Aqueous aluminum ion batteries (AAIBs) hold significant potential for grid-scale energy storage owing to their intrinsic safety, high theoretical capacity, and abundance of aluminum. However, the strong electrostatic interactions and delayed charge compensation between high-charge-density aluminum ions and the fixed lattice in conventional cathodes impede the development of high-performance AAIBs. To address this issue, this work introduces, for the first time, high-entropy Prussian blue analogs (HEPBAs) as cathodes in AAIBs with unique lattice tolerance and efficient multipath electron transfer. Benefiting from the intrinsic long-range disorder and robust lattice strain field, HEPBAs enable the manifestation of the lattice respiration effect and minimize lattice volume changes, thereby achieving one of the best long-term stabilities (91.2% capacity retention after 10 000 cycles at 5.0 A g⁻¹) in AAIBs. Additionally, the interaction between the diverse metal atoms generates a broadened d-band and reduced degeneracy compared with conventional Prussian blue and its analogs (PBAs), which enhances the electron transfer efficiency with one of the best rate performance (79.2 mAh g⁻¹ at 5.0 A g⁻¹) in AAIBs. Furthermore, exceptional element selectivity in HEPBAs with unique cocktail effect can facile tune electrochemical behavior. Overall, the newly developed HEPBAs with a high-entropy effect exhibit promising solutions for advancing AAIBs and multivalent-ion batteries.

中文翻译：

---

高熵普鲁士蓝类似物能够实现超稳定水系铝离子电池的晶格呼吸


水性铝离子电池（AAIB）由于其本质安全性、高理论容量和丰富的铝元素，在电网规模储能方面具有巨大潜力。然而，高电荷密度铝离子与传统阴极中固定晶格之间的强静电相互作用和延迟电荷补偿阻碍了高性能AAIB的发展。为了解决这个问题，这项工作首次引入高熵普鲁士蓝类似物（HEPBA）作为 AAIB 中的阴极，具有独特的晶格容差和高效的多路径电子转移。受益于固有的长程无序和强大的晶格应变场，HEPBA 能够表现晶格呼吸效应并最大限度地减少晶格体积变化，从而实现最佳的长期稳定性之一（5.0 循环 10 000 次后容量保持率为 91.2%） AAIB 中的 g ⁻¹ )。此外，与传统的普鲁士蓝及其类似物 (PBA) 相比，不同金属原子之间的相互作用产生了更宽的 d 带并减少了简并性，从而提高了电子传输效率，具有最佳倍率性能之一 (79.2 mAh g ⁻¹ at 5.0 A g ⁻¹ ) 在AAIBs中。此外，HEPBA 中出色的元素选择性和独特的鸡尾酒效应可以促进电化学行为的调节。总体而言，新开发的具有高熵效应的 HEPBA 为推进 AAIB 和多价离子电池提供了有前景的解决方案。