Innovative High‐Entropy Strategy Extending Traditional Metal Substitution for Optimizing Prussian Blue Analogues in Rechargeable Batteries

ABSTRACT High‐entropy materials (HEMs) possess unique properties that can be tailored for specific performance characteristics, making them suitable for various battery applications. In particular, HEMs have shown significant promise in enhancing the electrochemical performance of Prussian blue analogues (PBAs) across various battery systems, including sodium‐ion, potassium‐ion, lithium‐sulfur, aqueous zinc‐ion, and aqueous ammonium‐ion batteries. This article examines case studies to explore how the high‐entropy strategy enhances PBA performance. It also provides an overview of traditional metal substitution methods in modifying the two main types of PBAs, that is, Fe‐based and Mn‐based PBA electrode materials. Additionally, other optimization methods, such as defect modulation, surface modification, composite structures, and electrolyte modulation, are also discussed. Finally, the article delves deeply into the relationship between high‐entropy techniques and traditional metal substitution in modifying PBA electrode materials from the perspectives of element design and performance enhancement, aiming to provide comprehensive theoretical guidance for readers.