Herein, potential-tunable Na2 Ni1-x Cux Fe(CN)6 nanoparticles with three-dimensional frameworks and large interstitial spaces were synthesized as alternative cathode materials for aqueous sodium-ion batteries by controlling the molar ratio of Ni(II) to Cu(II) at ambient temperature. The influence of the value of x on the crystalline structure, lattice parameters, electrochemical properties, and charge transfer of the resultant compound was explored by using powder X-ray diffractometry, density functional theory, cyclic voltammetry, galvanostatic charge-discharge techniques, and Bader charge analysis. Of the various formulations investigated, that with x=0.25 delivered the highest reversible capacity, superior rate capability, and outstanding cycling performance. These attributes are ascribed to its unique face-centered cubic structure for facile sodium-ion insertion/extraction and the strong interactions between Cu and N atoms, which promote structural stability.
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