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![a1) Photograph of the coprecipitation system with 10 L capacity. a2) SEM image of Na[Li0.05Mn0.50Ni0.30Cu0.10Mg0.05]O2 cathode material. a3) STEM image of primary Na[Li0.05Mn0.50Ni0.30Cu0.10Mg0.05]O2 nanoplate. a4) XRD pattern and refinement results, with molecular model structure as inset image. a5) EELS signals of corresponding elements. Reproduced with permission.[¹⁰¹] Copyright 2017, Wiley‐VCH. b1) Powder XRD pattern and Rietveld refinement plot. b2) SEM image. b3) TEM image. b4,b5) HRTEM image at the [001] zone axis and corresponding selected area electron diffraction (SAED) image. b6) HRTEM image at the [010] zone axis of P2‐NaNMCM cathode material. Reproduced with permission.[¹⁰²] Copyright 2019, Wiley‐VCH. c1) Schematic illustration of fabrication process for Na0.7CoO2 arrays. c2) XRD pattern. c3) SEM image. Reproduced with permission.[¹⁰³] Copyright 2018, Elsevier.](profile/Yao-Xiao-108/publication/341043759/figure/fig2/AS:11431281173282235@1688811724659/a1-Photograph-of-the-coprecipitation-system-with-10-L-capacity-a2-SEM-image-of.png)
a1) Photograph of the coprecipitation system with 10 L capacity. a2) SEM image of Na[Li0.05Mn0.50Ni0.30Cu0.10Mg0.05]O2 cathode material. a3) STEM image of primary Na[Li0.05Mn0.50Ni0.30Cu0.10Mg0.05]O2 nanoplate. a4) XRD pattern and refinement results, with molecular model structure as inset image. a5) EELS signals of corresponding elements. Reproduced with permission.[¹⁰¹] Copyright 2017, Wiley‐VCH. b1) Powder XRD pattern and Rietveld refinement plot. b2) SEM image. b3) TEM image. b4,b5) HRTEM image at the [001] zone axis and corresponding selected area electron diffraction (SAED) image. b6) HRTEM image at the [010] zone axis of P2‐NaNMCM cathode material. Reproduced with permission.[¹⁰²] Copyright 2019, Wiley‐VCH. c1) Schematic illustration of fabrication process for Na0.7CoO2 arrays. c2) XRD pattern. c3) SEM image. Reproduced with permission.[¹⁰³] Copyright 2018, Elsevier.
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Considering the ever‐growing climatic degeneration, sustainable and renewable energy sources are needed to be effectively integrated into the grid through large‐scale electrochemical energy storage and conversion (EESC) technologies. With regard to their competent benefit in cost and sustainable supply of resource, room‐temperature sodium‐ion batte...
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Citations
... Being a critical element of SIBs, the cathode material significantly influences their specific capacities, energy densities, power densities, and overall lifespan [27][28][29][30] . However, due to the large size of Na + (1.02 Å) embedded in/out of the electrode structure, the material will produce irreversible volume and structural deformation, resulting in capacity decay, limiting the development of SIBs [31][32][33][34] . Therefore, it is crucial to develop a stable cathode material. ...
Sodium-ion batteries (SIBs) are recognized as a leading option for energy storage systems, attributed to their environmental friendliness, natural abundance of sodium, and uncomplicated design. Cathode materials are crucial in defining the structural integrity and functional efficacy of SIBs. Recent studies have extensively focused on manganese (Mn)-based layered oxides, primarily due to their substantial specific capacity, cost-effectiveness, non-toxic nature, and ecological compatibility. Additionally, these materials offer a versatile voltage range and diverse configurational possibilities. However, the complex phase transition during a circular process affects its electrochemical performance. Herein, we set the multiphase Mn-based layered oxides as the research target and take the relationship between the structure and phase transition of these materials as the starting point, aiming to clarify the mechanism between the microstructure and phase transition of multiphase layered oxides. Meanwhile, the structure-activity relationship between structural changes and electrochemical performance of Mn-based layered oxides is revealed. Various modification methods for multiphase Mn-based layered oxides are summarized. As a result, a reasonable structural design is proposed for producing high-performance SIBs based on these oxides.
... 22 There have been relatively systematic and comprehensive studies on anodes for SIBs, and the key factor limiting the battery performance and lifespan is the cathode material. 23,24 As a result, from Figure 1A we can tell that the study of cathode materials occupies a considerable part of researches in the field of sodium-ion batteries. Up to now, layered transition metal oxides, polyanionic type compounds, organic compounds and Prussians blue compounds take up the majority of the commonly used cathode materials for SIBs. ...
With the advantages of similar theoretical basis to lithium batteries, relatively low budget and the abundance of sodium resources, sodium ion batteries (SIBs) are recognized as the most competitive alternative to lithium‐ion batteries. Among various types of cathodes for SIBs, advantages of high theoretical capacity, nontoxic and facile synthesis are introduced for layered transition metal oxide cathodes and therefore they have attracted huge attention. Nevertheless, layered oxide cathodes suffer from various degradation issues. Among these issues, interface instability including surface residues, phase transitions, loss of active transition metal and oxygen loss takes up the major part of the degradation of layered oxides. These degradation mechanisms usually lead to irreversible structure collapse and cracking generation, which significantly influence the interface stability and electrochemical performance of layered cathodes. This review briefly introduces the background of researches on layered cathodes for SIBs and their basic structure types. Then the origins and effects on layered cathodes of degradation mechanisms are systematically concluded. Finally, we will summarize various interface modification methods including surface engineering, doping modification and electrolyte composition which are aimed to improve interface stability of layered cathodes, perspectives of future research on layered cathodes are mentioned to provide some theoretical proposals.
... The high-resolution spectrum of Ti 2p is presented in Fig. S3c, where the peaks at the binding energy of 463.38 eV and 457.58 eV can be correspond with Ti 2p 1/2 and Ti 2p 3/2 , indicating the tetravalent stoichiometry of Ti. As depicted in Fig. S3d, the Mn 2p spectrum of L-NaMT-0 and L/T-NaMT-1 consists of Mn 2p 1/2 and Mn 2p 2/3 peaks located adjacent to 642 eV and 653 eV, with each peak fitting to be divided to Mn 3+ and Mn 4+ peaks [41][42][43]. The morphological microstructure of L/T-NaMT-X cathode materials was characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). ...
... With the rise of the EV and HEV markets, the demand for lithium has increased dramatically, while the uneven distribution and limited reserves of lithium resources in the earth's crust have further triggered the fluctuating prices. Compared with lithium, sodium with high abundance is widely distributed in the earth's crust and sea, and have similar intercalation chemistry [1][2][3][4][5], which demonstrates great potential for application in stationary energy storage systems [6,7]. ...
... In addition, the protective layer can further improve its environmental stability. Atomic layer deposition (ALD) technology is an effective way to realize surface coating at atomic scale with a precise and uniform thickness control, have been widely applied in many energy storage systems [7,[130][131][132]. Yang [133] prepared thin Al 2 O 3 coating (about 3 nm) NaNi 0.5 Mn 0.5 O 2 via ALD, which presents an excellent capacity retention of 68.0% after 300 cycles at 0.5 C, along with improved rate capability. ...
Sodium ion batteries (SIBs) have attracted great interest as candidates in stationary energy storage systems relying on low cost, high abundance and outstanding electrochemical properties. The foremost challenge in advanced NIBs lies in developing high-performance and low-cost electrode materials. To accelerate the commercialization of sodium ion batteries, various types of materials are being developed to meet the increasing energy demand. O3-type layered oxide cathode materials show great potential for commercial applications due to their high reversible capacity, moderate operating voltage and easy synthesis, while allowing direct matching of the negative electrode to assemble a full battery. Here, representative progress for Ni/Fe/Mn based O3-type cathode materials have been summarized, and existing problems, challenges and solutions are presented. In addition, the effects of irreversible phase transitions, air stability, structural distortion and ion migration on electrochemical performance are systematically discussed. We hope to provide new design ideas or solutions to advance the commercialization of sodium ion batteries.
... A well-designed internal structure can even activate reversible anionic redox to get high specific capacity; therefore, the energy density is also enhanced. 106 ...
Considering the abundance and low price of sodium, sodium‐ion batteries (SIBs) have shown great potential as an alternative to existing lithium‐based batteries in large‐scale energy storage systems, including electric automobiles and smart grids. Cathode materials, which largely decide the cost and the electrochemical performance of the full SIBs, have been extensively studied. Among the reported cathodes, layered transition‐metal oxides (LTMOs) are regarded as the most extremely promising candidates for the commercial application of the SIBs owing to their high specific capacity, superior redox potential, and suitable scalable preparation. Nevertheless, irreversible structural evolution, sluggish kinetics, and water sensitivity are still the critical bottlenecks for their practical utilization. Nanoengineering may offer an opportunity to address the above issues by increasing reactivity, shortening diffusion pathways, and strengthening structural stability. Herein, a comprehensive summary of the modification strategies for LTMOs is presented, emphasizing optimizing the structure, restraining detrimental phase transition, and promoting diffusion kinetics. This review intends to facilitate an in‐depth understanding of structure–composition–property correlation and offer guidance to the further development of the LTMO cathodes for next‐generation energy storage systems.
... Meanwhile, it must be admitted that SIBs show inferior performance in terms of energy density and diffusion kinetics compared with LIBs as Na has a relatively higher weight (Li: 6.9 g mol À1 , Na: 23 g mol À1 ), ionic radius (Li + : 0.76 Å, Na + : 1.02 Å), and standard electrochemical potential (Li: À3.04 V, Na: À2.71 V vs. standard hydrogen electrode) than Li. [38][39][40][41] These intrinsic factors also pose a great challenge for applying layered oxide cathodes in SIBs to completely meet the practical application requirements of large-scale EESs. ...
Sodium‐ion batteries (SIBs) are considered as a low‐cost complementary or alternative system to prestigious lithium‐ion batteries (LIBs) because of their similar working principle to LIBs, cost‐effectiveness, and sustainable availability of sodium resources, especially in large‐scale energy storage systems (EESs). Among various cathode candidates for SIBs, Na‐based layered transition metal oxides have received extensive attention for their relatively large specific capacity, high operating potential, facile synthesis, and environmental benignity. However, there are a series of fatal issues in terms of poor air stability, unstable cathode/electrolyte interphase, and irreversible phase transition that lead to unsatisfactory battery performance from the perspective of preparation to application, outside to inside of layered oxide cathodes, which severely limit their practical application. This work is meant to review these critical problems associated with layered oxide cathodes to understand their fundamental roots and degradation mechanisms, and to provide a comprehensive summary of mainstream modification strategies including chemical substitution, surface modification, structure modulation, and so forth, concentrating on how to improve air stability, reduce interfacial side reaction, and suppress phase transition for realizing high structural reversibility, fast Na⁺ kinetics, and superior comprehensive electrochemical performance. The advantages and disadvantages of different strategies are discussed, and insights into future challenges and opportunities for layered oxide cathodes are also presented.
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... The SLOC with different specific microstructure can effectively improve its electrochemical kinetics, stable cycling performance, and excellent rate performance. Among all kinds of microscopic morphologies, the microsphere structure can not only improve the volume energy density by enhancing the high tap density, but also fasten ions' motion by shortening the electron/Na + transport diffusion paths [67,68]. ...
Because of the low price and abundant reserves of sodium compared with lithium, the research of sodium-ion batteries (SIBs) in the field of large-scale energy storage has returned to the research spotlight. Layered oxides distinguish themselves from the mains cathode materials of SIBs owing to their advantages such as high specific capacity, simple synthesis route, and environmental benignity. However, the commercial development of the layered oxides is limited by sluggish kinetics, complex phase transition and poor air stability. Based on the research ideas from macro-to micro-scale, this review systematically summarizes the current optimization strategies of sodium-ion layered oxide cathodes (SLOC) from different dimensions: microstructure design, local chemistry regulation and structural unit construction. In the dimension of microstructure design, the various structures such as the microspheres, nanoplates, nanowires and exposed active facets are prepared to improve the slow kinetics and electrochemical performance. Besides, from the view of local chemistry regulation by chemical element substitution , the intrinsic electron/ion properties of SLOC have been enhanced to strengthen the structural stability. Furthermore, the optimization idea of endeavors to regulate the physical and chemical properties of cathode materials essentially is put forward from the dimension of structural unit construction. The opinions and strategies proposed in this review will provide some inspirations for the design of new SLOC in the future. sodium-ion batteries, layered oxide cathodes, microstructure design, local chemistry, structural unit Citation:
... [6][7][8][9][10][11][12][13][14][15] Owing to the lower cost and inferior energy density of SIBs than LIBs, the SIBs are undoubtedly promising candidates for grid-scale energy storage systems, which are of great importance for the effective utilization of the renewable energy. [16][17][18][19][20][21][22][23][24] Moreover, to integrate the intermittent renewables into the electric grid, the SIBs with high power and low cost are highly demanded. 25 In addition, the electrochemical performance of SIBs including capacity, efficiency, and energy/power density will deteriorate obviously when the temperature decreases/increases. [26][27][28] Accordingly, the wide-temperature operation of SIBs is essential for satisfying the demand for practical applications in extreme weather and different regions (e.g., high-altitude and tropical zones). ...
Low‐cost sodium‐ion batteries (SIBs) are promising candidates for grid‐scale energy‐storage systems, and the wide‐temperature operations of SIBs are highly demanded to accommodate extreme weather. Herein, a low‐cost SIB is fabricated with a Na4Fe3(PO4)2P2O7 (NFPP) cathode, a natural graphite (NG) anode, and an ether‐based electrolyte. The prepared NG//NFPP batteries deliver a long lifespan of 1000 cycles, high‐power density of 5938 W/kg, and remarkable rate performance of 10 A/g with a high capacity retention of 60%. Benefiting from the solvent co‐intercalation process of the NG anode and the high Na+ diffusion rate of the NFPP cathode, the NG//NFPP battery displays outstanding performance at −40 °C and even can work at an ultralow temperature of −70 °C. Furthermore, the high boiling point of the electrolytes and high thermal stability of the electrode materials also enable the high‐temperature operation of the full battery up to 130 °C. This work will guide the design of the wide‐temperature SIBs. A high‐power, low‐cost, and wide‐temperature SIB, which involves an NG anode, an NFPP cathode, and a diglyme‐based electrolyte, is successfully fabricated. Owing to the solvent co‐intercalation mechanism of the NG anode and the electrolyte with a high boiling point and low freezing point, the prepared wide‐temperature SIB can operate in a wide temperature range from −70°C to 130°C.
... However, the achieved energy density of SIBs is much lower than that of commercial lithium-ion batteries (LIBs) mainly because of the inferior capacity of cathode materials [2,3]. Among the existing cathode materials, sodium layered transition-metal oxides (Na x TMO 2 ), on account of their advantages of simple processing, high specific capacity, and adjustable structure, have gained enormous research interest [4][5][6][7]. The crystalline structure of Na x TMO 2 featured by alternant TMO 2 and Na layers provides effective diffusion pathways for Na + intercalation/deintercalation. ...
As the analogs of Li-rich materials, Na-rich transition metal layered oxides are promising cathode materials for Na-ion batteries owing to their high theoretical capacity and energy density through cumulative cationic and anionic redox. However, most of the reported Na-rich cathode materials are mainly Ru- and Ir-based layered oxides, which limits the practical application. Herein, we report a Na-rich and Ru-doped O3-type Na 1.1 Ni 0.35 Mn 0.55 O 2 cathode to mitigate this issue. By partially substituting Mn ⁴⁺ with high-electronegativity Ru ⁴⁺ , the structural stability and electrochemical performance of the cathode are both greatly improved. It is validated that the high covalency of Ru-O bonds could harden the structural integrity with rigid oxygen framework upon cycling, leading to enhanced O3-P3 phase transition reversibility. Ru doping also induces an enlarged interlayer spacing to boost the Na+ diffusion kinetics for improved rate capability. In addition, benefiting from the large energetic overlap between Ru 4d and O 2p states, the reinforced Ru-O covalency enables highly reversible Ru ⁴⁺ /Ru ⁵⁺ redox accompanied with more stable oxygen redox, leading to improved specific capacity and cycling stability over cycling. Our present study provides a promising strategy for designing high-performance Na-rich layered oxide cathode materials through covalency modulation toward practical applications.
... Sodium-ion batteries (SIBs), as a promising alternative to LIBs, have attracted interests due to their abundant resources and low cost [3][4][5][6]. Compared with other cathode materials for SIBs, transition metal (TM)-layered oxides exhibit advantages of high reversible capacity and operating voltage [7][8][9]. Fe and Mn are abundant and inexpensive raw materials, and thus Fe/Mn-based cathode materials for sodium batteries have significant price advantages. P2-Na x Fe 0.5 Mn 0.5 O 2 cathode was first reported by Komaba et al. [10], which provides a higher initial discharge capacity of 190 mAh g −1 . ...
As a cathode material for sodium-ion batteries (SIBs), P2-Na0.67Fe0.5Mn0.5O2 has the advantages of high capacity and high working voltage. However, the irreversible phase transition of P2-O2 causes the electrochemical performances to rapidly decline with cycling. The phase stability and therefore cycle stability could be effectively improved by cation doping. The precursor Fe0.5Mn0.5CO3 is prepared by coprecipitation method. The initial discharge-specific capacity of P2-Na0.67Fe0.5Mn0.5O2 in the voltage range of 2–4.3 V is 164 mAh·g−1, and its capacity retention rate after 100 cycles is 48.6%. Mg doping can improve the cycling stability and rate capability, while slightly reducing the initial capacity. The capacity retention is improved from 48.6 to 75.3% with Mg doping.
