Sodium-ion batteries (SIBs) are a viable alternative to meet the requirements of future large-scale energy storage systems due to the uniform distribution and abundant sodium resources. Among the various cathode materials for SIBs, phosphate-based polyanionic compounds exhibit excellent sodium-storage properties, such as high operation voltage, remarkable structural stability, and superior safety. However, their undesirable electronic conductivities and specific capacities limited their application in large-scale energy storage systems. Herein, the development history and recent progress of phosphate-based polyanionic cathodes are first overviewed. Subsequently, the effective modification strategies of phosphate-based polyanionic cathodes are summarized toward high-performance SIBs, including surface coating, morphological control, ion doping, and electrolyte optimization. Besides, the electrochemical performance, cost, and industrialization analysis of phosphate-based polyanionic cathodes for SIBs are discussed for accelerating commercialization development. Finally, the future directions of phosphate-based polyanionic cathodes are comprehensively concluded.  We believe that this review can provide instructive insight into developing practical phosphate-based polyanionic cathodes for SIBs. This article is protected by copyright. All rights reserved.

The Distance Between Phosphate-Based Polyanionic Compounds and Their Practical Application For Sodium-Ion Batteries.

Constructing an inorganic-rich and robust solid electrolyte interphase (SEI) is one of the crucial approaches to improving the electrochemical performance of sodium metal batteries (SMBs). However, the low conductivity and distribution of common inorganics in SEI disturb Na+ diffusion and induce nonuniform sodium deposition. Here, we construct a unique SEI with evenly scattered high-conductivity inorganics by introducing a self-sacrifice LiTFSI into the sodium salt-base carbonate electrolyte. The reductive competition effect between LiTFSI and FEC facilitates the formation of the SEI with evenly scattered inorganics. In which the high-conductive Li3N and inorganics provide fast ions transport domains and high-flux nucleation sites for Na+, thus conducive to rapid sodium deposition at a high rate. Therefore, the SEI derived from LiTFSI and FEC enables the Na∥Na3V2(PO4)3 cell to show 89.15% capacity retention (87.62 mA h g-1) at an ultrahigh rate of 60 C after 10,000 cycles, while the cell without LiTFSI delivers only 48.44% capacity retention even after 8000 cycles. Moreover, the Na∥Na3V2(PO4)3 pouch cell with the special SEI presents a stable capacity retention of 92.05% at 10 C after 2000 cycles. This unique SEI design elucidates a new strategy to propel SMBs to operate under extreme high-rate conditions.

Reductive Competition Effect-Derived Solid Electrolyte Interphase with Evenly Scattered Inorganics Enabling Ultrahigh Rate and Long-Life Span Sodium Metal Batteries.

At present, the energy density of the mainstream lithium iron phosphate battery and ternary lithium battery is between 200 and 300 Wh kg−1 or even <200 Wh kg−1, which can hardly meet the continuous requirements of electronic products and large mobile electrical equipment for small size, light weight and large capacity of the battery. In order to achieve high energy density batteries, researchers have tried to develop electrode materials with higher energy density or modify existing electrode materials, improve the design of lithium batteries and develop new electrochemical energy systems, such as lithium air, lithium sulfur batteries, etc. Here, we analyze the influence of the existing chemical system and structure of lithium-ion battery on the energy density of lithium-ion battery, and summarizes the methods of improving the energy density of lithium-ion battery in the aspects of material preparation and battery structure design. Strategies such as improving the active material of the cathode, improving the specific capacity of the cathode/anode material, developing lithium metal anode/anode-free lithium batteries, using solid-state electrolytes and developing new energy storage systems have been used in the research of improving the energy density of lithium batteries. However, due to a number of difficulties, these high energy density batteries are still in the experimental stage, and further study is needed to improve their practical applicability. 

Strategies toward the development of high-energy-density lithium batteries

Low-cost Prussian blue analogues for sodium-ion batteries and other metal-ion batteries.

Sodium‐ion batteries (SIBs) are regarded as next‐generation secondary batteries and complement to lithium‐ion batteries (LIBs) for large‐scale electrochemical energy storage applications due to the abundant availability, even distribution, and cost‐effectiveness of raw sodium resources. The phosphate‐based polyanions stand out of various cathode material owing to their high operation voltage, stable structure, superior safety, and excellent sodium‐storage properties. The undesirable electric conductivities and specific capacities limit their large‐scale industrialization. Herein, a recent research development of phosphate‐based polyanion cathodes including orthophosphate, oxyphosphate, pyrophosphate, and mixed phosphates is thoroughly reviewed. Subsequently, the effect of modification strategies including element doping, surface coating, morphology control, and electrode design toward high‐performance cathode materials for SIBs are systematically explored. Finally, the future research directions of phosphate‐based polyanion cathodes based on electrochemical performance including reversible capacity, voltage, energy density, rate capacity, cycling stability, and commercial applications are comprehensively concluded. It is believed that current review will present instructive perspectives into developing practicable phosphate‐based polyanion cathode materials for SIBs.

Recent Development of Phosphate Based Polyanion Cathode Materials for Sodium‐Ion Batteries

Metal‐organic frameworks (MOFs) integrate several advantages such as adjustable pore sizes, large specific surface areas, controllable geometrical morphology, and feasible surface modification. Benefiting from these appealing merits, MOFs have recently been extensively explored in the field of advanced secondary batteries. However, a systematic summarization of the specific functional units that these materials can act as in batteries as well as their related design strategies to underline their functions has not been perceived to date. Motivated by this point, this review dedicates to the elucidation of diverse functions of MOFs for batteries, which involve the electrodes, separators, interface modifiers, and electrolytes. Particularly, the main engineering strategies based on the physical and chemical features to enable their enhanced performance have been highlighted for the individual functions. In addition, perspectives and possible research questions in the future development of these materials have also been outlined. This review captures such progress ranging from fundamental understanding and optimized protocols to multidirectional applications of MOF‐based materials in advanced secondary batteries.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/bte2.20220064

Engineering strategies of metal‐organic frameworks toward advanced batteries

Simultaneous cation-anion regulation of sodium vanadium phosphate cathode materials for high-energy and cycle-stable sodium-ion batteries

Polyanion-type phosphate materials with Na-super-ionic conductor structures are promising for next-generation sodium-ion battery cathodes, although the intrinsically low electroconductivity and limited energy density have restricted their practical applications. In this study, we put forward substituting an inert phosphate with a redox-active silicate to improve the energy density and intrinsic electroconductivity of polyanion-type phosphate materials, thus enabling an advance in sodium-ion battery cathodes. As a proof of concept, some of the phosphate of Na3V2(PO4)3 was replaced by silicate to fabricate Na3V2(PO4)2.9(SiO4)0.1, which exhibited a higher average discharge voltage of 3.36 V and a higher capacity of 115.8 mA h g-1 than pristine Na3V2(PO4)3 (3.31 V, 109.6 mA h g-1) at 0.5 C, therefore improving the energy density. Moreover, the introduced silicate enhanced the intrinsic electroconductivity of Na3V2(PO4)3 materials, as confirmed by both theoretical simulation and electrochemical measurements. After pairing with a commercial hard carbon anode, the optimized Na3V2(PO4)2.9(SiO4)0.1 cathode enabled a stable-cycling full cell with 90.1% capacity retention after 300 cycles at 5 C and a remarkable average coulombic efficiency of 99.88%.

Substituting inert phosphate with redox-active silicate towards advanced polyanion-type cathode materials for sodium-ion batteries.

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Engineering strategies of metal‐organic frameworks toward advanced batteries

Simultaneous cation-anion regulation of sodium vanadium phosphate cathode materials for high-energy and cycle-stable sodium-ion batteries

Substituting inert phosphate with redox-active silicate towards advanced polyanion-type cathode materials for sodium-ion batteries.