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Prussian blue attracts the attention of many researchers as a promising candidate for use in sodium-ion battery cathodes due to its open frameworks and high working potential. However, the interstitial water in its crystal structure and its poor electronic conductivity limits its performance in practical sodium-ion batteries. Here, acid-assisted ball milling synthesis was employed as a versatile method for the production of surface-modified Prussian blue. With (CH3COO)2Fe being used as the raw material, the Prussian blue produced using ball milling synthesis was modified by the carboxyl functional group on its surface, which resulted in lower interstitial water content and enhanced electrochemical cycling performance. In addition, ball milling synthesis provided the as-prepared Prussian blue with a large surface area, improving its electrochemical rate performance. When used as the cathode of sodium-ion batteries, as-prepared Prussian blue delivered a specific capacity of 145.3 mAh g−1 at 0.2 C and 113.7 mAh g−1 at 1 C, maintaining 54.5% of the initial capacity after 1000 cycles at 1 C (1 C = 170 mA g−1). Furthermore, a solid-state sodium-ion battery was mounted, with as-prepared Prussian blue being employed as the cathode and Na metal as the anode, which delivered a high specific capacity of 128.7 mAh g−1 at 0.2 C. The present study put forward an effective solution to overcome the limitations of Prussian blue for its commercial application.

Acid-Assisted Ball Mill Synthesis of Carboxyl-Functional-Group-Modified Prussian Blue as Sodium-Ion Battery Cathode