-and-error" methodologies is impeded by the long period and high cost of the tedious experiments. Machine learning (ML) technologies have become a mainstream force, redefining the revolutionary paradigm, enabling intelligently capturing the complex structure-performance relationships across vast compositional and structural spaces. Herein, ML applications in the discovery of electrolytes, electrodes, and interface engineering are reviewed, with the emphasis on ML-driven investigation workflow covering data collection, feature engineering, model selection and ML-assisted simulations. Moreover, task-oriented ML technologies for expediting materials screening, informative descriptors extraction, mechanistic elucidation, and reverse design of novel electrodes and electrolytes are highlighted. Finally, future trajectories centered on multiscale materials simulation, multimodal modeling, and intelligent platform establishment to overcome persistent challenges are outlined, aiming at catalyzing the rational design of highly stable lithium electrode-electrolyte interface for long-lasting rechargeable LMBs.