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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. To overcome the inherent incompatibility between high-charge-density Al3+ and conventional cathode materials in AAIBs, this work proposes a novel family of high-entropy Prussian blue analogs (HEPBAs) with a unique lattice "respiration" characteristic and efficient multipath electron transfer. The optimized HEPBAs achieve one of the best long-term stabilities in AAIBs (91.2% capacity retention after 10 000 cycles at 5.0 A g-1). image
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ADVANCED MATERIALS
ISSN: 0935-9648
Year: 2024
Issue: 30
Volume: 36
2 9 . 4 0 0
JCR@2022
Cited Count:
WoS CC Cited Count: 25
SCOPUS Cited Count: 26
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 3
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