Synthesis of Low-Defect Iron-Based Prussian Blue with Low Water Content for High-Stability Sodium-Ion Batteries.

This study proposes an innovative two-step synthesis strategy to significantly enhance the performance of sodium-ion batteries by developing low-defect, low water content iron-based Prussian blue (PB) materials. Addressing the limitations of traditional co-precipitation methods-such as rapid reaction rates leading to excessive crystal defects and interstitial water content-the research team introduced a synergistic approach combining non-aqueous phase precursor synthesis and controlled water-concentration secondary crystallization. The process involves preparing a PB precursor in a glycerol system, followed by secondary crystallization in a water-/ethanol-mixed solvent with a precisely regulated water content, achieving the dual objectives of water content reduction and crystal morphology optimization. Systematic characterization revealed that water concentration during secondary synthesis critically influences the material's crystal structure, morphological features, and water content. The optimized PB50-24 material exhibited a highly regular cubic morphology with a sodium content of 9.2% and a remarkably low interstitial water content of 2.1%. Electrochemical tests demonstrated outstanding performance-an initial charge-discharge capacity of 120 mAh g-1 at a 1C rate, the retention of 105 mAh g-1 after 100 cycles, and a high rate capability of 86 mAh g-1 at 10C, representing significant improvements in cycling stability and rate performance over conventional methods. This work not only establishes a cost-effective, scalable synthesis pathway for Prussian blue materials but also provides theoretical guidance for developing other metal-based Prussian blue analogs, offering substantial value for advancing the industrial application of sodium-ion batteries in next-generation energy storage systems.