Prussian blue and its analogues have received particular attention as superior cathodes for Na-ion batteries due to their potential 2-Na storage capacity (∼170 mAh g(-1)) and low cost. However, most of the Prussian blue compounds obtained from the conventional synthetic routes contain large amounts of Fe(CN)6 vacancies and coordinated water molecules, which leads to the collapse of cyano-bridged framework and serious deterioration of their Na-storage ability. Herein, we propose a facile citrate-assisted controlled crystallization method to obtain low-defect Prussian blue lattice with greatly improved Na-storage capacity and cycling stability. As an example, the as-prepared Na2CoFe(CN)6 nanocrystals demonstrate a reversible 2-Na storage reaction with a high specific capacity of 150 mAh g(-1) and a ∼ 90% capacity retention over 200 cycles, possibly serving as a low cost and high performance cathode for Na-ion batteries. In particular, the synthetic strategy described in this work may be extended to other coordination-framework materials for a wide range of energy conversion and storage applications.

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