Prussian blue analogues (PBAs) have attracted wide attention for their application in the energy storage and conversion field due to their low cost, facile synthesis, and appreciable electrochemical performance. At the present stage, most research on PBAs is focused on their material-level optimization, whereas their properties in practical battery systems are seldom considered. This review aims to first provide an overview of the history and parameters of PBA materials and analyze the fundamental principles toward rational design of PBAs, and then evaluate the prospects and challenges for PBAs for practical sodium-ion batteries, hoping to bridge the gap between laboratory research and commercial reality. 

Prussian Blue Analogues for Sodium‐Ion Batteries: Past, Present, and Future

Hexacyanoferrate-Type Prussian Blue Analogs: Principles and Advances Toward High-Performance Sodium and Potassium Ion Batteries

Prussian blue, its analogues and their derived materials for electrochemical energy storage and conversion

Recent advancements in Prussian blue analogues: Preparation and application in batteries

The Na-ion battery is currently the focus of much research interest due to its cost advantages and the relative abundance of sodium as compared to lithium. Olivine NaMPO4 (M = Fe, Fe0.5Mn0.5, Mn) and layered Na2FePO4F are interesting materials that have been reported recently as attractive positive electrodes. Here, we report their Na-ion conduction behavior and intrinsic defect properties using atomistic simulation methods. In the olivines, Na ion migration is essentially restricted to the [010] direction along a curved trajectory, similar to that of LiMPO4, but with a lower migration energy (0.3 eV). However, Na/M antisite defects are also predicted to have a lower formation energy: the higher probability of tunnel occupation with a relatively immobile M2+ cation – along with a greater volume change on redox cycling – contributes to the poor electrochemical performance of the Na-olivine. Na+ ion conduction in Na2FePO4F is predicted to be two-dimensional (2D) in the interlayer plane with a similar low activation energy. The antisite formation energy is slightly higher; furthermore, antisite occupation would not be predicted to impede transport significantly owing to the 2D pathway. This factor, along with the much lower volume change on redox cycling, is undoubtedly responsible for the better electrochemical performance of the layered structure. Where volume change and structural effects do not incur impediments, Na-ion materials may present significant advantages over their Li counterparts.

Na-ion mobility in layered Na2FePO4F and olivine Na[Fe,Mn]PO4

Low-cost manganese hexacyanoferrate (NMHCF) possesses many favorable advantages including high theoretical capacity, ease of preparation, and robust open channels that enable faster Na+ diffusion kinetics However, high lattice water and low electronic conductivity are the main bottlenecks to their pragmatic realization Here, we present a strategy by anchoring NMHCF on reduced graphene oxide (RGO) to alleviate these problems, featuring a specific discharge capacity of 161/121 mA h g–1 at a current density of 20/200 mA g–1 Moreover, the sodiation process is well revealed by ex situ X-ray diffraction, EIS and Car–Parrinello molecular dynamics simulations At a rate of 20 mA g–1, the hard carbon//NMHCF/RGO full cell affords a stable discharge capacity of 84 mA h g–1 (based on the weights of cathode mass) over 50 cycles, thus highlighting NMHCF/RGO an alternative cathode for sodium-ion batteries

Reduced Graphene Oxide-Anchored Manganese Hexacyanoferrate with Low Interstitial H2O for Superior Sodium-Ion Batteries

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Reduced Graphene Oxide-Anchored Manganese Hexacyanoferrate with Low Interstitial H2O for Superior Sodium-Ion Batteries