Experimental and computational optimization of Prussian blue analogues as high-performance cathodes for sodium-ion batteries: a review

In this article, we discuss the electrochemical properties of Prussian Blue (PB) for Na+ storage by combining structural engineering and electrolyte modifications. We integrated experimental data and density functional theory (DFT) in sodium-ion battery (SIB) research to refine the atomic arrangements and crystal lattices and introduce substitutions and dopants. These changes affect the lattice stability, intercalation, electronic and ionic conductivities, and electrochemical performance. We unraveled the intricate structure-electrochemical behavior relationship by combining experimental data with computational models, including first-principles calculations. This holistic approach identified techniques for optimizing PB and Prussian Blue Analog (PBA) structural properties for SIBs. We also discuss the tuning of electrolytes by systematically adjusting their composition, concentration, and additives using a combination of molecular dynamics (MD) simulations and DFT computations. Our review offers a comprehensive assessment of strategies for enhancing the electrochemical properties of PB and PBAs through structural engineering and electrolyte modifications, combining experimental insights with advanced computational simulations, and paving the way for next-generation energy storage systems.