Sodium-ion batteries (SIBs) are experiencing a large-scale renaissance to supplement or replace expensive lithium-ion batteries (LIBs) and low energy density lead-acid batteries in electrical energy storage systems and other applications. In this case, layered oxide materials have become one of the most popular cathode candidates for SIBs because of their low cost and comparatively facile synthesis method. However, the intrinsic shortcomings of layered oxide cathodes, which severely limit their commercialization process, urgently need to be addressed. In this review, inherent challenges associated with layered oxide cathodes for SIBs, such as their irreversible multiphase transition, poor air stability, and low energy density, are systematically summarized and discussed, together with strategies to overcome these dilemmas through bulk phase modulation, surface/interface modification, functional structure manipulation, and cationic and anionic redox optimization. Emphasis is placed on investigating variations in the chemical composition and structural configuration of layered oxide cathodes and how they affect the electrochemical behavior of the cathodes to illustrate how these issues can be addressed. The summary of failure mechanisms and corresponding modification strategies of layered oxide cathodes presented herein provides a valuable reference for scientific and practical issues related to the development of SIBs.

Routes to high-performance layered oxide cathodes for sodium-ion batteries.

Lithium-ion batteries (LIBs) have dominated the secondary batteries market in the past few decades. However, their widespread application is seriously hampered by the limited lithium resource and high cost. Recently, sodium-ion batteries (SIBs) have generated significant attention because of their characteristics of abundant raw sources, low cost, and similar “rocking chair” mechanism with LIBs, which hold great application potential in large-scale energy storage. Cathode materials with excellent electrochemical performance are in urgent demand for next-generation SIBs. Herein, this review provides a comprehensive overview of the recent advances of the most promising SIBs cathode candidates, including layered oxides, polyanionic materials, and Prussian blue analogues. The currently existing issues that need to be addressed for these cathodes are pointed out, such as insufficient energy density, low electron conductivity, air sensitivity, and so on. This review also details the structural characteristics of these three cathode candidates. Moreover, the recent optimization strategies for improving the electrochemical performance are summarized, including element doping, morphology modification, structure architecture, and so on. Finally, the current research status and proposed future developmental directions of these three cathode materials are concluded. This review aims to provide practical guidance for the development of cathode materials for next-generation SIBs. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/sstr.202300150

Recent Progress of Promising Cathode Candidates for Sodium‐Ion Batteries: Current Issues, Strategy, Challenge, and Prospects

With the widespread application of electrical energy storage technology, it is particularly essential to develop a new generation of rechargeable batteries with low cost, high capacity, and long cycle life. Alkali-metal ion batteries (AIBs) have attracted great attention in the field of secondary batteries due to their high capacity and impressive rate and cycle performance. As a typical class of AIB cathode material, transition metal (TM) layered oxides have been widely studied and applied by virtue of their unique structure and excellent tunability, but there are still some limitations such as poor capacity retention and inferior structural stability. To date, various modification strategies have been investigated to address these issues. In particular, heteroatom doping is considered to be an effective strategy to modify the lattice architecture of cathode materials. This review summarizes the effect of magnesium ion doping on the structure and performance of AIBs, including alkali metal site doping and TM site doping. Specifically, Mg doping can stabilize the structure, eliminate the order, increase conductivity, and enhance the kinetics, which are beneficial to improve the performance of AIBs. Moreover, some typical materials synthesis methods and in-situ characterization techniques for mechanistic studies are also discussed. Finally, the future development trend of electrode doping strategies for advanced AIBs is analyzed. 

Magnesium ion-doped layered oxide cathodes for alkali-metal ion batteries: recent research progress and outlook

Owing to multi-electron redox reactions and versatile cation storage capabilities, laminated structured metallic vanadate of NH4V4O10 (NHVO) has been regarded as a kind of promising cathode materials for aqueous Zn-ion batteries with satisfactory electrochemical performance. Nevertheless, the NHVO cathode is still limited by the sluggish electrochemical kinetics and structural instability. Here, defect engineering was conducted to introduce the vanadium (V) and oxygen (O) dual defects into NHVO cathode for improving electrochemical performance. As revealed experimentally and theoretically, the migration of Zn-ion inside V/O-defected NHVO cathode can be effectively fostered by increasing active sites, lowering the migration barrier and reducing Gibbs free energy, which are rooted in the synergy impact of the presence of O defect and V defect. As the consequence, the outstanding electrochemical performance has been achieved, which delivers higher capacity of 489 mAh g−1 at 0.5 A g−1 with the capacity retention of 98 % after 100 cycles and exhibits singular cyclic stability at 15 A g−1, maintaining reversible capacity of 198 mAh g−1 after 8000 cycles. This synergistic strategy paves an avenue for accelerating the application of HNVO-based cathode for aqueous Zn-ion battery with satisfactory electrochemical performance and lifespan, advancing the approach of "carbon neutrality" society. 

Synergetic impact of oxygen and vanadium defects endows NH4V4O10 cathode with superior performances for aqueous zinc-ion battery

Sodium‐ion batteries (SIBs) with high energy/power density and low‐cost characteristics are deemed to be one of the best replacements to lithium‐ion batteries for utilizing in large‐scale electric energy storage (EES) devices. Fe‐Mn‐based cathode materials take the leading position in realizing high‐performance SIBs because of their high capacity, environment‐friendly, earth abundant, and low‐cost features, exhibiting huge commercial potential. However, the energy density and cyclic stability are still limited so far, considering the increasing demands for practical applications. In this review, aiming to better understanding the research level and currently existed sore points, the research progress is overviewed for several types of Fe‐Mn‐based cathode materials, including layered oxides, polyanionic compounds and Prussian blue analogues, and refine the electrochemical storage mechanism and structure–performance relationship. Finally, the representative electrochemical performances of these three kinds of cathode materials is summarized, compare the advantages and disadvantages of various materials, point out the existing key scientific problems of these materials, and propose the direction of development in near future. This review makes a thoroughly understanding for Fe‐Mn‐based cathode materials, providing new guidance for future research on SIBs toward real‐world applications.

Earth‐Abundant Fe‐Mn‐Based Compound Cathodes for Sodium‐Ion Batteries: Challenges and Progress

Potassium‐ion batteries (PIBs) have attracted significant research interest in the context of driving the advancement of grid energy storage due to K's elemental abundance and high theoretical output voltage. The main challenge facing PIBs is to find suitable cathode materials with fast transport kinetics and stable framework structures to intercalate/de‐intercalate the large‐size K+. Among these candidates, transition‐metal layered oxides are have excellent potential and have been extensively exploited due to their stable skeleton structure, simple synthetic chemistry, and high working potential. Herein, the current research status and prospects of layered transition‐metal oxide cathodes are summarized, especially focussing on the fine structure optimization engineering and energy storage mechanism. In addition, a brief overview of the research on advanced characterization techniques for PIBs is introduced in detail. Finally, the main research directions and hot spots of new‐type transition‐metal layered oxide cathode are also predicted, in order to guide the future development of advanced PIBs.

Advances in Fine Structure Optimizations of Layered Transition‐Metal Oxide Cathodes for Potassium‐Ion Batteries

To enhance the energy density of batteries and explore intrinsic charge storage mechanism of the active materials, it is important to reduce or eliminate the use of non‐active materials in electrodes, such as binder and conductive additives. Herein, free‐standing Na4MnV(PO4)3@C (F‐NMVP@C) fiber membrane is fabricated and directly used as a sodium‐ion battery (SIB) cathode. In situ X‐ray diffraction reveals that the V3+/V4+ redox reaction occurs through a solid‐solution reaction while a two‐phase Mn2+/Mn3+ redox reaction is identified, and both are highly reversible. Meanwhile, ex situ electrochemical impedance spectroscopy reveals that both the ion diffusion coefficient and charge transfer resistance of F‐NMVP@C change reversibly during the Na+ intercalation/de‐intercalation. Battery full cells are assembled based on the free‐standing F‐NMVP@C cathodes and F‐Sb@C anodes, which manifests a high energy density (293 Wh kg−1) and good cyclability (87.5% after 100 cycles at 1 C). The high‐performance free‐standing cathodes and anodes shed light on the development of flexible SIBs.

Sodium Ion Storage in Na4MnV(PO4)3@C Free‐Standing Electrode

Carbon-based materials are one of the ideal negative electrode materials for potassium ion batteries. However, the limited active sites and sluggish diffusion ion kinetics still hinder its commercialization process. To address these problems, we design a novel carbon composite anode, by confining highly reactive short-chain sulfur molecules into nitrogen-doped hollow carbon nanospheres (termed SHC-450). The formation process involves the controlled synthesis of hollow polyaniline (PANI) nanospheres as precursors via an Ostwald ripening mechanism and subsequent sulfuration treatment. The high content of constrained short-chain sulfur molecules (20.94 wt%) and considerable N (7.15 wt%) ensure sufficient active sites for K+ storage in SHC-450. Accordingly, the SHC-450 electrode exhibits a high reversible capacity of 472.05 mAh g−1 at 0.1 A g−1 and good rate capability (172 mAh g−1 at 2 A g−1). Thermogravimetric analysis shows that SHC-450 has impressive thermal stability to withstand a high temperature of up to 640 °C. Ex situ spectroscopic characterizations reveal that the short-chain sulfur provides high capacity through reversible formation of K2S. Moreover, its special hollow structure not only provides ample space for highly active short-chain sulfur reactants but also effectively mitigates volume expansion during the sulfur conversion process. This work offers new perspectives on enhanced K+ storage performance from an interesting anode design and the space-limited domain principle.

Short-Chain Sulfur Confined into Nitrogen-Doped Hollow Carbon Nanospheres for High-Capacity Potassium Storage

Lignin modification for in-situ cured lignin-maleyl network in semi-crystalline polyamide/lignin shape memory composites

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Advances in Fine Structure Optimizations of Layered Transition‐Metal Oxide Cathodes for Potassium‐Ion Batteries

Sodium Ion Storage in Na4MnV(PO4)3@C Free‐Standing Electrode

Short-Chain Sulfur Confined into Nitrogen-Doped Hollow Carbon Nanospheres for High-Capacity Potassium Storage

Lignin modification for in-situ cured lignin-maleyl network in semi-crystalline polyamide/lignin shape memory composites