Stable Manganese-Based High-Entropy Prussian Blue for Enhanced Sodium-Ion Storage

Prussian blue (PB) and its analogs (PBAs) are considered ideal cathode materials for sodium-ion batteries (SIBs) due to the following merits, including high redox potential, simple synthesis methods, and excellent structural stability. Herein, we synthesized a high-entropy PB cathode material, Na1.20Mn0.38Fe0.15Ni0.14Co0.15Cu0.16[Fe(CN)6]0.82□0.18·0.38H2O (HE-HCF), through a facile co-precipitation method. The five transition metals in HE-HCF have similar atomic sizes and electronegativity, collectively occupying the high-spin Fe-HS sites. The manganese-based system design reduces the preparation cost, and the high-entropy doping approach further decreases the content of crystalline water in the structure. Benefiting from the synergistic effects of the multiple component elements, HE-HCF demonstrates a capacity retention rate of 72.7% at 0.1 A g−1. Moreover, it even maintains 85.3% of its initial capacity after 1000 cycles at 1 A g−1. Electrochemical impedance spectroscopy (EIS) and galvanostatic intermittent titration technique (GITT) analyses further confirm that HE-HCF exhibits low charge transfer resistance and a small reaction activation energy.