Abstract In recent decades, sodium‐ion batteries (SIBs) have received increasing attention because they offer cost and safety advantages and avoid the challenges related to limited lithium/cobalt/nickel resources and environmental pollution. Because the sodium storage performance and production cost of SIBs are dominated by the cathode performance, developing cathode materials with large‐scale production capacity is the key to achieving commercial applications of SIBs. Therefore, developing host materials with high energy density, long cycling life, low production cost, and high chemical/environmental stability is crucial for implementing advanced SIBs. Among the developed cathode materials for SIBs, O3‐type sodiated transition‐metal oxides have attracted extensive attention owing to their simple synthesis methods, high theoretical specific capacity, and sufficient Na content. However, the relatively large Na‐ion radius leads to sluggish diffusion kinetics and inevitable complex phase transitions during the deintercalation/intercalation process, resulting in poor rate capability and cycling stability. Therefore, this review comprehensively summarizes the research progress and modification strategies for O3‐type cathodes, including the component design, surface modification, and optimization of synthesis methods. This work aims to guide the development of commercial layered oxides and provide technical support for the next generation of energy‐storage systems. 

Practical Cathodes for Sodium‐Ion Batteries: Who Will Take The Crown?

Low‐cost sodium‐ion batteries (SIBs) have been extensively considered as a supplement or even a replacement for successful lithium‐ion batteries. However, the practical application of SIBs is limited by their energy density and cyclic performance, which are mainly constrained by the cathode side. Therefore, the development of advanced cathode materials is essential for the practical application of SIBs. Among the various cathode materials, layered transition metal oxides (LTMOs) are highly promising candidates due to their compact crystal structure, low‐cost, ease of preparation, and similarities to successful Li‐based LTMOs. Unfortunately, the bottleneck issues faced by Na‐based LTMOs, such as severe phase transitions, sluggish diffusion kinetics, and interface deterioration, pose significant challenges in achieving high‐performance cathodes. In this review, a comprehensive overview and summary of recently reported modification strategies for layered oxides are provided and the structure–function–performance relationship is refined. A perspective on the outlook and development direction for Na‐based LTMOs cathodes is also provided. This review comprehensively explores the modification strategies of Na‐based LTMOs, providing a new horizon for future research on Na‐based LTMOs.

Recent Progress in the Emerging Modification Strategies for Layered Oxide Cathodes toward Practicable Sodium Ion Batteries

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.

Alloying‐type bismuth with high volumetric capacity has emerged as a promising anode for sodium‐ion batteries but suffers from large volume expansion and continuous pulverization. Herein, a coordination constraint strategy is proposed, that is, chemically confining atomic Bi in an intercalation host framework via reconstruction‐favorable linear coordination bonds, enabling a novel quasi‐topological intercalation mechanism. Specifically, micron‐sized Bi0.67NbS2 is synthesized, in which the Bi atom is linearly coordinated with two S atoms in the interlayer of NbS2. The robust Nb−S host framework provides fast ion/electron diffusion channels and buffers the volume expansion of Na+ insertion, endowing Bi0.67NbS2 with a lower energy barrier (0.141 vs. 0.504 eV of Bi). In situ and ex situ characterizations reveal that Bi atom alloys with Na+ via a solid‐solution process and is constrained by the reconstructed Bi−S bonds after dealloying, realizing complete recovery of crystalline Bi0.67NbS2 phase to avoid the migration and aggregation of atomic Bi. Accordingly, the Bi0.67NbS2 anode delivers a reversible capacity of 325 mAh g−1 at 1 C and an extraordinary ultrahigh‐rate stability of 226 mAh g−1 at 100 C over 25 000 cycles. The proposed quasi‐topological intercalation mechanism induced by coordinated mode modulation is expected to be be conducive to the practical electrode design for fast‐charging batteries.

Quasi‐Topological Intercalation Mechanism of Bi0.67NbS2 Enabling 100 C Fast‐Charging for Sodium‐Ion Batteries

When compared to expensive lithium metal, the metal sodium resources on Earth are abundant and evenly distributed. Therefore, low-cost sodium-ion batteries are expected to replace lithium-ion batteries and become the most likely energy storage system for large-scale applications. Among the many anode materials for sodium-ion batteries, hard carbon has obvious advantages and great commercial potential. In this review, the adsorption behavior of sodium ions at the active sites on the surface of hard carbon, the process of entering the graphite lamellar, and their sequence in the discharge process are analyzed. The controversial storage mechanism of sodium ions is discussed, and four storage mechanisms for sodium ions are summarized. Not only is the storage mechanism of sodium ions (in hard carbon) analyzed in depth, but also the relationships between their morphology and structure regulation and between heteroatom doping and electrolyte optimization are further discussed, as well as the electrochemical performance of hard carbon anodes in sodium-ion batteries. It is expected that the sodium-ion batteries with hard carbon anodes will have excellent electrochemical performance, and lower costs will be required for large-scale energy storage systems.

/pdf/the-progress-of-hard-carbon-as-an-anode-material-in-sodium-3uhlpdpj.pdf

The Progress of Hard Carbon as an Anode Material in Sodium-Ion Batteries

Cathode materials are critical for Na-ion batteries while facing challenges due to the instability of the structure and interfaces. In this work, we propose a strategy to achieve an in situ plastic-crystal Na3–3xAlxPO4 coating and bulk Al doping for an O3-NaNi0.4Fe0.2Mn0.4O2 cathode through a simple one-step method. Na3–3xAlxPO4 exhibits high ion transport performance due to its unique “paddle-wheel” mechanism. The in situ formed Na3–3xAlxPO4 could consume the residual alkali compounds and induce the formation of a Na-deficient phase, thus leading to enhanced Na+ transport kinetics. Furthermore, strong Al–O bonds formed in the bulk further enhance the crystal structure stability. In a full cell, the capacity retention rate reached 70% after 500 cycles, making its commercial operation possible. Altogether, these results suggest that the in situ plastic-crystal-coating strategy can significantly improve the surface and bulk structure stability of NaNi0.4Fe0.2Mn0.4O2, thus leading to improved electrochemical performance. 

In Situ Plastic-Crystal-Coated Cathode toward High-Performance Na-Ion Batteries

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